From 0f495b198e247d57c06754e8c008a83f7c180021 Mon Sep 17 00:00:00 2001 From: Davide Grilli Date: Fri, 9 Oct 2026 19:06:40 +0200 Subject: [PATCH 1/5] Imposta la LLM-wiki: sposta i grezzi in raw/, riscrive CLAUDE.md, genera le note figura - Sposta tesi.md, immagini, cataloghi e schede fonti in raw/ (immutabile); rimuove CHANGELOG, tesi.pdf e tesi.docx - Riscrive CLAUDE.md: dominio, regole sui dati, ingest per capitolo, tesi_loc - Aggiunge scripts/gen_figures.py e le 78 note in wiki/figures/ da raw/immagini.json - Aggiunge index.md, log.md, wiki/tesi.md (mappa) e le cartelle wiki/{compounds,techniques,concepts,analyses} Co-Authored-By: Claude Sonnet 5.5 --- .gitignore | 1 + .obsidian/app.json | 1 + .obsidian/appearance.json | 1 + .obsidian/core-plugins.json | 33 +++++ .obsidian/graph.json | 22 ++++ CHANGELOG.md | 30 ----- CLAUDE.md | 124 +++++++++++++----- index.md | 20 +++ log.md | 18 +++ bibliografia.json => raw/bibliografia.json | 0 {fonti => raw/fonti}/01-bao-2020.md | 0 {fonti => 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mode 100644 wiki/overview.md create mode 100644 wiki/techniques/.gitkeep create mode 100644 wiki/tesi.md diff --git a/.gitignore b/.gitignore new file mode 100644 index 0000000..3f23e13 --- /dev/null +++ b/.gitignore @@ -0,0 +1 @@ +.obsidian/workspace.json diff --git a/.obsidian/app.json b/.obsidian/app.json new file mode 100644 index 0000000..9e26dfe --- /dev/null +++ b/.obsidian/app.json @@ -0,0 +1 @@ +{} \ No newline at end of file diff --git a/.obsidian/appearance.json b/.obsidian/appearance.json new file mode 100644 index 0000000..9e26dfe --- /dev/null +++ b/.obsidian/appearance.json @@ -0,0 +1 @@ +{} \ No newline at end of file diff --git a/.obsidian/core-plugins.json b/.obsidian/core-plugins.json new file mode 100644 index 0000000..639b90d --- /dev/null +++ b/.obsidian/core-plugins.json @@ -0,0 +1,33 @@ +{ + "file-explorer": true, + "global-search": true, + "switcher": true, + "graph": true, + "backlink": true, + "canvas": true, + "outgoing-link": true, + "tag-pane": true, + "footnotes": false, + "properties": true, + "page-preview": true, + "daily-notes": true, + "templates": true, + "note-composer": true, + "command-palette": true, + "slash-command": false, + "editor-status": true, + "bookmarks": true, + "markdown-importer": false, + "zk-prefixer": false, + "random-note": false, + "outline": true, + "word-count": true, + "slides": false, + "audio-recorder": false, + "workspaces": false, + "file-recovery": true, + "publish": false, + "sync": true, + "bases": true, + "webviewer": false +} \ No newline at end of file diff --git a/.obsidian/graph.json b/.obsidian/graph.json new file mode 100644 index 0000000..42a46ec --- /dev/null +++ b/.obsidian/graph.json @@ -0,0 +1,22 @@ +{ + "collapse-filter": true, + "search": "", + "showTags": false, + "showAttachments": false, + "hideUnresolved": false, + "showOrphans": true, + "collapse-color-groups": true, + "colorGroups": [], + "collapse-display": true, + "showArrow": false, + "textFadeMultiplier": 0, + "nodeSizeMultiplier": 1, + "lineSizeMultiplier": 1, + "collapse-forces": true, + "centerStrength": 0.518713248970312, + "repelStrength": 10, + "linkStrength": 1, + "linkDistance": 250, + "scale": 1, + "close": true +} \ No newline at end of file diff --git a/CHANGELOG.md b/CHANGELOG.md deleted file mode 100644 index 8fc89f6..0000000 --- a/CHANGELOG.md +++ /dev/null @@ -1,30 +0,0 @@ -# Changelog - -Tutte le modifiche rilevanti al repository sono documentate in questo file. -Formato ispirato a [Keep a Changelog](https://keepachangelog.com/it/1.1.0/); le versioni seguono il versionamento semantico. - -## [0.1.0] - 2026-10-09 - -Preparazione del materiale grezzo: dalla tesi originale (PDF/DOCX) a un sorgente Markdown canonico, con cataloghi strutturati e schede delle fonti, pronto per la trasformazione in wiki Obsidian. - -### Aggiunto - -- `tesi.pdf` e `tesi.docx` come grezzo di partenza (non modificati). -- `tesi.md`: sorgente canonico ottenuto dalla fusione dell'output MinerU con il contenuto del DOCX, con formattazione uniformata (titoli numerati con ancore del sommario, didascalie `**Figura N** - *testo*`, tabelle a pipe, formule LaTeX, decimali con la virgola, citazioni `[N](#ref-N)`). -- `immagini/`: 79 figure rinominate con hash SHA-256 e referenziate da `tesi.md`. -- `immagini.json`: catalogo delle 78 figure logiche (schema v2) con pannelli, sezioni, indici, `search_text` per embedding, righe di citazione e note di qualità (`review_notes`). -- `bibliografia.json`: 59 riferimenti parsati con righe e sezioni di citazione. -- `fonti/`: una scheda markdown per ciascuna delle 59 fonti della bibliografia (citazione verificata, DOI e link, abstract, argomenti, frasi della tesi in cui è citata, riferimenti correlati), con campo `fonte` collegato in `bibliografia.json`. -- `CLAUDE.md`: guida alla pipeline PDF/DOCX → MinerU → wiki Obsidian, convenzioni di `tesi.md` e difetti noti della tesi originale. - -### Modificato - -- Corrette le Figure 22 e 35 e verificate le annotazioni del catalogo immagini. -- Rimossa la didascalia stampata nell'immagine della Figura 19. - -### Rimosso - -- JSON intermedi di MinerU e versioni intermedie dei file. -- Figure non referenziate in `tesi.md`. - -[0.1.0]: #010---2026-10-09 diff --git a/CLAUDE.md b/CLAUDE.md index 971f8c6..06aef50 100644 --- a/CLAUDE.md +++ b/CLAUDE.md @@ -1,44 +1,108 @@ -# CLAUDE.md +# CLAUDE.md — Schema della LLM Wiki -This file provides guidance to Claude Code (claude.ai/code) when working with code in this repository. +Schema: struttura, convenzioni, workflow. Leggilo all'inizio di ogni sessione. Utente e LLM lo fanno evolvere insieme; ogni modifica va registrata in `log.md`. -## Cos'è questo repository +## Ruoli +- **Utente**: sceglie cosa ingerire, pone le domande, decide cosa conta. +- **LLM**: scrive e mantiene la wiki (pagine, link, indice, log, coerenza). L'utente non modifica `wiki/` a mano. +- Lingua: **italiano**. Titoli di fonti e termini tecnici restano nella lingua originale (l'Abstract della tesi è in inglese). -Non c'è codice: pipeline documentale **PDF/DOCX grezzi → Markdown (MinerU) → LLM-wiki / vault Obsidian**, a partire da una tesi di laurea magistrale (Chimica Industriale, "Sintesi e caratterizzazione di copolimeri bottle brush foto-elettro attivi", in italiano). Non ci sono build, lint o test; MinerU non è installato in locale (i JSON intermedi sono stati rimossi dalla storia). +## Dominio +Tesi magistrale in Chimica Industriale (Università di Bologna, Dipartimento "Toso Montanari"), a.a. 2025-2026: **"Sintesi e caratterizzazione di copolimeri bottle brush foto-elettro attivi"**. Candidata: Aurora Luzi. Relatore: Dr. Stefano Scurti. -## File +- **Tema:** semiconduttori polimerici emissivi π-coniugati con architettura bottle brush: scheletro DPP-3HT (polimerizzazione ossidativa con Fe(III)) e catene laterali di PCL ottenute per ROP dell'ε-caprolattone da gruppi OH pendenti. +- **Research question** (dall'Abstract e dal cap. 2): una architettura bottle brush può superare l'ACQ (Aggregation-Caused Quenching) allo stato solido, mantenendo l'integrità elettrochimica del core DPP? +- Risultati dichiarati nell'Abstract: il PCL agisce da spaziatore sterico e mantiene emissione nel rosso allo stato solido; il bandgap elettrochimico cresce linearmente con la % di DPP incorporato. -- `tesi.docx`, `tesi.pdf` — **grezzo di partenza** (tesi originale): mai da modificare né da usare come fonte di lavoro; servono solo per verificare dubbi di estrazione (es. `pdftotext -f -l tesi.pdf -`; la bibliografia è a p. 108). -- `tesi.md` — **sorgente canonico** già rifinito (fusione docx + output MinerU, formattazione uniformata). Lavorare qui. -- `immagini/` — le 79 figure usate da `tesi.md` (`![](immagini/.jpg)`). Nomi = hash: **non rinominare**, non rompere i riferimenti. Le immagini non referenziate sono state eliminate. -- `immagini.json` — catalogo delle figure per l'ingest (schema v2): `figures` (78 figure logiche, id `fig-NNN`, con `panels` = file fisici; 79 file), `sections`, `indexes`, `search_text` per embedding, `cited_in_md_lines`, `quality` (confidenza, flag, `review_notes` = discrepanze da verificare). Descrizioni e didascalie generate guardando le immagini, **non** verificate una per una. -- `bibliografia.json` — 59 riferimenti parsati (autori, titolo, rivista, anno, DOI) con `cited_in_md_lines`/`cited_in_sections`; `text` è la fonte di verità, gli altri campi sono euristici. -- `fonti/` — una scheda markdown per ognuna delle 59 fonti della bibliografia (`fonti/NN-cognome-anno.md`, frontmatter YAML): citazione verificata, autori/affiliazioni, DOI e link (anche ad accesso aperto), abstract, argomenti, riassunto del contenuto (solo per le fonti ad accesso aperto lette: campo `contenuto_letto`), frasi della tesi in cui è citata, bibliografia della fonte (primi 40 riferimenti), lavori correlati. Generate con Crossref, OpenAlex, Europe PMC e ricerca manuale; i testi integrali non sono riprodotti. In `bibliografia.json` ogni voce ha un campo `fonte` con file, stato e DOI verificato. +## Fonti (`raw/`, SOLA LETTURA — mai modificare, rinominare o cancellare) +| Percorso | Contenuto | +|---|---| +| `raw/tesi.md` | Sorgente canonico (1411 righe). Cap. 1 Introduzione (r.66), 2 Scopo (r.545), 3 Procedure sperimentali (r.562), 4 Discussione dei risultati (r.717), 5 Conclusioni (r.1279); bibliografia in fondo | +| `raw/immagini/` | 79 file figura (nomi = hash) | +| `raw/immagini.json` | Catalogo di 78 figure logiche: pannelli, didascalia stampata e generata, testo visibile, composti, concetti, contesto, qualità | +| `raw/bibliografia.json` | 59 riferimenti parsati con righe e sezioni di citazione; `text` è la fonte di verità, gli altri campi sono euristici | +| `raw/fonti/NN-cognome-anno.md` | Una scheda per riferimento (citazione verificata, DOI, abstract, frasi della tesi in cui è citato) | -**Numeri di riga:** `immagini.json` e `bibliografia.json` contengono righe 1-based di `tesi.md` (`md_line`, `caption_md_line`, `cited_in_md_lines`). Se aggiungi o togli righe in `tesi.md`, ricalcolale (o evita di cambiare il numero di righe). +I numeri di riga (`md_line`, `cited_in_md_lines`…) riferiscono `raw/tesi.md` e sono stabili perché `raw/` è immutabile: sono il localizzatore standard. -## Convenzioni di tesi.md +Convenzioni di `tesi.md`: decimali con la virgola; codici composto con il punto (`3.1b`); formule in `$...$`; citazioni `[N](#ref-N)`; apici/pedici in HTML. Anchor `#ref-N` e `#_TocNNN` non funzionano in Obsidian: nella wiki si traducono in wikilink. -- Titoli: `# 1 **Introduzione**`, `## 1.1 **Titolo**`, `### 1.1.1 **Titolo**` (numero senza punto, solo il titolo in grassetto). Il sommario (righe ~35-65) usa ancore `` prima di ogni titolo: funzionano, non rimuoverle. -- Didascalie sotto l'oggetto: `**Figura N** - *testo senza punto finale*`; stesso formato per `Tabella N` ed `Equazione N`. Richiami nel corpo: `**Figura N**`. -- Tabelle dati in markdown a pipe (rowspan ripetuti, colspan eliminati); restano HTML solo le due tabelle di frontespizio. Formule in `$...$` / `$$ ... $$`. -- Decimali con la **virgola** (anche in LaTeX: `4{,}8`); fanno eccezione l'Abstract in inglese, i dati NMR delle procedure sperimentali, le liste separate da virgole e i DOI. I codici composto restano con il punto (`3.1b`, `3.2.c`). -- Citazioni: `[N](#ref-N)` verso `` nella bibliografia (ultima sezione, voci `N. ...`). Esponenti/apici/pedici in HTML (``, ``); `1H-NMR`, `UV-Vis`, `bottle brush` (senza trattino), apostrofi dritti. +## Architettura +``` +CLAUDE.md index.md log.md +raw/ immutabile (vedi sopra) +scripts/gen_figures.py genera wiki/figures/ da raw/immagini.json +wiki/ + overview.md sintesi evolutiva, research question, risultati + tesi.md mappa capitolo/sezione → pagine wiki (unica pagina "source" della tesi) + bibliografia.md i 59 riferimenti raggruppati per tema, con link alle schede raw/fonti/ + concepts/ meccanismi, ROP, ACQ, bottle brush, π-stacking, ciclovoltammetria… + compounds/ un file per composto numerato (composto-32.md) o polimero/campione + techniques/ NMR, FT-IR, GPC, UV-Vis, fluorescenza, DSC, CV: condizioni usate nella tesi + figures/ note GENERATE dallo script (una per figura, non modificare a mano) + analyses/ query salvate; difetti-noti.md +``` +Niente pagine `source` per capitolo (duplicherebbero la tesi) e niente `entities/` generica. -## Difetti noti della tesi originale (non del markdown) +## Convenzioni pagine +- File `kebab-case.md`. Composti: `composto-32.md` con `aliases` (nome, codice come `3.1b`). Figure: `fig-026.md`. +- Link: wikilink `[[nome-file]]`, `[[nome|testo]]` per alias. Riferimenti bibliografici: `[[01-bao-2020|1]]` (link alla scheda in `raw/fonti/`; usare il numero della tesi). +- Frontmatter YAML: +```yaml +--- +title: Titolo leggibile +type: concept | compound | technique | analysis | overview | figure +tags: [tag1, tag2] +created: YYYY-MM-DD +updated: YYYY-MM-DD +tesi_loc: "§4.2 r.812-840" # dove la tesi sostiene il contenuto +refs: [3, 12] # numeri della bibliografia citati (opzionale) +figures: ["fig-026"] # opzionale +status: draft | stable +--- +``` +- **Ogni affermazione non banale cita la posizione**: `(§4.2, Fig. 27, r.812)` e, se serve, il riferimento `[[01-bao-2020|1]]`. Niente affermazioni non riconducibili a `raw/`. +- Inferenze dell'LLM marcate _(inferenza)_. Se non sai, dillo; non inventare fonti o dati. +- Ogni pagina termina con `## Collegamenti`. Nessuna pagina orfana. Crea una pagina concetto solo se serve a ≥2 sezioni/figure o è centrale. -- Bibliografia: voce 44 duplica la 1; voci 20, 22, 36, 53 incomplete anche nel PDF; DOI errati/non registrati nelle voci 47, 48 (il DOI corretto è 10.1080/15583720802231833) e 49; voci 47, 49, 53 non identificabili (vedi le rispettive schede in `fonti/`). -- Il testo cita "paragrafo XX (XX)" come segnaposto non risolto (4.4.4). -- Discrepanze figura/testo già annotate in `immagini.json` (`quality.review_notes`: Figure 26, 27, 29, 57, 62, 65, 66, 68). +## Regole sui dati scientifici +- **Copia alla lettera**: valori, unità, condizioni (T, P, solvente, tempo, carico, resa/conversione), formule LaTeX, formule chimiche, nomi di composti e sigle (DPP, 3HT, ROP, PCL, ACQ, CV, GPC…) restano come nella tesi. Non tradurre, riassumere, convertire o arrotondare dati sperimentali. Decimali con la virgola come in `tesi.md`; eccezioni: Abstract, dati NMR, liste, DOI. +- **Procedure sperimentali (cap. 3):** non riscriverle; la wiki rimanda al paragrafo (`tesi_loc`) e riporta solo i dati necessari alla pagina. +- **Sospetti errori di estrazione** (formula, tabella, valore): confronta con la fonte originale se disponibile, **segnala e non correggere**. Valori da condizioni diverse non vanno confrontati senza dirlo. +- **Sicurezza:** niente procedure di sintesi pericolose oltre quanto riporta la tesi; riporta i pericoli noti dei reagenti se citati. -## Convenzioni per la trasformazione in wiki Obsidian +## Figure +- `wiki/figures/*.md` sono **derivate**: `python scripts/gen_figures.py` le rigenera da `raw/immagini.json`, riportando ogni campo (didascalie, descrizioni e testo visibile per pannello, composti, concetti, contesto, righe di citazione, note di revisione) senza riassumere. Eccezione alla regola "solo l'LLM scrive in `wiki/`"; non modificarle a mano, correggi `raw/immagini.json` solo se l'utente lo chiede e poi rigenera. +- **Attendibilità:** solo `caption_printed` è testo della tesi. Descrizioni, `visible_text` e didascalia generata derivano dall'immagine e non sono verificati: valori letti da grafici o schemi (rese, picchi, potenziali) vanno confermati sull'immagine/tesi prima di riusarli. +- Le pagine concept/compound/technique richiamano le figure con `[[fig-026]]` o con l'embed `![[immagini/]]` (da `panels[].embed`). Le figure con `flags` o `review_notes` (Figure 26, 27, 29, 57, 62, 65, 66, 68 hanno discrepanze didascalia/testo) vanno citate con l'avvertenza. +- `compounds` nel catalogo sono numeri della tesi; `concepts` sono slug candidati, non nomi definitivi: crea la pagina solo se la regola dei ≥2 usi è soddisfatta. -- Non modificare `tesi.md` in modo distruttivo: generare le note in una cartella separata (es. `wiki/`), una per sezione/concetto, con wikilink `[[...]]`, frontmatter YAML e embed `![[immagini/]]` (già pronti in `immagini.json` → `panels[].embed`); usare le skill `obsidian:obsidian-markdown` e `obsidian:obsidian-bases`. -- Gli anchor `#ref-N` e `#_TocNNN` sono HTML: in Obsidian non si risolvono, vanno tradotti in wikilink alle note di riferimento. -- Testo scientifico: mantenere invariati formule LaTeX, formule chimiche, nomi di composti, unità, valori numerici e sigle (DPP, 3HT, ROP, PCL, ACQ, CV…). Non tradurre né riassumere dati sperimentali. -- Se una formula/tabella/valore sembra un errore di estrazione, confrontarlo con `tesi.pdf`/`tesi.docx` prima di correggere; segnalare, non indovinare. -- Ogni affermazione di una nota deve essere riconducibile a una sezione di `tesi.md` (citare capitolo/figura/riferimento). +## Difetti noti della tesi +Raccolti in `wiki/analyses/difetti-noti.md` (una sola pagina; le altre rimandano lì): bibliografia con voce 44 duplicata della 1; voci 20, 22, 36, 53 incomplete; DOI errati nelle voci 47, 48 (corretto 10.1080/15583720802231833) e 49; voci 47, 49, 53 non identificabili; segnaposto "paragrafo XX (XX)" in 4.4.4; discrepanze figura/testo sopra elencate. -## Git +## Workflow -Cronologia: tesi grezza MinerU → fusione docx+pdf → rinomina immagini in hash → pulizia intermedi → CLAUDE.md, catalogo immagini, uniformazione. Commit in italiano, descrittivi (es. "Rifinisce tesi.md: …"). +### Ingest (per capitolo, non per fonte) +Ordine: Abstract/Introduzione/Scopo (concepts, research question) → Procedure sperimentali (compounds, techniques) → Discussione (dati, overview) → Conclusioni → bibliografia. +1. Leggi per intero il capitolo/sezione in `raw/tesi.md` e le figure collegate (`sections[].figure_ids`). +2. Dopo il primo capitolo, discuti 3–5 takeaway e chiedi cosa enfatizzare; poi procedi a blocchi senza chiedere ogni volta. +3. Crea/aggiorna `concepts/`, `compounds/`, `techniques/`; segnala discrepanze in `analyses/difetti-noti.md`. +4. Aggiorna `wiki/tesi.md` (mappa), `overview.md` se la sintesi cambia, `bibliografia.md` se tocchi riferimenti. +5. Rigenera le figure se `raw/immagini.json` è cambiato. +6. Aggiorna `index.md` e appendi a `log.md`. + +### Query +Leggi `index.md` e le pagine rilevanti (non rileggere `raw/` se la wiki basta); rispondi in italiano con citazioni `[[...]]` e `tesi_loc`; proponi di salvare in `analyses/` le risposte durevoli; log `query`. + +### Lint (su richiesta o ogni ~10 ingest) +Contraddizioni, pagine orfane, concetti citati senza pagina, link rotti, frontmatter mancante, valori che non tornano con `raw/tesi.md`. Riporta, correggi dopo conferma. Log `lint`. + +## index.md e log.md +- `index.md`: catalogo per categoria (Overview, Tesi e bibliografia, Concetti, Composti, Tecniche, Figure, Analisi), voci `- [[pagina]] — riga di sintesi`, ordine alfabetico, conteggi aggiornati. Le 78 figure non si elencano una per una: una riga con link alla cartella e il conteggio per tipo. +- `log.md`: append-only, mai riscrivere le voci vecchie. Prefisso `## [YYYY-MM-DD] tipo | titolo` con tipo ∈ `setup, ingest, query, lint, schema`. Parsing: `grep "^## \[" log.md | tail -5`. + +## Regole d'oro +- Mai modificare `raw/`. Mai inventare dati, fonti o citazioni. +- Prima di cancellare o rinominare pagine chiedi conferma e aggiorna i link in entrata. +- Cambi allo schema: proponi, attendi ok, poi registra in `log.md` (tipo `schema`). +- Lavoro proporzionato: nessuna pagina "per dopo". diff --git a/index.md b/index.md new file mode 100644 index 0000000..1fdccb9 --- /dev/null +++ b/index.md @@ -0,0 +1,20 @@ +# Indice della wiki + +_Catalogo di tutte le pagine. Aggiornato a ogni ingest/query. Pagine curate: 2 · Figure generate: 78_ + +## Overview +- [[overview]] — sintesi evolutiva della tesi (da compilare) + +## Tesi e bibliografia +- [[tesi]] — mappa capitolo/sezione → pagine wiki + +## Concetti + +## Composti + +## Tecniche + +## Figure +- [[wiki/figures]] — 78 note generate da `raw/immagini.json` (28 reaction_scheme, 11 diagram, 8 mechanism, 7 spectrum_uv_vis, 6 spectrum_nmr, 5 chemical_structure, 5 plot, 4 spectrum_ir, 2 cv_voltammogram, 1 photo, 1 spectrum_fluorescence) + +## Analisi diff --git a/log.md b/log.md new file mode 100644 index 0000000..07baf42 --- /dev/null +++ b/log.md @@ -0,0 +1,18 @@ +# Log + +_Append-only. Formato: `## [YYYY-MM-DD] tipo | titolo`_ + +## [2026-10-09] setup | Inizializzazione wiki +- Creati: CLAUDE.md (schema), index.md, log.md, wiki/overview.md +- Cartelle: raw/, raw/assets/, wiki/{sources,entities,concepts,analyses} + +## [2026-10-09] schema | Dominio: tesi in Chimica Industriale +- CLAUDE.md: aggiunta sezione "Convenzioni specifiche di chimica industriale" (entità, dati con unità e condizioni, template composto/processo, sicurezza, DOI) + +## [2026-10-09] schema | Riscrittura CLAUDE.md per tesi singola con fonti in raw/ +- Dominio e research question compilati dall'Abstract e dal cap. 2; regole sui dati scientifici e difetti noti riportate dalla vecchia CLAUDE.md +- Struttura: tolta `entities/`; aggiunte `compounds/`, `techniques/`, `figures/`; `wiki/tesi.md` e `wiki/bibliografia.md` al posto delle pagine `source` +- Ingest per capitolo; riferimenti alle schede `raw/fonti/`; localizzatore `tesi_loc` (§ + riga di raw/tesi.md) +- Figure: `scripts/gen_figures.py` genera 78 note in `wiki/figures/` da `raw/immagini.json` (derivate, senza riassunti) + +## [2026-10-09] setup | Generate le 78 note figura e wiki/tesi.md (mappa) diff --git a/bibliografia.json b/raw/bibliografia.json similarity index 100% rename from bibliografia.json rename to raw/bibliografia.json diff --git a/fonti/01-bao-2020.md b/raw/fonti/01-bao-2020.md similarity index 100% rename from fonti/01-bao-2020.md rename to raw/fonti/01-bao-2020.md diff --git a/fonti/02-shaikh-2022.md b/raw/fonti/02-shaikh-2022.md similarity index 100% rename from fonti/02-shaikh-2022.md rename to raw/fonti/02-shaikh-2022.md diff --git a/fonti/03-auwalu-2021.md b/raw/fonti/03-auwalu-2021.md similarity index 100% rename from fonti/03-auwalu-2021.md rename to raw/fonti/03-auwalu-2021.md diff --git a/fonti/04-zhang-2024.md b/raw/fonti/04-zhang-2024.md similarity index 100% rename from fonti/04-zhang-2024.md rename to raw/fonti/04-zhang-2024.md diff --git a/fonti/05-iqbal-1988.md b/raw/fonti/05-iqbal-1988.md 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Nessun riassunto: ogni campo del catalogo viene riportato. +Uso: python scripts/gen_figures.py (rigenera tutto; le note sono derivate, non si modificano a mano).""" +import json +from pathlib import Path + +root = Path(__file__).resolve().parent.parent +cat = json.loads((root / "raw/immagini.json").read_text(encoding="utf8")) +out = root / "wiki/figures" +out.mkdir(parents=True, exist_ok=True) + + +def q(s): + return json.dumps(str(s), ensure_ascii=False) + + +def lst(xs): + return "[" + ", ".join(q(x) for x in xs) + "]" + + +for f in cat["figures"]: + loc, qual = f["location"], f["quality"] + f["label"] = f.get("label") or f["id"] # figure senza numero stampato + v = qual.get("verification") or {} + tesi_loc = f"§{loc['section']} r.{loc['md_line']}" + fm = [ + "---", + f"title: {q(' - '.join(x for x in (f['label'], f.get('title') or f.get('caption_printed')) if x))}", + "type: figure", + f"id: {f['id']}", + f"tipo: {f['type']}", + f"capitolo: {q(loc['chapter'])}", + f"sezione: {q(loc['section'])}", + f"tesi_loc: {q(tesi_loc)}", + f"composti: {lst(f.get('compounds', []))}", + f"concetti: {lst(f.get('concepts', []))}", + f"keywords: {lst(f.get('keywords', []))}", + f"confidence: {qual['confidence']}", + f"flags: {lst(qual.get('flags', []))}", + f"verifica: {v.get('verdict', 'n/d')}", + "derivata: true", + "---", + "", + ] + body = [f"# {f['label']}", ""] + body += [f"**Didascalia stampata (testo della tesi):** {f.get('caption_printed') or 'n/d'}", ""] + cap = f", didascalia r.{loc['caption_md_line']}" if loc.get("caption_md_line") else "" + body += [f"_Posizione: tesi.md {tesi_loc} (sezione {loc['section']} {loc['section_title']}){cap}_", ""] + body += ["> Sotto: contenuto generato guardando l'immagine, non verificato una per una.", ""] + body += [f"**Didascalia generata:** {f['caption']}", ""] + for p in f["panels"]: + body += [p["embed"], ""] + body += [f"- Pannello: {p['panel'] or 'unico'} · file `{p['file']}` · {p['width']}×{p['height']} · confidence {p['confidence']}"] + body += [f"- Descrizione: {p['description']}"] + body += ["- Testo visibile: " + (" · ".join(p["visible_text"]) or "n/d")] + if p.get("quality_flags"): + body += ["- Flag: " + ", ".join(p["quality_flags"])] + body += [""] + if f.get("text_context"): + body += ["## Contesto nel testo", f["text_context"], ""] + if f.get("cited_in_md_lines"): + body += ["Citata in tesi.md alle righe: " + ", ".join(map(str, f["cited_in_md_lines"])), ""] + if qual.get("review_notes"): + body += ["## Da verificare", qual["review_notes"], ""] + if v.get("issues"): + body += ["Esito revisione indipendente: " + "; ".join(v["issues"]), ""] + body += ["## Collegamenti", "- [[tesi]]", ""] + (out / f"{f['id']}.md").write_text("\n".join(fm + body), encoding="utf8") + +print(f"{len(cat['figures'])} note in {out}") diff --git a/tesi.docx b/tesi.docx deleted file mode 100644 index ec73940f1d166293d6220c3a3ac4b860722a3f0d..0000000000000000000000000000000000000000 GIT binary patch literal 0 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zsWN4oN>5`>IZq5(+~rPXwBo#IT{f&Ad>?@4dSJub9`IZbQ-EIC235I$=Xz)W(w1ZP zFm2feLz&wF{BSMchm*|v74XAJ&+PzyIO(|^zz-)qw?kwgMH_@K;|)RCSQ~e>gkocH zOV^2g{L4IY(N@3@Cs|n+m8)kr^B5~;dRvdsQ4M{U_4*CV0Dl0U13#Q7QOh={@&i2A ziek}LLp{fj;5E%S1N?9*w`_x9eqaaSxmLQo42aKxAFdT|cv$@)KG!N4==t~2g!o)! z5uO&}bKr;5fCc^lJO_R_r3HULd=C6@F;GIC!4AN4U99x95TEN}An1WV0MCIRPIN}# z4_|MW9@vrQ0#*M5JO_R_Q6_;Mfakyur?k+oe7#+I;19ra9rX1!1w03SH~}Hp0r9z3 zOrQ*~1LAY>aY0(}N16*%{($&gb4AY&;&UA)0X?t-;&VkRkQVHK_*|Q~o)++2(FW*& zKOjC=bO33=9}u5wHV)pIpH~V0z3zPIDKwl2jDsI z!znF%=YZ#Wh}`R(V*AQoz;ob-tL`q@_yTwyYgMjSjuBP4fakyur*gp#z;ob-({SbZ z0sL^%bAJFoob=od;D?i*_bcFslb-i0;D^(&26h0R13#S7x<7y)PI}(2fFDkJ?hoLH zlb(O)zz-)XQJ)M0ngij=WU43+koepTW(l}*&%T`4rv`j%hY+^snOo0;)=BTgYNAU+Agv;;crNby8hogE`)T%TZvkv>@5i@3u8@uz) zJ0ASWPtTa3n7+5;K}R2b`~=lx!a+Okd(_OMCsf;H@sH6D?L691b59i+_FmoHJA1UJ z?y>vm?xF~3w@2H1?!J3(u*?5j<0BJx*=5|= Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Struttura generica di un dichetopirrolopirrolo (DPP) con sostituenti R sugli azoti e R1 aromatici/eterociclici in posizione 3 e 6. + +![[immagini/455dd3d0c7bf0fe6ac581ee70795075c998d4dc7156eaa77a4576774f6fd8050.jpg]] + +- Pannello: unico · file `455dd3d0c7bf0fe6ac581ee70795075c998d4dc7156eaa77a4576774f6fd8050.jpg` · 643×209 · confidence high +- Descrizione: Nucleo biciclico DPP a due lattami fusi con due C=O; sugli azoti i sostituenti R (in blu), sui carboni olefinici i sostituenti R1 (in rosso). A destra la legenda dei sostituenti. +- Testo visibile: R · R1 · O · N · R = H, alchile, arile, acile ed eterociclico · R1 = aromatico e/o eterociclico + +## Contesto nel testo +Il testo introduce i DPP come nucleo di due anelli lattamici condensati con sostituenti aromatici/eteroaromatici periferici, come in Figura 1. + +Citata in tesi.md alle righe: 71 + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-002.md b/wiki/figures/fig-002.md new file mode 100644 index 0000000..fed8ed7 --- /dev/null +++ b/wiki/figures/fig-002.md @@ -0,0 +1,40 @@ +--- +title: "Figura 2 - meccanismo di formazione del DPP proposto da Farnum et al2" +type: figure +id: fig-002 +tipo: reaction_scheme +capitolo: "1" +sezione: "1.1.1" +tesi_loc: "§1.1.1 r.88" +composti: ["1", "2", "3"] +concetti: ["reformatskij", "farnum", "meccanismo", "dimerizzazione-ossidativa", "ciclizzazione", "benzonitrile"] +keywords: ["Reformatskij", "Farnum", "meccanismo", "dimerizzazione ossidativa", "ciclizzazione", "benzonitrile"] +confidence: high +flags: [] +verifica: ok +derivata: true +--- + +# Figura 2 + +**Didascalia stampata (testo della tesi):** Figura 2 - meccanismo di formazione del DPP proposto da Farnum et al2 + +_Posizione: tesi.md §1.1.1 r.88 (sezione 1.1.1 Storia e sintesi), didascalia r.90_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Meccanismo di formazione del DPP proposto da Farnum et al.: benzonitrile e reagente di Reformatskij danno il beta-amminocinnamato 1, dimerizzazione ossidativa a 2 e ciclizzazione a DPP 3. + +![[immagini/12c29dc9e968dc2801ea23927ce3ef650e1a3ac5d429a00d260b0ad226cd3d96.jpg]] + +- Pannello: unico · file `12c29dc9e968dc2801ea23927ce3ef650e1a3ac5d429a00d260b0ad226cd3d96.jpg` · 1256×304 · confidence high +- Descrizione: Benzonitrile + BrZn-CH2-COOR porta a 3-ammino-3-fenilacrilato (1); con [O] (dimerizzazione) si ottiene il dimero 2 con due NH2, due COOR e due fenili; con -2 ROH (ciclizzazione) si ottiene il 3,6-difenil-DPP (3) non sostituito. +- Testo visibile: BrZn · OR · NH2 · [O] · dimerizzazione · -2 ROH · ciclizzazione · COOR · ROOC · H2N · HN · 1 · 2 · 3 + +## Contesto nel testo +Farnum nel 1974 ottenne i DPP come sottoprodotti con una reazione di Reformatskij modificata; l'ipotesi prevede intermedio 1, dimero 2 e ciclizzazione. + +Citata in tesi.md alle righe: 86 + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-003.md b/wiki/figures/fig-003.md new file mode 100644 index 0000000..cc5401c --- /dev/null +++ b/wiki/figures/fig-003.md @@ -0,0 +1,40 @@ +--- +title: "Figura 3 - esperimento crossover in presenza di amminocinnamato" +type: figure +id: fig-003 +tipo: reaction_scheme +capitolo: "1" +sezione: "1.1.1" +tesi_loc: "§1.1.1 r.100" +composti: ["A", "B", "1", "3", "4", "5"] +concetti: ["crossover", "reformatskij", "amminocinnamato", "dpp-asimmetrico"] +keywords: ["crossover", "Reformatskij", "amminocinnamato", "DPP asimmetrico"] +confidence: high +flags: [] +verifica: ok +derivata: true +--- + +# Figura 3 + +**Didascalia stampata (testo della tesi):** Figura 3 - esperimento crossover in presenza di amminocinnamato + +_Posizione: tesi.md §1.1.1 r.100 (sezione 1.1.1 Storia e sintesi), didascalia r.102_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Esperimento di crossover: 4-metilbenzonitrile (A), etilbromoacetato (B) e Zn in presenza di amminocinnamato 1 forniscono la miscela dei DPP 5, 4 e 3. + +![[immagini/0287775d86d0d7a03631bd068b0f3f7ddc40dac6d140a671cb82d95c6427370b.jpg]] + +- Pannello: unico · file `0287775d86d0d7a03631bd068b0f3f7ddc40dac6d140a671cb82d95c6427370b.jpg` · 1262×392 · confidence high +- Descrizione: A sinistra 4-metilbenzonitrile (A), bromoacetato BrCH2COOR (B), Zn; sulla freccia il beta-amminocinnamato 1. Prodotti: DPP simmetrico con due p-tolil (5), DPP asimmetrico p-tolil/fenil (4), DPP difenil (3). +- Testo visibile: CH3 · H3C · Br · OR · Zn · NH2 · 1 · A · B · 5 · 4 · 3 · HN · NH + +## Contesto nel testo +L'esperimento di crossover verifica la partecipazione dell'intermedio 1; l'aggiunta di 1 aumenta il prodotto asimmetrico 4 (Tabella 1). + +Citata in tesi.md alle righe: 98 + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-004.md b/wiki/figures/fig-004.md new file mode 100644 index 0000000..293849f --- /dev/null +++ b/wiki/figures/fig-004.md @@ -0,0 +1,46 @@ +--- +title: "Figura 4 - sale di zinco derivato dall'intermedio 3" +type: figure +id: fig-004 +tipo: chemical_structure +capitolo: "1" +sezione: "1.1.1" +tesi_loc: "§1.1.1 r.116" +composti: [] +concetti: ["sale-di-zinco", "reformatskij", "intermedio"] +keywords: ["sale di zinco", "Reformatskij", "intermedio"] +confidence: medium +flags: ["low_resolution"] +verifica: fix +derivata: true +--- + +# Figura 4 + +**Didascalia stampata (testo della tesi):** Figura 4 - sale di zinco derivato dall'intermedio 3 + +_Posizione: tesi.md §1.1.1 r.116 (sezione 1.1.1 Storia e sintesi), didascalia r.118_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Sale di zinco dell'enammina (intermedio 1; la didascalia stampata riporta 'intermedio 3'): fenile, C=CH-COOR e azoto NH legato a BrZn. + +![[immagini/72aff80c81e497a042a6b102de0ab896c676af9c8881a5a940fc187c201db4df.jpg]] + +- Pannello: unico · file `72aff80c81e497a042a6b102de0ab896c676af9c8881a5a940fc187c201db4df.jpg` · 173×193 · confidence medium +- Descrizione: Struttura piccola e a bassa risoluzione: fenile legato a C=CH-C(=O)OR, azoto NH legato a BrZn, con BrZn in prossimita' dell'ossigeno carbonilico (legame di coordinazione non chiaramente disegnato). +- Testo visibile: HN · BrZn · O · OR +- Flag: low_resolution + +## Contesto nel testo +Né l'intermedio 1 né il suo sale di zinco dimerizzano; lo studio porta a un nuovo meccanismo. + +Citata in tesi.md alle righe: 114 + +## Da verificare +Immagine molto piccola. + +Esito revisione indipendente: La didascalia stampata dice 'intermedio 3' ma il testo (riga 114) indica il sale di zinco dell'intermedio 1 (3 e' il DPP); l'immagine mostra N-ZnBr senza legame di coordinazione al carbonile chiaramente disegnato + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-005.md b/wiki/figures/fig-005.md new file mode 100644 index 0000000..7460052 --- /dev/null +++ b/wiki/figures/fig-005.md @@ -0,0 +1,40 @@ +--- +title: "Figura 5 - meccanismo di formazione del DPP tramite la reazione di Reformtskij" +type: figure +id: fig-005 +tipo: mechanism +capitolo: "1" +sezione: "1.1.1" +tesi_loc: "§1.1.1 r.124" +composti: ["6", "7A", "7B", "8", "9", "DPP3"] +concetti: ["reformatskij", "meccanismo", "c-alchilazione", "tautomeria"] +keywords: ["Reformatskij", "meccanismo", "C-alchilazione", "tautomeria"] +confidence: high +flags: [] +verifica: ok +derivata: true +--- + +# Figura 5 + +**Didascalia stampata (testo della tesi):** Figura 5 - meccanismo di formazione del DPP tramite la reazione di Reformtskij + +_Posizione: tesi.md §1.1.1 r.124 (sezione 1.1.1 Storia e sintesi), didascalia r.126_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Meccanismo di formazione del DPP3 tramite reazione di Reformatskij: sale di Zn 6, C-alchilazione a 7A/7B, ciclizzazione a 8, aggiunta di benzonitrile a 9 e chiusura a DPP3. + +![[immagini/0777b568504fb43b6ef573876dba6f5a272671791d8027d1bcaa42eaf7a9d0fe.jpg]] + +- Pannello: unico · file `0777b568504fb43b6ef573876dba6f5a272671791d8027d1bcaa42eaf7a9d0fe.jpg` · 1262×548 · confidence high +- Descrizione: Benzonitrile + BrCH2CO2R + Zn danno il sale di zinco 6; con un secondo BrCH2CO2R si forma 7A, in equilibrio tautomerico con 7B (carbonio 'a' indicato); ciclizzazione al lattame 8; reazione con benzonitrile porta a 9 (ammino-metilene) e infine a DPP3. +- Testo visibile: CN · + BrCH2CO2R + Zn · BrCH2CO2R · BrZn · HN · a · NH2 · COOR · ROOC · 6 · 7A · 7B · 8 · 9 · DPP3 + +## Contesto nel testo +Nuovo meccanismo proposto: condensazione a sale di Zn 6, C-alchilazione con secondo bromoacetato, intermedi 7A/7B. + +Citata in tesi.md alle righe: 122, 130 + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-006.md b/wiki/figures/fig-006.md new file mode 100644 index 0000000..31bcc63 --- /dev/null +++ b/wiki/figures/fig-006.md @@ -0,0 +1,40 @@ +--- +title: "Figura 6 - analisi retrosintetica del DPP proposta da Iqbal et al." +type: figure +id: fig-006 +tipo: reaction_scheme +capitolo: "1" +sezione: "1.1.1" +tesi_loc: "§1.1.1 r.132" +composti: ["DPP3"] +concetti: ["retrosintesi", "iqbal", "estere-succinico", "benzonitrile"] +keywords: ["retrosintesi", "Iqbal", "estere succinico", "benzonitrile"] +confidence: high +flags: [] +verifica: ok +derivata: true +--- + +# Figura 6 + +**Didascalia stampata (testo della tesi):** Figura 6 - analisi retrosintetica del DPP proposta da Iqbal et al. + +_Posizione: tesi.md §1.1.1 r.132 (sezione 1.1.1 Storia e sintesi), didascalia r.134_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Analisi retrosintetica del DPP secondo Iqbal et al.: disconnessioni dei legami C-N/C-C fino a benzonitrile e estere succinico, preservando il legame centrale 'a'. + +![[immagini/817f7a716828f78218ddabd380b9fcad36a14ce9094fed0e9c6db973b0311197.jpg]] + +- Pannello: unico · file `817f7a716828f78218ddabd380b9fcad36a14ce9094fed0e9c6db973b0311197.jpg` · 1253×329 · confidence high +- Descrizione: Da sinistra: DPP difenil con tagli tratteggiati rossi, intermedio acciclico con enammine e aldeidi, frammenti X (benzilammina), Y (dialdeide succinica) e X, infine due benzonitrili e un diestere succinico ROOC-CH2CH2-COOR. Il legame 'a' è evidenziato. +- Testo visibile: a · X · Y · H2N · NH2 · HN · NH · N · RO · OR · O + +## Contesto nel testo +Strategia retrosintetica di Iqbal con tre frammenti (X, Y, X) che preserva il legame C-C centrale 'a'. + +Citata in tesi.md alle righe: 136 + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-007.md b/wiki/figures/fig-007.md new file mode 100644 index 0000000..97139fc --- /dev/null +++ b/wiki/figures/fig-007.md @@ -0,0 +1,40 @@ +--- +title: "Figura 7 - sintesi del DPP proposta da Iqbal et al." +type: figure +id: fig-007 +tipo: reaction_scheme +capitolo: "1" +sezione: "1.1.1" +tesi_loc: "§1.1.1 r.140" +composti: [] +concetti: ["iqbal", "estere-succinico", "base", "sintesi-dpp"] +keywords: ["Iqbal", "estere succinico", "base", "sintesi DPP"] +confidence: high +flags: [] +verifica: ok +derivata: true +--- + +# Figura 7 + +**Didascalia stampata (testo della tesi):** Figura 7 - sintesi del DPP proposta da Iqbal et al. + +_Posizione: tesi.md §1.1.1 r.140 (sezione 1.1.1 Storia e sintesi), didascalia r.142_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Sintesi del DPP di Iqbal et al.: due equivalenti di benzonitrile sostituito e un estere succinico, in presenza di base, danno DPP 3,6-diarile e 2 R'OH. + +![[immagini/cf12dd5b5015150d07e4e39c793edc69b197be98844c93bb294624f24b3a24fc.jpg]] + +- Pannello: unico · file `cf12dd5b5015150d07e4e39c793edc69b197be98844c93bb294624f24b3a24fc.jpg` · 868×304 · confidence high +- Descrizione: 2 ArCN (R sull'anello) + R'OOC-CH2CH2-COOR' con 'base' danno DPP 3,6-diaril sostituito + 2 R'OH. +- Testo visibile: 2 · CN · R · COOR' · R'OOC · base · HN · NH · + 2 R'OH · O + +## Contesto nel testo +La reazione supera il problema del legame C-C centrale grazie all'estere succinico; richiede una base forte non nucleofila (alcolato). + +Citata in tesi.md alle righe: 138, 144 + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-008.md b/wiki/figures/fig-008.md new file mode 100644 index 0000000..4373459 --- /dev/null +++ b/wiki/figures/fig-008.md @@ -0,0 +1,42 @@ +--- +title: "Figura 8 - reazione competitiva di ciclizzazione dell'estere succinico" +type: figure +id: fig-008 +tipo: reaction_scheme +capitolo: "1" +sezione: "1.1.1" +tesi_loc: "§1.1.1 r.146" +composti: [] +concetti: ["estere-succinico", "ciclizzazione-competitiva", "base"] +keywords: ["estere succinico", "ciclizzazione competitiva", "base"] +confidence: high +flags: [] +verifica: fix +derivata: true +--- + +# Figura 8 + +**Didascalia stampata (testo della tesi):** Figura 8 - reazione competitiva di ciclizzazione dell'estere succinico + +_Posizione: tesi.md §1.1.1 r.146 (sezione 1.1.1 Storia e sintesi), didascalia r.148_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Reazione competitiva di ciclizzazione dell'estere succinico in presenza di base, con formazione di un derivato cicloesandionico diestere. + +![[immagini/527a3cd0e4d0468cd19b0a75b855eb4903fcb344ef3efab2714fe7265004a236.jpg]] + +- Pannello: unico · file `527a3cd0e4d0468cd19b0a75b855eb4903fcb344ef3efab2714fe7265004a236.jpg` · 631×173 · confidence high +- Descrizione: 2 diesteri succinici ROOC-CH2CH2-COOR con base danno un anello a sei termini con due C=O e due gruppi COOR (2,5-dicarbossilato di cicloesan-1,4-dione). +- Testo visibile: 2 · COOR · ROOC · base · O + +## Contesto nel testo +Ciclizzazione competitiva dell'estere succinico in presenza di base, inibita dall'aggiunta graduale dell'estere (bassa concentrazione locale). + +Citata in tesi.md alle righe: 144 + +Esito revisione indipendente: text_context: nel testo la ciclizzazione competitiva e' inibita dall'aggiunta graduale dell'estere; l'eccesso di base serve a compensare l'acidita' del DPP + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-009.md b/wiki/figures/fig-009.md new file mode 100644 index 0000000..0c9e481 --- /dev/null +++ b/wiki/figures/fig-009.md @@ -0,0 +1,44 @@ +--- +title: "Figura 9 - sintesi del DPP3 proposta da Closs e Gompper" +type: figure +id: fig-009 +tipo: reaction_scheme +capitolo: "1" +sezione: "1.1.1" +tesi_loc: "§1.1.1 r.164" +composti: ["DPP3"] +concetti: ["closs-gompper", "succindiammide", "t-buok", "amidina"] +keywords: ["Closs-Gompper", "succindiammide", "t-BuOK", "amidina"] +confidence: high +flags: ["caption_mismatch"] +verifica: ok +derivata: true +--- + +# Figura 9 + +**Didascalia stampata (testo della tesi):** Figura 9 - sintesi del DPP3 proposta da Closs e Gompper + +_Posizione: tesi.md §1.1.1 r.164 (sezione 1.1.1 Storia e sintesi), didascalia r.166_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Sintesi del DPP3 secondo Closs e Gompper: succindiammide e N,N-dimetilbenzammide dietilacetale danno il bis-amidino intermedio, che con t-BuOK cicla a DPP3. + +![[immagini/d930a8d7b48446faf3acb4839a5330e3cf9dbf19e1ba59b5cdac9da94addf461.jpg]] + +- Pannello: unico · file `d930a8d7b48446faf3acb4839a5330e3cf9dbf19e1ba59b5cdac9da94addf461.jpg` · 1181×640 · confidence high +- Descrizione: Succindiammide H2N-CO-CH2CH2-CO-NH2 + acetale del N,N-dimetilbenzammide; due frecce: una verso DPP3 diretto, una verso il bis(N-acilamidina) che con t-BuOK forma il DPP3. +- Testo visibile: H2N · NH2 · O · N · t-BuOK · HN · NH · + +- Flag: caption_mismatch + +## Contesto nel testo +Nel 1987 Closs e Gompper propongono la sintesi da succindiammidi; resa globale circa 60%. + +Citata in tesi.md alle righe: 160 + +## Da verificare +Nel markdown la didascalia riportava 'Gloss' (refuso), corretto in 'Closs'. + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-010.md b/wiki/figures/fig-010.md new file mode 100644 index 0000000..453c084 --- /dev/null +++ b/wiki/figures/fig-010.md @@ -0,0 +1,39 @@ +--- +title: "Figura 10 - DDQ (2,3-dicloro-5,6-dicianobenzochinone)" +type: figure +id: fig-010 +tipo: chemical_structure +capitolo: "1" +sezione: "1.1.1" +tesi_loc: "§1.1.1 r.170" +composti: ["DDQ"] +concetti: ["ddq", "deidrogenazione", "chinone"] +keywords: ["DDQ", "deidrogenazione", "chinone"] +confidence: high +flags: ["low_resolution"] +verifica: ok +derivata: true +--- + +# Figura 10 + +**Didascalia stampata (testo della tesi):** Figura 10 - DDQ (2,3-dicloro-5,6-dicianobenzochinone) + +_Posizione: tesi.md §1.1.1 r.170 (sezione 1.1.1 Storia e sintesi), didascalia r.172_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Struttura del DDQ (2,3-dicloro-5,6-dicianobenzochinone), ossidante usato per deidrogenare i tetraidro-DPP. + +![[immagini/8c6bb2792de10aac72c41042ed82f8d74646772be1a73ef09237e408b5666b0f.jpg]] + +- Pannello: unico · file `8c6bb2792de10aac72c41042ed82f8d74646772be1a73ef09237e408b5666b0f.jpg` · 215×195 · confidence high +- Descrizione: Anello chinonico con due C=O, due Cl adiacenti e due gruppi CN adiacenti. +- Testo visibile: Cl · Cl · O · O · CN · CN +- Flag: low_resolution + +## Contesto nel testo +DDQ è il reagente scelto per deidrogenare i tetraidrodichetopirrolopirroli. + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-011.md b/wiki/figures/fig-011.md new file mode 100644 index 0000000..1c05829 --- /dev/null +++ b/wiki/figures/fig-011.md @@ -0,0 +1,38 @@ +--- +title: "Figura 11 - esempio di sintesi proposta da Sprake et al.6" +type: figure +id: fig-011 +tipo: reaction_scheme +capitolo: "1" +sezione: "1.1.1" +tesi_loc: "§1.1.1 r.176" +composti: ["11", "12", "13", "DDQ"] +concetti: ["sprake", "tetraidro-dpp", "ddq", "immina"] +keywords: ["Sprake", "tetraidro-DPP", "DDQ", "immina"] +confidence: high +flags: [] +verifica: ok +derivata: true +--- + +# Figura 11 + +**Didascalia stampata (testo della tesi):** Figura 11 - esempio di sintesi proposta da Sprake et al.6 + +_Posizione: tesi.md §1.1.1 r.176 (sezione 1.1.1 Storia e sintesi), didascalia r.178_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Sintesi proposta da Sprake et al.: l'immina 11 con estere succinico e base dà il tetraidro-DPP 12, deidrogenato con DDQ al DPP N,N'-di(3-piridil) 13. + +![[immagini/f4ba478941a0c0eb6302ebfee66f43039e2c9e06c55022c8b2e84bbd89d49dda.jpg]] + +- Pannello: unico · file `f4ba478941a0c0eb6302ebfee66f43039e2c9e06c55022c8b2e84bbd89d49dda.jpg` · 1259×342 · confidence high +- Descrizione: Immina da benzaldeide e 3-amminopiridina (11) + ROOC-CH2CH2-COOR, base, porta al biciclo saturo 12 con due fenili e due 3-piridil; DDQ in solvente dà il DPP insaturo 13. +- Testo visibile: N · RO · OR · O · base · DDQ · solvente · 11 · 12 · 13 + +## Contesto nel testo +Via ai precursori tetraidrati basata sulla condensazione di una immina (11) con estere succinico; 12 convertito in DPP. + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-012.md b/wiki/figures/fig-012.md new file mode 100644 index 0000000..1e14bbb --- /dev/null +++ b/wiki/figures/fig-012.md @@ -0,0 +1,40 @@ +--- +title: "Figura 12 - metodi di sintesi per ottenere il nucleo furo[3,4-c]furandione" +type: figure +id: fig-012 +tipo: reaction_scheme +capitolo: "1" +sezione: "1.1.1" +tesi_loc: "§1.1.1 r.186" +composti: ["14", "15", "16", "17"] +concetti: ["langhals", "furofurandione", "accoppiamento-ossidativo"] +keywords: ["Langhals", "furofurandione", "accoppiamento ossidativo"] +confidence: high +flags: [] +verifica: ok +derivata: true +--- + +# Figura 12 + +**Didascalia stampata (testo della tesi):** Figura 12 - metodi di sintesi per ottenere il nucleo furo[3,4-c]furandione + +_Posizione: tesi.md §1.1.1 r.186 (sezione 1.1.1 Storia e sintesi), didascalia r.188_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Metodi di sintesi del nucleo furo[3,4-c]furandione 17: da benzoilacetati 14 via 15 (Na, I2, poi 300 °C) o da bis-diazo 16 a 100 °C. + +![[immagini/88b885a66e23030d331ef30dc6888e32056f3bf1b70dee168799f897a6e6e66f.jpg]] + +- Pannello: unico · file `88b885a66e23030d331ef30dc6888e32056f3bf1b70dee168799f897a6e6e66f.jpg` · 840×434 · confidence high +- Descrizione: Riga 1: benzoilacetati ArCOCH2COOR (14) con Na, I2 danno 15, che a 300 °C forma 17. Riga 2: composto bis-diazo-tetrachetonico 16 a 100 °C dà 17 (furofurandione con due Ar). +- Testo visibile: Ar · RO · OR · Na, I2 · 300 °C · 100 °C · N2 · 14 · 15 · 16 · 17 + +## Contesto nel testo +Intermedio furofurandionico 17 ottenuto per via termica o con accoppiamento radicalico/ossidativo iodio/sodio e chiusura termica. + +Citata in tesi.md alle righe: 184 + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-013.md b/wiki/figures/fig-013.md new file mode 100644 index 0000000..e8bb505 --- /dev/null +++ b/wiki/figures/fig-013.md @@ -0,0 +1,40 @@ +--- +title: "Figura 13 - sintesi dei N-aril-DPP proposta da Langhals et al." +type: figure +id: fig-013 +tipo: reaction_scheme +capitolo: "1" +sezione: "1.1.1" +tesi_loc: "§1.1.1 r.192" +composti: ["17", "18", "19", "20", "21"] +concetti: ["langhals", "dcc", "tfa", "dmap", "n-aril-dpp"] +keywords: ["Langhals", "DCC", "TFA", "DMAP", "N-aril-DPP"] +confidence: high +flags: [] +verifica: ok +derivata: true +--- + +# Figura 13 + +**Didascalia stampata (testo della tesi):** Figura 13 - sintesi dei N-aril-DPP proposta da Langhals et al. + +_Posizione: tesi.md §1.1.1 r.192 (sezione 1.1.1 Storia e sintesi), didascalia r.194_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Sintesi dei N-aril-DPP secondo Langhals et al.: il furofurandione 17 reagisce con ammine, DCC e TFA per dare DPP asimmetrici 19, simmetrici 20 e N-alchil 21. + +![[immagini/92ca1a28a7507b12e73b2e34eb1b92e6ed2b1d241fa8fc2ccfe589b6793c3012.jpg]] + +- Pannello: unico · file `92ca1a28a7507b12e73b2e34eb1b92e6ed2b1d241fa8fc2ccfe589b6793c3012.jpg` · 1176×654 · confidence high +- Descrizione: 17 + Ar1-NH2, DCC, TFA porta a 18, poi con Ar2-NH2 a 19 (N-Ar1/N-Ar2); 17 + Ar1-NH2, DCC, TFA porta a 20 (due Ar1); 17 + Alk-NH2, DCC, DMAP, TFA porta a 21 (due Alk). +- Testo visibile: Ar1-NH2, DCC, TFA · Ar2-NH2 · Alk-NH2, DCC, DMAP, TFA · Ar · Alk · 17 · 18 · 19 · 20 · 21 + +## Contesto nel testo +Metodo per N-arilati simmetrici (20), asimmetrici (19) e con catene alchiliche (21). + +Citata in tesi.md alle righe: 190 + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-014.md b/wiki/figures/fig-014.md new file mode 100644 index 0000000..540bb7a --- /dev/null +++ b/wiki/figures/fig-014.md @@ -0,0 +1,42 @@ +--- +title: "Figura 14 - schema riassuntivo dei metodi sintetici analizzati per ottenere un dichetopirrolopirrolo" +type: figure +id: fig-014 +tipo: reaction_scheme +capitolo: "1" +sezione: "1.1.1" +tesi_loc: "§1.1.1 r.198" +composti: [] +concetti: ["riepilogo-sintesi-dpp", "farnum", "iqbal", "closs-gompper", "langhals", "ddq"] +keywords: ["riepilogo sintesi DPP", "Farnum", "Iqbal", "Closs-Gompper", "Langhals", "DDQ"] +confidence: high +flags: [] +verifica: fix +derivata: true +--- + +# Figura 14 + +**Didascalia stampata (testo della tesi):** Figura 14 - schema riassuntivo dei metodi sintetici analizzati per ottenere un dichetopirrolopirrolo + +_Posizione: tesi.md §1.1.1 r.198 (sezione 1.1.1 Storia e sintesi), didascalia r.200_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Schema riassuntivo dei metodi di sintesi dei DPP: Farnum, Iqbal, Closs-Gompper, metodo riduttivo e Langhals convergono sul DPP generico. + +![[immagini/d3804894a7e99bbf5bba8abce2680291b0b6dc0c435b453fa6beb143231ce6f9.jpg]] + +- Pannello: unico · file `d3804894a7e99bbf5bba8abce2680291b0b6dc0c435b453fa6beb143231ce6f9.jpg` · 1262×885 · confidence high +- Descrizione: Cinque righe: Farnum (benzonitrile + etilbromoacetato), Iqbal (2 ArCN + diestere succinico, base), Closs-Gompper (succindiammide + acetale, base), metodo riduttivo (tetraidro-DPP, DDQ), Langhals (furofurandione, R-NH2, DCC, TFA). Per i metodi riduttivo e Langhals le frecce multiple a sinistra indicano stadi precedenti non mostrati; la freccia di Farnum non riporta reagenti. Tutte puntano al DPP generico in riquadro, con R sugli azoti e in posizione 3,6. +- Testo visibile: Metodo di Farnum · Metodo di Iqbal · Metodo di Closs-Gompper · Metodo riduttivo · Metodo di Langhals · base · DDQ · R-NH2, DCC, TFA · R · Ar · COOR' · OEt · CN · Br · H2N · NH2 + +## Contesto nel testo +Schema riassuntivo di tutte le sintesi dei DPP descritte nel capitolo. + +Citata in tesi.md alle righe: 196 + +Esito revisione indipendente: Il riquadro finale mostra R sia sugli azoti sia sui carboni 3,6 (non solo N,N'); metodi riduttivo e Langhals partono da frecce multiple (stadi precedenti non mostrati); Farnum senza reagenti sulla freccia + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-015.md b/wiki/figures/fig-015.md new file mode 100644 index 0000000..5be6924 --- /dev/null +++ b/wiki/figures/fig-015.md @@ -0,0 +1,42 @@ +--- +title: "Figura 15 - spettro di assorbimento del DPP non sostituito in film con spessore di 1200 Å (linea tratteggiata)" +type: figure +id: fig-015 +tipo: spectrum_uv_vis +capitolo: "1" +sezione: "1.1.2" +tesi_loc: "§1.1.2 r.209" +composti: ["DPP"] +concetti: ["uv-vis", "assorbimento", "stato-solido-vs-soluzione", "dmso", "interazioni-intermolecolari"] +keywords: ["UV-vis", "assorbimento", "stato solido vs soluzione", "DMSO", "interazioni intermolecolari"] +confidence: high +flags: [] +verifica: fix +derivata: true +--- + +# Figura 15 + +**Didascalia stampata (testo della tesi):** Figura 15 - spettro di assorbimento del DPP non sostituito in film con spessore di 1200 Å (linea tratteggiata) + +_Posizione: tesi.md §1.1.2 r.209 (sezione 1.1.2 Struttura e reattività), didascalia r.211_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Spettro di assorbimento del DPP non sostituito in DMSO (linea continua) e in film di 1200 Å (linea tratteggiata). + +![[immagini/0fcb29bca38442ebe113d2d1621fed515e47c21e4535d7737fad11648e42fb62.jpg]] + +- Pannello: unico · file `0fcb29bca38442ebe113d2d1621fed515e47c21e4535d7737fad11648e42fb62.jpg` · 590×565 · confidence high +- Descrizione: Asse x: Wavelength (nm) 300-700; asse y sinistro: Mol. extinct. coeff./10^4 (0-3); asse y destro: Optical density (0.0-1.0, tacche 0.0, 0.5, 1.0). Soluzione (linea continua): banda a ~300 nm (~1.3), spalla ~320, picchi ~470 (circa 2.4) e ~508 (massimo circa 2.9). Solido (tratteggio): banda a ~305 nm, spalla ~490 e massimo circa 540 nm; spostamento batocromico e allargamento. Due frecce indicano l'asse di riferimento di ciascuna curva. +- Testo visibile: Solution · Solid · Mol. extinct. coeff./10^4 · Optical density · Wavelength (nm) · 300 · 400 · 500 · 600 · 700 · 0 · 1 · 2 · 3 · 0.0 · 0.5 · 1.0 + +## Contesto nel testo +Le interazioni intermolecolari influenzano le proprietà ottiche: lo spettro solido è spostato e allargato rispetto alla soluzione. + +Citata in tesi.md alle righe: 207 + +Esito revisione indipendente: Asse OD destro: tacche leggibili solo 0.0, 0.5, 1.0 (non fino a 1.2); omessi picco ~300 nm e solvente DMSO non presente in immagine + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-016.md b/wiki/figures/fig-016.md new file mode 100644 index 0000000..9de575d --- /dev/null +++ b/wiki/figures/fig-016.md @@ -0,0 +1,40 @@ +--- +title: "Figura 16 - struttura cristallina del DPP3 (distanze in Å)16" +type: figure +id: fig-016 +tipo: chemical_structure +capitolo: "1" +sezione: "1.1.2" +tesi_loc: "§1.1.2 r.241" +composti: ["DPP3"] +concetti: ["struttura-cristallina", "planarita", "torsione-fenilica", "contatti-hh-e-ho", "distanze-di-legame"] +keywords: ["struttura cristallina", "planarità", "torsione fenilica", "contatti H···H e H···O", "distanze di legame"] +confidence: high +flags: [] +verifica: fix +derivata: true +--- + +# Figura 16 + +**Didascalia stampata (testo della tesi):** Figura 16 - struttura cristallina del DPP3 (distanze in Å)16 + +_Posizione: tesi.md §1.1.2 r.241 (sezione 1.1.2 Struttura e reattività), didascalia r.243_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Struttura cristallina del DPP3 con distanze di legame in Å e torsione di 7.1° dei fenili rispetto al piano del nucleo. + +![[immagini/423e5b40dafcfcf5a959f73e6d8eed74b1f01972cef60482333c2a59f3292753.jpg]] + +- Pannello: unico · file `423e5b40dafcfcf5a959f73e6d8eed74b1f01972cef60482333c2a59f3292753.jpg` · 781×368 · confidence high +- Descrizione: Modello a bastoncini del 3,6-difenil-DPP con atomi etichettati (C1-C9, N, O, H1-H6). Distanze: 1.41, 1.44, 1.37, 1.46, 1.42, 1.38; interazioni tratteggiate H2...H1 2.19 e H6...O 2.32; angolo di torsione 7.1°. +- Testo visibile: H1 · H2 · H3 · H4 · H5 · H6 · C1 · C2 · C2' · C3 · C4 · C5 · C6 · C7 · C8 · C9 · N · O · 2.19 · 2.32 · 1.41 · 1.44 · 1.37 · 1.46 · 1.42 · 1.38 · 7.1° + +## Contesto nel testo +I fenili hanno torsione di soli 7° rispetto al piano del DPP, spiegando la sensibilità ai sostituenti periferici. + +Esito revisione indipendente: keyword 'legami idrogeno intramolecolari' non supportata: le linee tratteggiate sono contatti corti H...H (2.19) e H...O (2.32 Å); torsione 7.1° indicata su un solo fenile + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-017.md b/wiki/figures/fig-017.md new file mode 100644 index 0000000..ac7397f --- /dev/null +++ b/wiki/figures/fig-017.md @@ -0,0 +1,40 @@ +--- +title: "Figura 17 - reattività dei dichetopirrolopirroli2" +type: figure +id: fig-017 +tipo: diagram +capitolo: "1" +sezione: "1.1.2" +tesi_loc: "§1.1.2 r.251" +composti: ["DPP"] +concetti: ["reattivita", "nucleofilo", "elettrofilo", "cross-coupling"] +keywords: ["reattività", "nucleofilo", "elettrofilo", "cross coupling"] +confidence: high +flags: [] +verifica: ok +derivata: true +--- + +# Figura 17 + +**Didascalia stampata (testo della tesi):** Figura 17 - reattività dei dichetopirrolopirroli2 + +_Posizione: tesi.md §1.1.2 r.251 (sezione 1.1.2 Struttura e reattività), didascalia r.253_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Reattività dei DPP: siti attaccabili da nucleofili (a-d), siti nucleofili verso elettrofili (e-h) e reazione di cross coupling con organometalli (i). + +![[immagini/95db13c0d0b8c409535d4e0501600f0d207c24ed35d9e6dcbd1478b16f470d32.jpg]] + +- Pannello: unico · file `95db13c0d0b8c409535d4e0501600f0d207c24ed35d9e6dcbd1478b16f470d32.jpg` · 846×487 · confidence high +- Descrizione: DPP 3,6-diaril al centro. Frecce blu da Nu- verso carbonile ammidico (a), carbonio olefinico (b), anello con EWG (c, d). Frecce rosse verso E+ da O carbonilico (e), NH (f), anelli con EDG (g, h). Freccia verde da Organometalli verso X su un anello (i). +- Testo visibile: Nu- · E+ · EWG · EDG · X · Organometalli · a · b · c · d · e · f · g · h · i · NH · O + +## Contesto nel testo +Mostra i gruppi funzionali coinvolti nella reattività; due macrocategorie: siti elettrofili e siti nucleofili. + +Citata in tesi.md alle righe: 249 + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-018.md b/wiki/figures/fig-018.md new file mode 100644 index 0000000..8e051e3 --- /dev/null +++ b/wiki/figures/fig-018.md @@ -0,0 +1,38 @@ +--- +title: "Figura 18 - deprotonazione stabilizzata per risonanza mesomerica del DPP" +type: figure +id: fig-018 +tipo: mechanism +capitolo: "1" +sezione: "1.1.2" +tesi_loc: "§1.1.2 r.263" +composti: ["DPP", "22", "23", "24"] +concetti: ["deprotonazione", "risonanza", "anione-amidato"] +keywords: ["deprotonazione", "risonanza", "anione amidato"] +confidence: high +flags: [] +verifica: ok +derivata: true +--- + +# Figura 18 + +**Didascalia stampata (testo della tesi):** Figura 18 - deprotonazione stabilizzata per risonanza mesomerica del DPP + +_Posizione: tesi.md §1.1.2 r.263 (sezione 1.1.2 Struttura e reattività), didascalia r.265_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Deprotonazione del DPP con base e stabilizzazione dell'anione per risonanza mesomerica (strutture 22, 23, 24). + +![[immagini/ae4331727c45faf9a9b2dcf15ab197430625cbbd896ae767a1558fba1d404205.jpg]] + +- Pannello: unico · file `ae4331727c45faf9a9b2dcf15ab197430625cbbd896ae767a1558fba1d404205.jpg` · 909×493 · confidence high +- Descrizione: DPP + Base- (-BH) dà l'anione amidato 22 con carica negativa su N; frecce di risonanza verso 23 (carica su O dello stesso lattame) e 24 (carica sull'altro O, anello pirrolico aromatico). +- Testo visibile: DPP · Base- · -BH · Ar · HN · N · O · 22 · 23 · 24 + +## Contesto nel testo +La carica è distribuita tra N e O e anche sul secondo ossigeno (24, unità pirrolica aromatica), stabilizzando l'anione. + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-019.md b/wiki/figures/fig-019.md new file mode 100644 index 0000000..5545558 --- /dev/null +++ b/wiki/figures/fig-019.md @@ -0,0 +1,40 @@ +--- +title: "Figura 19 - reazione di protezione e deprotezione con gruppo Boc" +type: figure +id: fig-019 +tipo: reaction_scheme +capitolo: "1" +sezione: "1.1.2" +tesi_loc: "§1.1.2 r.275" +composti: ["3", "25"] +concetti: ["boc", "protezione", "deprotezione-termica", "pigmenti-latenti"] +keywords: ["Boc", "protezione", "deprotezione termica", "pigmenti latenti"] +confidence: high +flags: [] +verifica: ok +derivata: true +--- + +# Figura 19 + +**Didascalia stampata (testo della tesi):** Figura 19 - reazione di protezione e deprotezione con gruppo Boc + +_Posizione: tesi.md §1.1.2 r.275 (sezione 1.1.2 Struttura e reattività), didascalia r.277_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Protezione del DPP 3 con gruppo Boc (Boc2O, DMAP, THF) a 25 e Boc-deprotezione termica (180 °C, 2 min) con rigenerazione di 3, CO2 e isobutene. + +![[immagini/b9a386a9e36a6d42b793aa25702aacb59f0a71bdbccf09d9a281c8ea9b7e6d3e.jpg]] + +- Pannello: unico · file `b9a386a9e36a6d42b793aa25702aacb59f0a71bdbccf09d9a281c8ea9b7e6d3e.jpg` · 954×407 · confidence high +- Descrizione: 3 (difenil-DPP) con Boc2O, DMAP, THF dà il N,N'-di-Boc-DPP 25. Sotto: 25 a 180 °C, 2 min dà 3 + 2 CO2 + 2 isobutene. +- Testo visibile: Ph · HN · NH · Boc2O, DMAP, THF · 3 · 25 · Boc-deprotezione · 180 °C, 2 min · 3 + 2CO2 + 2 + +## Contesto nel testo +Il Boc aumenta la solubilità; i DPP protetti sono pigmenti latenti per colorare polimeri. + +Citata in tesi.md alle righe: 273 + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-020.md b/wiki/figures/fig-020.md new file mode 100644 index 0000000..b2b7aea --- /dev/null +++ b/wiki/figures/fig-020.md @@ -0,0 +1,40 @@ +--- +title: "Figura 20 - reazioni di sostituzione elettrofile aromatiche sugli anelli del DPP 3" +type: figure +id: fig-020 +tipo: reaction_scheme +capitolo: "1" +sezione: "1.1.2" +tesi_loc: "§1.1.2 r.289" +composti: ["3", "26", "27", "28"] +concetti: ["sostituzione-elettrofila-aromatica", "solfonazione", "bromurazione", "clorurazione"] +keywords: ["sostituzione elettrofila aromatica", "solfonazione", "bromurazione", "clorurazione"] +confidence: high +flags: [] +verifica: ok +derivata: true +--- + +# Figura 20 + +**Didascalia stampata (testo della tesi):** Figura 20 - reazioni di sostituzione elettrofile aromatiche sugli anelli del DPP 3 + +_Posizione: tesi.md §1.1.2 r.289 (sezione 1.1.2 Struttura e reattività), didascalia r.291_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Reazioni di sostituzione elettrofila aromatica sul DPP 3: solfonazione o bromurazione sui fenili (26, 27) e clorurazione con Cl2 gassoso (28). + +![[immagini/a6d0c2b1e32b84cb966e857c4cb74e90468ba7853ea4180a685a1f3226e2caad.jpg]] + +- Pannello: unico · file `a6d0c2b1e32b84cb966e857c4cb74e90468ba7853ea4180a685a1f3226e2caad.jpg` · 820×590 · confidence high +- Descrizione: DPP 3 con H2SO4/SO3 o Br2(g) dà 26 (X = SO3H) e 27 (X = Br) in para sui fenili; con Cl2(g) dà il prodotto 28 con quattro Cl su carboni sp3 (addizione). +- Testo visibile: H2SO4, SO3 · o Br2 (g) · Cl2 (g) · X · Ph · Cl · HN · NH · 3 · 26 X = SO3H · 27 X = Br · 28 + +## Contesto nel testo +Il DPP 3 è solfonato con acido solforico fumante e reagisce con Br2 e Cl2 gassosi. + +Citata in tesi.md alle righe: 287 + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-021.md b/wiki/figures/fig-021.md new file mode 100644 index 0000000..e15fa58 --- /dev/null +++ b/wiki/figures/fig-021.md @@ -0,0 +1,40 @@ +--- +title: "Figura 21 - bromurazione del DPP con sostituenti eteroaromatici in posizione 3 e 6" +type: figure +id: fig-021 +tipo: reaction_scheme +capitolo: "1" +sezione: "1.1.2" +tesi_loc: "§1.1.2 r.295" +composti: ["29", "30", "31", "32", "33", "34"] +concetti: ["bromurazione", "nbs", "tiofene", "furano", "selenofene", "dpp"] +keywords: ["bromurazione", "NBS", "tiofene", "furano", "selenofene", "DPP"] +confidence: high +flags: [] +verifica: ok +derivata: true +--- + +# Figura 21 + +**Didascalia stampata (testo della tesi):** Figura 21 - bromurazione del DPP con sostituenti eteroaromatici in posizione 3 e 6 + +_Posizione: tesi.md §1.1.2 r.295 (sezione 1.1.2 Struttura e reattività), didascalia r.297_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Bromurazione con NBS o Br2 dei DPP con eteroarili (S, O, Se) in 3 e 6: da 29-31 a 32-34 bromurati in posizione 5 degli eterocicli. + +![[immagini/b933e7c220a76882cc561e62bcab44a9ed60335dcafa353618f0a3a8eb36ade4.jpg]] + +- Pannello: unico · file `b933e7c220a76882cc561e62bcab44a9ed60335dcafa353618f0a3a8eb36ade4.jpg` · 921×373 · confidence high +- Descrizione: DPP N,N'-R con tiofene (29, X=S), furano (30, X=O), selenofene (31, X=Se); NBS o Br2 danno i bis(5-bromo-eteroaril) 32, 33, 34. R = alchile, acile, Boc. +- Testo visibile: NBS o Br2 · R · X · Br · 29 X = S · 30 X = O · 31 X = Se · 32 X = S · 33 X = O · 34 X = Se · R = alchile, acile, Boc + +## Contesto nel testo +Bromurazione dei DPP N,N'-disostituiti con eteroaromatici in 3 e 6, utile per funzionalizzazioni successive. + +Citata in tesi.md alle righe: 293, 363 + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-022.md b/wiki/figures/fig-022.md new file mode 100644 index 0000000..a33b547 --- /dev/null +++ b/wiki/figures/fig-022.md @@ -0,0 +1,42 @@ +--- +title: "Figura 22 - reazione di ciclizzazione mediante sostituzione elettrofila aromatica sui DPP studiata da Gryko et al.7" +type: figure +id: fig-022 +tipo: reaction_scheme +capitolo: "1" +sezione: "1.1.2" +tesi_loc: "§1.1.2 r.303" +composti: ["DPP", "35", "36"] +concetti: ["gryko", "ciclizzazione", "n-alchilazione", "tfoh", "sostituzione-elettrofila-aromatica"] +keywords: ["Gryko", "ciclizzazione", "N-alchilazione", "TfOH", "sostituzione elettrofila aromatica"] +confidence: high +flags: [] +verifica: fix +derivata: true +--- + +# Figura 22 + +**Didascalia stampata (testo della tesi):** Figura 22 - reazione di ciclizzazione mediante sostituzione elettrofila aromatica sui DPP studiata da Gryko et al.7 + +_Posizione: tesi.md §1.1.2 r.303 (sezione 1.1.2 Struttura e reattività), didascalia r.305_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Ciclizzazione per sostituzione elettrofila aromatica sui DPP (Gryko et al.): N-alchilazione con bromoacetaldeide dietilacetale a dare il diacetale 35 e chiusura in ambiente acido a 36. + +![[immagini/1d7d62195b9dfac2fc36ce6c359e0d5ed64e249c8967e57beb30b7fa6135e67c.jpg]] + +- Pannello: unico · file `1d7d62195b9dfac2fc36ce6c359e0d5ed64e249c8967e57beb30b7fa6135e67c.jpg` · 1167×465 · confidence high +- Descrizione: DPP con Ar fusi + BrCH2CH(OEt)2, TBAHS, K2CO3, DMF, 120-130 °C dà 35; poi 6M HCl aq o TfOH dà 36 policiclico con anelli piridinici fusi. Sotto sostituenti Ar a-e: 3,4-dimetossifenile, 2-tienile, 3-tienile, benzofurano di-tBu, fluorene con catene OMe e Br. Piccoli artefatti grafici accanto a 35 e 36. +- Testo visibile: TBAHS · K2CO3, DMF · 120-130 °C · 6M HClaq or TfOH · EtO · OEt · Br · DPP · 35 · 36 · Ar · a · b · c · d · e · OMe · tBu · S · MeO + +## Contesto nel testo +Il testo descrive l'alchilazione del DPP in DMF con K2CO3 e TBAHS (catalizzatore a trasferimento di fase) a dare i diacetali 35, trasformati con un acido forte di Brønsted in derivati carbonilici che ciclizzano per SEAr sull'anello aromatico elettron-ricco adiacente, ottenendo pigmenti 36 con almeno sei anelli fusi coniugati. + +Citata in tesi.md alle righe: 301 + +Esito revisione indipendente: alt_text troncato ('chius...'); nella didascalia '(35)' sembra indicare il reagente ma 35 e' il prodotto diacetale; text_context errato: il testo descrive la reazione (TBAHS, K2CO3, DMF, acido forte, ciclizzazione) e 36 ha almeno sei anelli fusi; MeO visibile in immagine + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-023.md b/wiki/figures/fig-023.md new file mode 100644 index 0000000..e140dbb --- /dev/null +++ b/wiki/figures/fig-023.md @@ -0,0 +1,40 @@ +--- +title: "Figura 23 - reazioni di cross coupling catalizzate da Pd sui DPP" +type: figure +id: fig-023 +tipo: reaction_scheme +capitolo: "1" +sezione: "1.1.2" +tesi_loc: "§1.1.2 r.313" +composti: ["32", "33", "34", "37"] +concetti: ["cross-coupling", "suzuki", "stille", "heck", "sonogashira", "buchwald-hartwig", "palladio"] +keywords: ["cross coupling", "Suzuki", "Stille", "Heck", "Sonogashira", "Buchwald-Hartwig", "palladio"] +confidence: high +flags: [] +verifica: ok +derivata: true +--- + +# Figura 23 + +**Didascalia stampata (testo della tesi):** Figura 23 - reazioni di cross coupling catalizzate da Pd sui DPP + +_Posizione: tesi.md §1.1.2 r.313 (sezione 1.1.2 Struttura e reattività), didascalia r.315_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Reazioni di cross coupling catalizzate da Pd sui DPP bromurati 32-34 e 37: Suzuki, Stille, Heck, Sonogashira e Buchwald-Hartwig. + +![[immagini/ab75adde10bed58f011b0e57bb27b271696d79594ff95462ce31eccc969448b1.jpg]] + +- Pannello: unico · file `ab75adde10bed58f011b0e57bb27b271696d79594ff95462ce31eccc969448b1.jpg` · 1234×464 · confidence high +- Descrizione: DPP bis(5-bromo-eteroaril) con [Pd] dà prodotti con Z in 5. Tabella reagente/reazione: ArB(OAlk)2 o ArB(OH)2 Suzuki; ArSnAlk3 Stille; alchene R2 Heck; alchino R2 Sonogashira; HNR2 o H2NR Buchwald-Hartwig. Z = -Ar, -CH=CH-R2, -C≡C-R2, -NR2 o -NHR2. R1 = alchil, aril, acil; R2 = aril, alchil. +- Testo visibile: [Pd] · Reagente · Reazione · ArB(OAlk)2, ArB(OH)2 · Suzuki · ArSnAlk3 · Stille · Heck · Sonogashira · HNR2, H2NR · Buchwald-Hartwig · 32 X = S · 33 X = O · 34 X = Se · 37 X = -CH=CH- · R1 · R2 · Z + +## Contesto nel testo +Reazioni di cross coupling con alte rese che sostituiscono il bromo con gruppi arilici, alchilici e amminici. + +Citata in tesi.md alle righe: 307 + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-024.md b/wiki/figures/fig-024.md new file mode 100644 index 0000000..ab169d8 --- /dev/null +++ b/wiki/figures/fig-024.md @@ -0,0 +1,42 @@ +--- +title: "Figura 24 - sintesi generica di polimeri a base di DPP mediante reazioni di cross coupling" +type: figure +id: fig-024 +tipo: reaction_scheme +capitolo: "1" +sezione: "1.1.2" +tesi_loc: "§1.1.2 r.319" +composti: ["32", "33", "34", "37"] +concetti: ["polimeri-coniugati", "suzuki", "stille", "cross-coupling", "tiofene", "fluorene", "carbazolo"] +keywords: ["polimeri coniugati", "Suzuki", "Stille", "cross coupling", "tiofene", "fluorene", "carbazolo"] +confidence: high +flags: [] +verifica: fix +derivata: true +--- + +# Figura 24 + +**Didascalia stampata (testo della tesi):** Figura 24 - sintesi generica di polimeri a base di DPP mediante reazioni di cross coupling + +_Posizione: tesi.md §1.1.2 r.319 (sezione 1.1.2 Struttura e reattività), didascalia r.323_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Sintesi generica di polimeri a base di DPP mediante cross coupling Pd-catalizzato dei DPP bromurati 32, 33, 34, 37 con composti aromatici bifunzionali Y-Ar-Y. + +![[immagini/967a337ba86d6286aa8b01f0989b91a248a31a2a91baafc916325bc124f4bb46.jpg]] + +- Pannello: unico · file `967a337ba86d6286aa8b01f0989b91a248a31a2a91baafc916325bc124f4bb46.jpg` · 1206×371 · confidence high +- Descrizione: 32, 33, 34, 37 + Y-Ar-Y con [Pd] danno il polimero [DPP-eteroarile-Ar]n con R1 sugli N. Sotto comonomeri Ar: oligotiofene (k = 1, 2), naftalene, fluorene dialchilato, tienotiofene, benzene con R2, carbazolo N-alchilato. Le definizioni X, Y, R1, R2 sono nel testo md, non nell'immagine. +- Testo visibile: 32 · 33 · 34 · 37 · Y · Ar · [Pd] · X · R1 · n · Alc · R2 · k = 1, 2 + +## Contesto nel testo +Composti aromatici bifunzionali polimerizzati con DPP bromurati in presenza di Pd; X = S, O, Se, -CH=CH-; Y = B(OH)2, B(OAlc)2, SnAlc3. + +Citata in tesi.md alle righe: 317, 325, 327 + +Esito revisione indipendente: alt_text troncato con '...' + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-025.md b/wiki/figures/fig-025.md new file mode 100644 index 0000000..b962405 --- /dev/null +++ b/wiki/figures/fig-025.md @@ -0,0 +1,40 @@ +--- +title: "Figura 25 - reazione di arilazione diretta del DPP 29 con diversi bromoarili" +type: figure +id: fig-025 +tipo: reaction_scheme +capitolo: "1" +sezione: "1.1.2" +tesi_loc: "§1.1.2 r.335" +composti: ["29", "38"] +concetti: ["arilazione-diretta", "pd-oac-2", "pivoh", "dma", "marder", "chen"] +keywords: ["arilazione diretta", "Pd(OAc)2", "PivOH", "DMA", "Marder", "Chen"] +confidence: high +flags: [] +verifica: ok +derivata: true +--- + +# Figura 25 + +**Didascalia stampata (testo della tesi):** Figura 25 - reazione di arilazione diretta del DPP 29 con diversi bromoarili + +_Posizione: tesi.md §1.1.2 r.335 (sezione 1.1.2 Struttura e reattività), didascalia r.337_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Arilazione diretta del DPP 29 con diversi bromoareni (Pd(OAc)2, PivOH, K2CO3, DMA, 100 °C) a dare 38 (a-h) con rese 39-96%. + +![[immagini/b60b2ed0441c7e89ab38e779618c5eee49a9df36d82e5122da708a9b7c78cbd2.jpg]] + +- Pannello: unico · file `b60b2ed0441c7e89ab38e779618c5eee49a9df36d82e5122da708a9b7c78cbd2.jpg` · 884×765 · confidence high +- Descrizione: 29 (DPP bis-tienile, R = 2-etilesile) + Ar-Br dà 38 con Ar in 5 dei tiofeni. Rese: a 3-metilfenile 85%, b 4-metossifenile 83%, c 5-metiltien-2-ile 39%, d fenile 96%, e 4-nitrofenile 91%, f 4-metilfenile 94%, g 4-trifluorometilfenile 92%, h difluorofenile 93%. +- Testo visibile: Ar-Br · Pd(OAc)2, PivOH · K2CO3, DMA · 100 °C · R · Bu · Et · 29 · 38 (a-h) · 85% · 83% · 39% · 96% · 91% · 94% · 92% · 93% · Me · OMe · NO2 · CF3 · F + +## Contesto nel testo +Marder e Chen impiegano il DPP 29 in arilazione diretta con diversi bromoareni. + +Citata in tesi.md alle righe: 339 + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-026.md b/wiki/figures/fig-026.md new file mode 100644 index 0000000..0cd70d1 --- /dev/null +++ b/wiki/figures/fig-026.md @@ -0,0 +1,46 @@ +--- +title: "Figura 26 - arilazione dei DPP di-brorumati con diversi areni" +type: figure +id: fig-026 +tipo: reaction_scheme +capitolo: "1" +sezione: "1.1.2" +tesi_loc: "§1.1.2 r.343" +composti: ["32", "37", "39", "40", "41"] +concetti: ["arilazione-diretta", "tiofene", "pd-oac-2", "dpp-bromurato"] +keywords: ["arilazione diretta", "tiofene", "Pd(OAc)2", "DPP bromurato"] +confidence: medium +flags: ["caption_mismatch"] +verifica: fix +derivata: true +--- + +# Figura 26 + +**Didascalia stampata (testo della tesi):** Figura 26 - arilazione dei DPP di-brorumati con diversi areni + +_Posizione: tesi.md §1.1.2 r.343 (sezione 1.1.2 Struttura e reattività), didascalia r.345_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Arilazione diretta dei DPP dibromurati 32 e 37 con tiofeni sostituiti (Y-tiofene) a dare i prodotti 39, 40 e 41. + +![[immagini/5968c5669dcfd68fd60100a31f5074a12c690f0b4cc45063e8f2b25b4afd949d.jpg]] + +- Pannello: unico · file `5968c5669dcfd68fd60100a31f5074a12c690f0b4cc45063e8f2b25b4afd949d.jpg` · 1251×593 · confidence medium +- Descrizione: 32 (X=S) e 37 (X=-CH=CH-) con 2-Y-tiofene, Pd(OAc)2, PivOH, K2CO3, DMA, 100 °C danno prodotti con bitiofene terminale. 39 (X=S): Y = CHO 40%, CO2Et 53%, CN 46%. 40 (X=-CH=CH-): CHO 75%, CO2Et 60%. 41: Y = unità DPP-tienil-fenile, 95%. +- Testo visibile: Pd(OAc)2, PivOH · K2CO3, DMA · 100 °C · Br · 32 X = S · 37 X = -CH=CH- · 39 · 40 · 41 · CHO (40%) · CO2Et (53%) · CN (46%) · CHO (75%) · CO2Et (60%) · (95%) · Ph · R · Bu · Et +- Flag: caption_mismatch + +## Contesto nel testo +Il testo afferma che l'arilazione diretta è efficace sia con bromoareni elettron-ricchi sia elettron-poveri, anche quando il bromuro è il DPP stesso, con rese minori (Figura 26). + +Citata in tesi.md alle righe: 341 + +## Da verificare +La didascalia ('DPP di-bromurati con diversi areni') non coincide col testo, che cita i prodotti 38(a-h) della Figura 25; l'immagine mostra l'arilazione di 32 e 37 con tiofeni sostituiti. + +Esito revisione indipendente: text_context vago: il testo dice che l'arilazione diretta e' efficace con bromoareni elettron-ricchi ed elettron-poveri, anche quando il bromuro e' il DPP stesso, con rese minori + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-027.md b/wiki/figures/fig-027.md new file mode 100644 index 0000000..72a6c4c --- /dev/null +++ b/wiki/figures/fig-027.md @@ -0,0 +1,46 @@ +--- +title: "Figura 27 - reazione di arilazione ossidativa" +type: figure +id: fig-027 +tipo: reaction_scheme +capitolo: "1" +sezione: "1.1.2" +tesi_loc: "§1.1.2 r.349" +composti: ["29", "42a", "42b", "42c"] +concetti: ["arilazione-ossidativa", "attivazione-c-h", "dpp", "tiofene", "fluoroareni", "pd-oac-2"] +keywords: ["arilazione ossidativa", "attivazione C-H", "DPP", "tiofene", "fluoroareni", "Pd(OAc)2"] +confidence: high +flags: ["caption_mismatch"] +verifica: fix +derivata: true +--- + +# Figura 27 + +**Didascalia stampata (testo della tesi):** Figura 27 - reazione di arilazione ossidativa + +_Posizione: tesi.md §1.1.2 r.349 (sezione 1.1.2 Struttura e reattività), didascalia r.351_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Arilazione ossidativa (attivazione C-H) del DPP 29 con fluoroareni polifluorurati (X = N, C-CN, C-F) per dare i prodotti 42a-c. + +![[immagini/8344868ae6e8de1151d7f70a43a30b2c1557784a0e8b48edd4a99431390092bd.jpg]] + +- Pannello: unico · file `8344868ae6e8de1151d7f70a43a30b2c1557784a0e8b48edd4a99431390092bd.jpg` · 1223×448 · confidence high +- Descrizione: Schema di reazione: il DPP 29 (nucleo dichetopirrolopirrolico con due tiofeni in 3,6 e due catene R sugli N, disegnate a scheletro come 2-etilesile con etichette Bu ed Et) reagisce con un fluoroarene (anello a sei termini con quattro F e X in para al C-H reattivo) in presenza di Pd(OAc)2, Ag2CO3, AcOH, DMSO, DMF a 140 °C per 8 h. Il prodotto 42 (a-c) porta due gruppi tetrafluoroarile sulle posizioni 5 dei tiofeni. Rese: a X = N 79%; b X = C-CN 45%; c X = C-F 23%. +- Testo visibile: 29 · 42 (a-c) · Pd(OAc)2, Ag2CO3, · AcOH, DMSO, DMF · 140 °C, 8 h · R = · Bu · Et · F · X · S · R · a: X = N (79%) · b: X = C-CN (45%) · c: X = C-F (23%) +- Flag: caption_mismatch + +## Contesto nel testo +Il testo descrive l'arilazione ossidativa via attivazione di legami C-H senza pre-attivazione dei reagenti; la resa migliore (79%) è per il composto citato come 45a, da tetrafluoropiridina e DPP 29. + +Citata in tesi.md alle righe: 355 + +## Da verificare +Il testo cita il prodotto '45a', ma l'immagine mostra i prodotti 42a-c: numerazione composti incoerente. + +Esito revisione indipendente: description: 'R = CH2-CH(Et)-Bu' e '2-etilesile-simili' non letterali (R e' disegnato a scheletro con etichette Bu ed Et); visible_text contiene testo non letterale + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-028.md b/wiki/figures/fig-028.md new file mode 100644 index 0000000..fbad9ff --- /dev/null +++ b/wiki/figures/fig-028.md @@ -0,0 +1,42 @@ +--- +title: "Figura 28 - meccanismo di polimerizzazione ossidativa mediante FeCl3" +type: figure +id: fig-028 +tipo: mechanism +capitolo: "1" +sezione: "1.1.2" +tesi_loc: "§1.1.2 r.357" +composti: [] +concetti: ["polimerizzazione-ossidativa", "fecl3", "politiofene", "radical-catione", "accoppiamento-ossidativo"] +keywords: ["polimerizzazione ossidativa", "FeCl3", "politiofene", "radical-catione", "accoppiamento ossidativo"] +confidence: high +flags: [] +verifica: fix +derivata: true +--- + +# Figura 28 + +**Didascalia stampata (testo della tesi):** Figura 28 - meccanismo di polimerizzazione ossidativa mediante FeCl3 + +_Posizione: tesi.md §1.1.2 r.357 (sezione 1.1.2 Struttura e reattività), didascalia r.359_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Meccanismo di polimerizzazione ossidativa del tiofene mediante FeCl3 (Fe3+), via radical-catione. + +![[immagini/043876b8b6cbe0ab2f02e61ee15320a65446a515e24ab474e51cb7ee2a53fe17.jpg]] + +- Pannello: unico · file `043876b8b6cbe0ab2f02e61ee15320a65446a515e24ab474e51cb7ee2a53fe17.jpg` · 1259×115 · confidence high +- Descrizione: Sequenza orizzontale: tiofene + Fe3+ (-> Fe2+) dà il radical-catione; perdita di H+ dà un radicale; attacco su una seconda molecola di tiofene dà un intermedio radicalico con H sp3; -H+ fornisce il bitiofene; frecce multiple conducono al politiofene, (tiofene)n. +- Testo visibile: Fe3+ · -Fe2+ · -H+ · -H+ · S · H · n + +## Contesto nel testo +Il testo confronta l'ossidazione chimica con FeCl3 con le reazioni di Suzuki/Stille: minore controllo su polidispersione e regioregolarità ma approccio diretto e scalabile. + +Citata in tesi.md alle righe: 355 + +Esito revisione indipendente: visible_text omette l'etichetta H sull'intermedio radicalico + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-029.md b/wiki/figures/fig-029.md new file mode 100644 index 0000000..bab3c7f --- /dev/null +++ b/wiki/figures/fig-029.md @@ -0,0 +1,46 @@ +--- +title: "Figura 29 - reazione di litiazione e funzionalizzazione con successiva reazione con elettrofili" +type: figure +id: fig-029 +tipo: reaction_scheme +capitolo: "1" +sezione: "1.1.2" +tesi_loc: "§1.1.2 r.365" +composti: ["29", "43", "44", "45", "46"] +concetti: ["litiazione", "lda", "elettrofili", "formilazione", "borilazione", "stannilazione", "iodurazione", "dpp"] +keywords: ["litiazione", "LDA", "elettrofili", "formilazione", "borilazione", "stannilazione", "iodurazione", "DPP"] +confidence: high +flags: ["caption_mismatch"] +verifica: fix +derivata: true +--- + +# Figura 29 + +**Didascalia stampata (testo della tesi):** Figura 29 - reazione di litiazione e funzionalizzazione con successiva reazione con elettrofili + +_Posizione: tesi.md §1.1.2 r.365 (sezione 1.1.2 Struttura e reattività), didascalia r.367_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Litiazione del DPP 29 con LDA a -78 °C e successiva reazione con elettrofili per dare i derivati 43-46 funzionalizzati in C5 dei tiofeni. + +![[immagini/eed9eb52dc858b172c4f6739c7b9f352bfa0e7ab10e422129a877a929c4e45bf.jpg]] + +- Pannello: unico · file `eed9eb52dc858b172c4f6739c7b9f352bfa0e7ab10e422129a877a929c4e45bf.jpg` · 1251×304 · confidence high +- Descrizione: Il DPP 29 reagisce con 1. LDA, -78 °C; 2. reagente, in THF (R = alchile). Prodotto 43-46 con gruppi X sulle posizioni 5 dei due tiofeni. Tabella a destra: Reagente / X / Prodotto: N-formilpiperidina o DMF -> CHO, 43 (24-86%); isopropossi-pinacolborano -> Bpin, 44 (78-94%); Me3SnCl -> SnMe3, 45 (45-94%); I2 -> I, 46 (67%). +- Testo visibile: 29 · 1. LDA, -78 °C · 2. Reagente · THF · R = alchile · 43-46 · Reagente · X · Prodotto · NCHO or DMF · -CHO · 43 24-86% · B-OiPr · 44 78-94% · Me3SnCl · -SnMe3 · 45 45-94% · I2 · -I · 46 67% +- Flag: caption_mismatch + +## Contesto nel testo +Il testo descrive la litiazione in C5 dei DPP 29, 30, 31 con LDA e le diverse funzionalizzazioni con elettrofili. + +Citata in tesi.md alle righe: 363 + +## Da verificare +Nell'immagine 45 e' il derivato SnMe3; controllare la numerazione dei composti col testo. + +Esito revisione indipendente: '-78 C' senza simbolo di grado in caption/alt_text/description (immagine: -78 °C) + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-030.md b/wiki/figures/fig-030.md new file mode 100644 index 0000000..cffc64f --- /dev/null +++ b/wiki/figures/fig-030.md @@ -0,0 +1,42 @@ +--- +title: "Figura 30 - sostituzione aromatica classica su derivati di DPP" +type: figure +id: fig-030 +tipo: reaction_scheme +capitolo: "1" +sezione: "1.1.2" +tesi_loc: "§1.1.2 r.371" +composti: ["27", "47", "48a", "48b", "48c", "48d"] +concetti: ["snar", "sostituzione-nucleofila-aromatica", "dpp", "autoclave", "ammine"] +keywords: ["SNAr", "sostituzione nucleofila aromatica", "DPP", "autoclave", "ammine"] +confidence: high +flags: [] +verifica: fix +derivata: true +--- + +# Figura 30 + +**Didascalia stampata (testo della tesi):** Figura 30 - sostituzione aromatica classica su derivati di DPP + +_Posizione: tesi.md §1.1.2 r.371 (sezione 1.1.2 Struttura e reattività), didascalia r.373_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Sostituzione nucleofila aromatica (SNAr) su DPP dialogenati (27 X = Br, 47 X = Cl) con ammine secondarie per dare i derivati 48a-d. + +![[immagini/5efb58f7f7d27a0467d9f14cd5191b3aeb168710c69f6fb0a27ac0cb188b2eac.jpg]] + +- Pannello: unico · file `5efb58f7f7d27a0467d9f14cd5191b3aeb168710c69f6fb0a27ac0cb188b2eac.jpg` · 1251×326 · confidence high +- Descrizione: DPP con due anelli fenilici para-sostituiti da X (27 X = Br; 47 X = Cl) e NH liberi; reagenti HNR2, NMP, 180-220 °C, 1-2 bar, autoclave; prodotto 48 con gruppi NR2 in para. Ammine: a -NMe2, b pirrolidina, c piperidina, d morfolina. +- Testo visibile: 27 X = Br · 47 X = Cl · HNR2, NMP · 180-220 °C, 1-2 bar · autoclave · 48 · -NR2 = · a · -NMe2 · b · c · d + +## Contesto nel testo +Il testo introduce la SNAr su DPP con buoni gruppi uscenti, in assenza di catalizzatori a base di Pd; la didascalia stampata parla di 'sostituzione aromatica classica'. + +Citata in tesi.md alle righe: 369 + +Esito revisione indipendente: '180-220 C' senza simbolo di grado nella description + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-031.md b/wiki/figures/fig-031.md new file mode 100644 index 0000000..4c0fcfb --- /dev/null +++ b/wiki/figures/fig-031.md @@ -0,0 +1,40 @@ +--- +title: "Figura 31 - diagramma di Jablonski" +type: figure +id: fig-031 +tipo: diagram +capitolo: "1" +sezione: "1.2" +tesi_loc: "§1.2 r.390" +composti: [] +concetti: ["diagramma-di-jablonski", "fluorescenza", "fosforescenza", "intersystem-crossing", "conversione-interna"] +keywords: ["diagramma di Jablonski", "fluorescenza", "fosforescenza", "intersystem crossing", "conversione interna"] +confidence: high +flags: [] +verifica: ok +derivata: true +--- + +# Figura 31 + +**Didascalia stampata (testo della tesi):** Figura 31 - diagramma di Jablonski + +_Posizione: tesi.md §1.2 r.390 (sezione 1.2 Fluorescenza), didascalia r.392_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Diagramma di Jablonski con assorbimento, conversione interna, intersystem crossing, fluorescenza e fosforescenza. + +![[immagini/a80b21103343058ce23aafb36ef90f8aa7f49d4ef4055f8e520fdb80d185a8b1.jpg]] + +- Pannello: unico · file `a80b21103343058ce23aafb36ef90f8aa7f49d4ef4055f8e520fdb80d185a8b1.jpg` · 1195×667 · confidence high +- Descrizione: Asse verticale ENERGIA. Livelli di singoletto S0 (stato fondamentale), S1, S2, Sn con sottolivelli vibrazionali a sinistra; livelli di tripletto T1, T2 a destra. Frecce: assorbimento (freccia gialla verso l'alto da S0), conversione interna (tratteggiata azzurra), fluorescenza (verde, S1 -> S0, emissione di luce), intersystem crossing (tratteggiata viola S1 -> T1), fosforescenza (rossa, T1 -> S0, emissione di luce), conversione interna da T1. +- Testo visibile: ENERGIA · Sn · S2 · S1 · T2 · T1 · stato fondamentale · Assorbimento (della radiazione elettromagnetica) · Conversione interna · Intersystem crossing · Fluorescenza (emissione di luce) · Fosforescenza (emissione di luce) + +## Contesto nel testo +Il testo introduce il diagramma di Jablonski come base per la trattazione di assorbimento e luminescenza; frecce continue per interazioni con la luce, tratteggiate per rilassamenti non radiativi. + +Citata in tesi.md alle righe: 388 + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-032.md b/wiki/figures/fig-032.md new file mode 100644 index 0000000..f1fe21d --- /dev/null +++ b/wiki/figures/fig-032.md @@ -0,0 +1,40 @@ +--- +title: "Figura 32 - schema rappresentativo del fenomeno di intersystem crossing" +type: figure +id: fig-032 +tipo: diagram +capitolo: "1" +sezione: "1.2" +tesi_loc: "§1.2 r.400" +composti: [] +concetti: ["intersystem-crossing", "singoletto", "tripletto", "regole-di-selezione-di-spin"] +keywords: ["intersystem crossing", "singoletto", "tripletto", "regole di selezione di spin"] +confidence: high +flags: [] +verifica: ok +derivata: true +--- + +# Figura 32 + +**Didascalia stampata (testo della tesi):** Figura 32 - schema rappresentativo del fenomeno di intersystem crossing + +_Posizione: tesi.md §1.2 r.400 (sezione 1.2 Fluorescenza), didascalia r.402_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Schema dell'intersystem crossing: popolazione di orbitali e spin nello stato fondamentale, singoletto e tripletto. + +![[immagini/2eb69c597f77449d9e46674c97478393268b91f0b3d19d8fb04ba6b6e22f2610.jpg]] + +- Pannello: unico · file `2eb69c597f77449d9e46674c97478393268b91f0b3d19d8fb04ba6b6e22f2610.jpg` · 1226×573 · confidence high +- Descrizione: Quattro schemi di coppie di orbitali con frecce di spin. Stato fondamentale (spin appaiati, somma S = 0); hv con Delta S = 0 porta al singoletto eccitato (S = 0, 2S+1 = 1); ISC (freccia tratteggiata rossa) porta al tripletto T (somma S = 1, 2S+1 = 3); transizione inversa dal fondamentale al tripletto barrata con X (Delta S = 1, vietata). +- Testo visibile: Energia · Stato fondamentale · hν · ΔS = 0 · ISC · ΔS = 1 · ΣS = 0 · ΣS = 1 · 2S+1 = 1 · 2S+1 = 3 · S · T + +## Contesto nel testo +Il testo spiega che le molecole in S1 possono invertire lo spin e passare a T1 (ISC), processo non radiativo. + +Citata in tesi.md alle righe: 404 + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-033.md b/wiki/figures/fig-033.md new file mode 100644 index 0000000..52c6a31 --- /dev/null +++ b/wiki/figures/fig-033.md @@ -0,0 +1,47 @@ +--- +title: "Figura 33 - stati elettronici per molecole rigide e flessibili" +type: figure +id: fig-033 +tipo: diagram +capitolo: "1" +sezione: "1.2" +tesi_loc: "§1.2 r.408" +composti: [] +concetti: ["fluorescenza", "rigidita-molecolare", "rilassamento-non-radiativo", "curve-di-energia-potenziale", "rilassamento-radiativo"] +keywords: ["fluorescenza", "rigidità molecolare", "rilassamento non radiativo", "curve di energia potenziale", "rilassamento radiativo"] +confidence: high +flags: ["cropped", "multi_panel"] +verifica: fix +derivata: true +--- + +# Figura 33 + +**Didascalia stampata (testo della tesi):** Figura 33 - stati elettronici per molecole rigide e flessibili + +_Posizione: tesi.md §1.2 r.408 (sezione 1.2 Fluorescenza), didascalia r.411_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Curve di energia potenziale per una molecola non rigida: lo stato eccitato è geometricamente distorto e favorisce il rilassamento non radiativo. Curve di energia potenziale per una molecola rigida: stato eccitato non distorto e rilassamento radiativo. + +![[immagini/ba021605d4b365536a686cb2f71f1c58ea2d5f5b9f962692d596f7a5a3d05ac7.jpg]] + +- Pannello: a · file `ba021605d4b365536a686cb2f71f1c58ea2d5f5b9f962692d596f7a5a3d05ac7.jpg` · 529×626 · confidence high +- Descrizione: Grafico E vs coordinate nucleari con due parabole (stato fondamentale in blu, stato eccitato in ocra) con minimi sfalsati. Freccia viola di eccitazione verticale, frecce verdi di rilassamento non radiativo, indicazione della distorsione geometrica tra i minimi. Titolo: STATO ECCITATO GEOMETRICAMENTE DISTORTO, molecola non rigida. +- Testo visibile: STATO ECCITATO GEOMETRICAMENTE DISTORTO · molecola non rigida · E · Coordinate nucleari · stato eccitato · eccitazione · stato fondamentale · rilassamento non radiativo · distorsione geometrica + +![[immagini/8047b55e3609435acd325d3602705c73a5308dc9b407322726ea6a1dde74af65.jpg]] + +- Pannello: b · file `8047b55e3609435acd325d3602705c73a5308dc9b407322726ea6a1dde74af65.jpg` · 512×609 · confidence high +- Descrizione: Grafico E vs coordinate nucleari con due parabole con minimi allineati (nessuna distorsione). Freccia viola di eccitazione e freccia verde di rilassamento radiativo verticali. Titolo parzialmente tagliato in alto: STATO ECCITATO NON DISTORTO, molecola rigida. +- Testo visibile: STATO ECCITATO · NON DISTORTO · molecola rigida · E · Coordinate nucleari · stato eccitato · eccitazione · rilassamento radiativo · stato fondamentale +- Flag: cropped + +## Contesto nel testo +Il testo afferma che per un'elevata efficienza di fluorescenza serve rigidità strutturale: nelle molecole poco flessibili geometria di stato fondamentale ed eccitato non sono distorte e l'energia è rilasciata come luce; la Figura 33 contrappone molecole non rigide (stato eccitato distorto) e rigide. + +Esito revisione indipendente: type 'plot' errato: diagrammi schematici di curve di energia potenziale senza dati; alt_text troncato; description con riferimenti interni a nomi di file; text_context con riferimento a nome file + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-034.md b/wiki/figures/fig-034.md new file mode 100644 index 0000000..0303284 --- /dev/null +++ b/wiki/figures/fig-034.md @@ -0,0 +1,41 @@ +--- +title: "Figura 34 - shift di Stokes37" +type: figure +id: fig-034 +tipo: diagram +capitolo: "1" +sezione: "1.2.1" +tesi_loc: "§1.2.1 r.422" +composti: [] +concetti: ["shift-di-stokes", "assorbimento", "fluorescenza", "fosforescenza", "livelli-vibrazionali"] +keywords: ["shift di Stokes", "assorbimento", "fluorescenza", "fosforescenza", "livelli vibrazionali"] +confidence: high +flags: ["low_resolution"] +verifica: ok +derivata: true +--- + +# Figura 34 + +**Didascalia stampata (testo della tesi):** Figura 34 - shift di Stokes37 + +_Posizione: tesi.md §1.2.1 r.422 (sezione 1.2.1 Shift di Stokes), didascalia r.424_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Shift di Stokes: livelli vibrazionali di S0 e S1 e spettri di assorbimento, fluorescenza e fosforescenza in funzione della lunghezza d'onda. + +![[immagini/0cb83724455d9b75cb980a077787323e0a434fb78192dc220e13069923f37fa6.jpg]] + +- Pannello: unico · file `0cb83724455d9b75cb980a077787323e0a434fb78192dc220e13069923f37fa6.jpg` · 629×524 · confidence high +- Descrizione: In alto due curve di potenziale S1 e S0 con livelli vibrazionali numerati 0-5; energie E1, E2 (0-0), E3 indicate con frecce. In basso spettri schematici di assorbimento (grigio), fluorescenza (nero, a destra dell'assorbimento) e fosforescenza (a lunghezze d'onda maggiori); asse E verso sinistra, lambda verso destra; marcatori E1, E2, E3. +- Testo visibile: S1 · S0 · E1 · E2 (0-0) · E3 · absorption · fluorescence · phosphorescence · E · λ · 0 1 2 3 4 5 +- Flag: low_resolution + +## Contesto nel testo +Il testo definisce lo shift di Stokes come differenza di lunghezza d'onda tra massimi di assorbimento ed emissione, dovuta a decadimenti vibrazionali. + +Citata in tesi.md alle righe: 420 + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-035.md b/wiki/figures/fig-035.md new file mode 100644 index 0000000..73f8193 --- /dev/null +++ b/wiki/figures/fig-035.md @@ -0,0 +1,42 @@ +--- +title: "Figura 35 - sistemi polimerici con inserimento di fluorofori, in verde il polimero e in rosso le unità di fluoroforo" +type: figure +id: fig-035 +tipo: diagram +capitolo: "1" +sezione: "1.3" +tesi_loc: "§1.3 r.483" +composti: [] +concetti: ["polimeri-fluorescenti", "host-guest", "matrice-polimerica", "fluoroforo-in-catena-principale-main-chain", "fluoroforo-pendente-side-chain", "fluoroforo-come-reticolante-cross-linked"] +keywords: ["polimeri fluorescenti", "host-guest", "matrice polimerica", "fluoroforo in catena principale (main-chain)", "fluoroforo pendente (side-chain)", "fluoroforo come reticolante (cross-linked)"] +confidence: high +flags: [] +verifica: fix +derivata: true +--- + +# Figura 35 + +**Didascalia stampata (testo della tesi):** Figura 35 - sistemi polimerici con inserimento di fluorofori, in verde il polimero e in rosso le unità di fluoroforo + +_Posizione: tesi.md §1.3 r.483 (sezione 1.3 Utilizzo di fluorofori in materiali polimerici), didascalia r.485_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Sistemi polimerici con inserimento di fluorofori (sfere rosse) in catene polimeriche (sfere verdi): a) fluorofori dispersi in una matrice reticolata, b) nella catena principale, c) come gruppi pendenti, d) come reticolanti tra catene. + +![[immagini/84a75adb472bc4fd46a5f6d27b0f8d6a3f709b8d073d033aeddaba16c2173b7e.png]] + +- Pannello: unico · file `84a75adb472bc4fd46a5f6d27b0f8d6a3f709b8d073d033aeddaba16c2173b7e.png` · 898×417 · confidence high +- Descrizione: Quattro schemi in griglia 2x2 con etichette a), b), c), d); catene polimeriche come file di sfere verdi, fluorofori come sfere rosse. a) Rete di catene reticolate con quattro fluorofori dispersi/intrappolati nelle maglie, non legati covalentemente. b) Un'unica catena con tre fluorofori intercalati nella catena principale (main chain). c) Catena con numerosi fluorofori legati lateralmente tramite bracci sottili (pendenti, side chain). d) Tre catene collegate da ponti con sfera rossa che fungono da reticolanti (crosslinker). +- Testo visibile: a) · b) · c) · d) + +## Contesto nel testo +Il testo elenca le categorie strutturali dei sistemi polimero-fluoroforo (dispersi, main chain, side chain, crosslinker); la figura unica le rappresenta nei pannelli a-d. + +Citata in tesi.md alle righe: 481 + +Esito revisione indipendente: keyword 'fluorofori disperso/guest-host' malformata + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-036.md b/wiki/figures/fig-036.md new file mode 100644 index 0000000..0079abf --- /dev/null +++ b/wiki/figures/fig-036.md @@ -0,0 +1,42 @@ +--- +title: "Figura 36 - rappresentazione schematica dei principi fisici alla base dei materiali optoelettronici: generazione di portatori di carica per assorbimento (sinistra) e ricombinazione radiativa per emissione (destra)" +type: figure +id: fig-036 +tipo: diagram +capitolo: "1" +sezione: "1.4" +tesi_loc: "§1.4 r.510" +composti: [] +concetti: ["optoelettronica", "band-gap", "celle-solari", "oled", "semiconduttori"] +keywords: ["optoelettronica", "band gap", "celle solari", "OLED", "semiconduttori"] +confidence: high +flags: [] +verifica: fix +derivata: true +--- + +# Figura 36 + +**Didascalia stampata (testo della tesi):** Figura 36 - rappresentazione schematica dei principi fisici alla base dei materiali optoelettronici: generazione di portatori di carica per assorbimento (sinistra) e ricombinazione radiativa per emissione (destra) + +_Posizione: tesi.md §1.4 r.510 (sezione 1.4 Applicazioni), didascalia r.512_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Principi fisici dei materiali optoelettronici: assorbimento (luce -> elettricità) ed emissione (elettricità -> luce) con bande di valenza e conduzione. + +![[immagini/84f29f22fa09304be18bab32ebed95a16f6ad53a8e0c3082c91550f724deaebc.jpg]] + +- Pannello: unico · file `84f29f22fa09304be18bab32ebed95a16f6ad53a8e0c3082c91550f724deaebc.jpg` · 969×495 · confidence high +- Descrizione: Due pannelli con asse Energia (E). Sinistra ASSORBIMENTO (Luce -> Elettricità): banda di conduzione Ec con e-, banda di valenza Ev con h+, band gap Eg, fotone hv assorbito; testo: la luce viene assorbita generando portatori di carica, es. celle solari, fotorivelatori. Destra EMISSIONE (Elettricità -> Luce): ricombinazione e-/lacuna con fotone emesso hv; es. LED, laser. +- Testo visibile: ASSORBIMENTO (Luce → Elettricità) · EMISSIONE (Elettricità → Luce) · Banda di Conduzione (Ec) · Banda di Valenza (Ev) · Band Gap (Eg) · Fotone (hν) · Fotone emesso (hν) · e- · h+ · Energia (E) · La luce viene assorbita, generando portatori di carica (elettrone-lacuna). Es. Celle solari, fotorivelatori · La ricombinazione di elettrone e lacuna emette energia sotto forma di luce. Es. LED, laser + +## Contesto nel testo +Introduce l'optoelettronica come interazione tra radiazione e semiconduttori; DPP come cromoforo chiave. + +Citata in tesi.md alle righe: 508 + +Esito revisione indipendente: alt_text troncato con '...' + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-037.md b/wiki/figures/fig-037.md new file mode 100644 index 0000000..db46dd5 --- /dev/null +++ b/wiki/figures/fig-037.md @@ -0,0 +1,40 @@ +--- +title: "Figura 37 - rappresentazione schematica dell'architettura OLED" +type: figure +id: fig-037 +tipo: diagram +capitolo: "1" +sezione: "1.4" +tesi_loc: "§1.4 r.530" +composti: [] +concetti: ["oled", "htl", "etl", "eml", "ito", "donatore-accettore"] +keywords: ["OLED", "HTL", "ETL", "EML", "ITO", "donatore-accettore"] +confidence: high +flags: [] +verifica: ok +derivata: true +--- + +# Figura 37 + +**Didascalia stampata (testo della tesi):** Figura 37 - rappresentazione schematica dell'architettura OLED + +_Posizione: tesi.md §1.4 r.530 (sezione 1.4 Applicazioni), didascalia r.532_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Architettura schematica di un OLED con relativo diagramma energetico dei livelli HOMO/LUMO. + +![[immagini/86a414964c7edb97a911082e5b5baced59db545ce7d435e1d67b21d038ceee5a.jpg]] + +- Pannello: unico · file `86a414964c7edb97a911082e5b5baced59db545ce7d435e1d67b21d038ceee5a.jpg` · 1037×526 · confidence high +- Descrizione: In alto stack di strati: Anodo/ITO, HTL (trasporto lacune), EML (emissivo, con emissione di luce hv), ETL (trasporto elettroni), Catodo. In basso diagramma energetico (eV) con LUMO/HOMO di HTL, EML (LUMO D-A, HOMO D-A) ed ETL; lacune h+ iniettate dall'anodo, elettroni e- dal catodo, ricombinazione nell'EML. +- Testo visibile: ANODO · HTL · ETL · CATODO · Luce (hν) · Anodo / ITO · HTL (Trasporto Lacune) · EML (Emissivo) · ETL (Trasporto Elettroni) · Catodo · LUMO · LUMO D-A · HOMO · HOMO D-A · Ricombinazione · Energia (eV) + +## Contesto nel testo +Il testo descrive lo strato emissivo tra elettrodi asimmetrici e gli strati ausiliari HTL ed ETL. + +Citata in tesi.md alle righe: 528 + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-038.md b/wiki/figures/fig-038.md new file mode 100644 index 0000000..3285857 --- /dev/null +++ b/wiki/figures/fig-038.md @@ -0,0 +1,42 @@ +--- +title: "Figura 38 - profilo energetico dell'elettroluminescenza in un polimero coniugato" +type: figure +id: fig-038 +tipo: diagram +capitolo: "1" +sezione: "1.4" +tesi_loc: "§1.4 r.536" +composti: [] +concetti: ["elettroluminescenza", "eccitone", "band-gap", "polimero-coniugato", "homo-lumo"] +keywords: ["elettroluminescenza", "eccitone", "band gap", "polimero coniugato", "HOMO/LUMO"] +confidence: high +flags: [] +verifica: fix +derivata: true +--- + +# Figura 38 + +**Didascalia stampata (testo della tesi):** Figura 38 - profilo energetico dell'elettroluminescenza in un polimero coniugato + +_Posizione: tesi.md §1.4 r.536 (sezione 1.4 Applicazioni), didascalia r.538_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Profilo energetico dell'elettroluminescenza in un polimero coniugato: iniezione di cariche, formazione dell'eccitone e rilassamento radiativo. + +![[immagini/af427dca9415944332b7e4022b98a9f345a78495915bbadf60d254143c3d545e.jpg]] + +- Pannello: unico · file `af427dca9415944332b7e4022b98a9f345a78495915bbadf60d254143c3d545e.jpg` · 1070×521 · confidence high +- Descrizione: Asse Energia (E). Anodo (+) a sinistra con iniezione e trasporto di lacune (h+), catodo (-) a destra con iniezione di elettroni (e-), campo elettrico dall'anodo al catodo. Nell'EML (strato emissivo/polimero coniugato) livelli LUMO e HOMO separati dal band gap Eg; formazione dell'eccitone, rilassamento radiativo con emissione di un fotone (hv). +- Testo visibile: Campo elettrico · Energia (E) · LUMO · HOMO · Band gap del polimero coniugato (Eg) · Formazione dell'eccitone · Rilassamento radiativo · Emissione di un fotone (hv) · Iniezione e trasporto di elettroni (e-) · Iniezione e trasporto di lacune (h+) · Anodo (+) · EML (Strato Emissivo / Polimero Coniugato) · Catodo (-) + +## Contesto nel testo +Il testo spiega che l'elettrone (sull'accettore DPP) e la lacuna (sul donatore tiofene) formano un eccitone che decade radiativamente. + +Citata in tesi.md alle righe: 540 + +Esito revisione indipendente: alt_text troncato con '...' + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-039.md b/wiki/figures/fig-039.md new file mode 100644 index 0000000..60bcdd5 --- /dev/null +++ b/wiki/figures/fig-039.md @@ -0,0 +1,38 @@ +--- +title: "Figura 39 - schema della cella elettrochimica impiegata nelle misure voltammetriche" +type: figure +id: fig-039 +tipo: diagram +capitolo: "3" +sezione: "3.4" +tesi_loc: "§3.4 r.708" +composti: [] +concetti: ["ciclovoltammetria", "cella-a-tre-elettrodi", "thf", "tbapf6", "glassy-carbon"] +keywords: ["ciclovoltammetria", "cella a tre elettrodi", "THF", "TBAPF6", "glassy carbon"] +confidence: high +flags: [] +verifica: ok +derivata: true +--- + +# Figura 39 + +**Didascalia stampata (testo della tesi):** Figura 39 - schema della cella elettrochimica impiegata nelle misure voltammetriche + +_Posizione: tesi.md §3.4 r.708 (sezione 3.4 Procedure sperimentali delle analisi voltammetriche), didascalia r.710_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Schema della cella elettrochimica a tre elettrodi usata nelle misure voltammetriche. + +![[immagini/7454f0793d62db92121d98aa27815bc85d5aae9f16807d3f188d7feb1ee83463.jpg]] + +- Pannello: unico · file `7454f0793d62db92121d98aa27815bc85d5aae9f16807d3f188d7feb1ee83463.jpg` · 550×615 · confidence high +- Descrizione: Cella in vetro con coperchio e quattro ingressi: elettrodo di lavoro (glassy carbon), elettrodo di riferimento (Ag/AgCl), controelettrodo (Pt, spirale) e tubo per flusso di N2 con bolle. Soluzione THF + TBAPF6 + polimero. +- Testo visibile: Elettrodo di lavoro (Glassy Carbon) · Elettrodo di riferimento (Ag/AgCl) · Controelettrodo (Pt) · Flusso di N2 · Cella in vetro · Soluzione (THF + TBAPF6 + polimero) + +## Contesto nel testo +Procedura voltammetrica con potenziostato CHI660C, THF e TBAPF6 0.1 M, degasaggio con N2. + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-040.md b/wiki/figures/fig-040.md new file mode 100644 index 0000000..1ad75e0 --- /dev/null +++ b/wiki/figures/fig-040.md @@ -0,0 +1,40 @@ +--- +title: "Figura 40 - sostituenti del DPP precedentemente studiati dal gruppo di ricerca" +type: figure +id: fig-040 +tipo: chemical_structure +capitolo: "4" +sezione: "4.1" +tesi_loc: "§4.1 r.726" +composti: [] +concetti: ["dpp", "benzonitrili", "ewg", "edg", "fluorescenza", "iso-dpp"] +keywords: ["DPP", "benzonitrili", "EWG", "EDG", "fluorescenza", "iso-DPP"] +confidence: high +flags: [] +verifica: ok +derivata: true +--- + +# Figura 40 + +**Didascalia stampata (testo della tesi):** Figura 40 - sostituenti del DPP precedentemente studiati dal gruppo di ricerca + +_Posizione: tesi.md §4.1 r.726 (sezione 4.1 Dichetopirrolopirroli), didascalia r.728_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Benzonitrili con sostituenti in para da EWG a EDG usati in precedenti lavori del gruppo, con indicazione dell'emissività dei DPP risultanti. + +![[immagini/b6398852c7419861eb44da7657cb2af96b59c5953a54007fb0df70f12a4c2cf9.jpg]] + +- Pannello: unico · file `b6398852c7419861eb44da7657cb2af96b59c5953a54007fb0df70f12a4c2cf9.jpg` · 898×321 · confidence high +- Descrizione: Sette benzonitrili: H, Cl, Br, OMe, NHAc, OH, NH2 in para, ordinati lungo una freccia da EWG (sinistra) a EDG (destra). Sopra i primi quattro, lampadine accese (rosa/rosse, la quarta viola) a indicare emissione; sopra gli altri tre nessuna lampadina. +- Testo visibile: EWG · EDG · CN · Cl · Br · OMe · HN-C(=O)CH3 · OH · NH2 + +## Contesto nel testo +EWG in para danno sistemi molto emissivi; EDG portano all'iso-DPP con fluorescenza inibita. + +Citata in tesi.md alle righe: 724 + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-041.md b/wiki/figures/fig-041.md new file mode 100644 index 0000000..1d3a8ec --- /dev/null +++ b/wiki/figures/fig-041.md @@ -0,0 +1,40 @@ +--- +title: "Figura 41 - schema di reazione del fluoroforo 2" +type: figure +id: fig-041 +tipo: reaction_scheme +capitolo: "4" +sezione: "4.1" +tesi_loc: "§4.1 r.738" +composti: ["1", "2"] +concetti: ["sintesi-dpp", "pseudo-stobbe", "n-alchilazione", "tiofene"] +keywords: ["sintesi DPP", "pseudo-Stobbe", "N-alchilazione", "tiofene"] +confidence: high +flags: [] +verifica: ok +derivata: true +--- + +# Figura 41 + +**Didascalia stampata (testo della tesi):** Figura 41 - schema di reazione del fluoroforo 2 + +_Posizione: tesi.md §4.1 r.738 (sezione 4.1 Dichetopirrolopirroli), didascalia r.740_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Schema di sintesi del fluoroforo 2: DPP 1 da tiofencarbonitrile e succinato, poi N-alchilazione con bromoesanolo. + +![[immagini/0238be4920f26782b3892465ff26009313f91823b3eaabb46aada5c489d49fd9.jpg]] + +- Pannello: unico · file `0238be4920f26782b3892465ff26009313f91823b3eaabb46aada5c489d49fd9.jpg` · 1215×337 · confidence high +- Descrizione: 2-tiofencarbonitrile + diisopropil succinato, t-AmOH/t-AmONa -> 1; poi Br-(CH2)5-CH2-OH, DMSO, t-BuOK -> 2 con R = catena esanolo terminante in OH. +- Testo visibile: t-AmOH / t-AmONa · DMSO, t-BuOK · 1 · 2 · R: · OH · Br · 5 + +## Contesto nel testo +Mostra la sintesi del fluoroforo 2 poi usato nelle polimerizzazioni. + +Citata in tesi.md alle righe: 736 + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-042.md b/wiki/figures/fig-042.md new file mode 100644 index 0000000..e9424a7 --- /dev/null +++ b/wiki/figures/fig-042.md @@ -0,0 +1,40 @@ +--- +title: "Figura 42 - meccanismo di reazione proposto per la formazione dei DPP" +type: figure +id: fig-042 +tipo: mechanism +capitolo: "4" +sezione: "4.1" +tesi_loc: "§4.1 r.744" +composti: [] +concetti: ["meccanismo", "pseudo-stobbe", "dpp", "t-amona"] +keywords: ["meccanismo", "pseudo-Stobbe", "DPP", "t-AmONa"] +confidence: high +flags: [] +verifica: ok +derivata: true +--- + +# Figura 42 + +**Didascalia stampata (testo della tesi):** Figura 42 - meccanismo di reazione proposto per la formazione dei DPP + +_Posizione: tesi.md §4.1 r.744 (sezione 4.1 Dichetopirrolopirroli), didascalia r.746_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Meccanismo proposto per la formazione del DPP a partire da succinato e 2-tiofencarbonitrile. + +![[immagini/b8095b77f46fe9daaa5430cabef072a05c35605430fd6ff6af09c38553a33d1c.jpg]] + +- Pannello: unico · file `b8095b77f46fe9daaa5430cabef072a05c35605430fd6ff6af09c38553a33d1c.jpg` · 1134×600 · confidence high +- Descrizione: Il succinato è deprotonato da t-AmONa/t-AmOH; il carbanione attacca il nitrile; l'immina/enammina ciclizza con perdita di ROH a dare il pirrolinone; una seconda deprotonazione e attacco a un secondo nitrile, ciclizzazione finale con perdita di RO- danno il DPP 3,6-ditienil. +- Testo visibile: t-AmONa · t-AmOH · Na+ · RO · OR · HN · H2N · COOR · NH · O · S · N + +## Contesto nel testo +Il tiofene è introdotto dopo la formazione dell'alcolato, il succinato è gocciolato lentamente per evitare reazioni parassite. + +Citata in tesi.md alle righe: 742 + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-043.md b/wiki/figures/fig-043.md new file mode 100644 index 0000000..d5d3780 --- /dev/null +++ b/wiki/figures/fig-043.md @@ -0,0 +1,42 @@ +--- +title: "Figura 43 - meccanismo di autocondensazione di Claisen" +type: figure +id: fig-043 +tipo: mechanism +capitolo: "4" +sezione: "4.1" +tesi_loc: "§4.1 r.750" +composti: [] +concetti: ["condensazione-di-claisen", "succinato", "reazione-collaterale", "meccanismo"] +keywords: ["condensazione di Claisen", "succinato", "reazione collaterale", "meccanismo"] +confidence: high +flags: [] +verifica: fix +derivata: true +--- + +# Figura 43 + +**Didascalia stampata (testo della tesi):** Figura 43 - meccanismo di autocondensazione di Claisen + +_Posizione: tesi.md §4.1 r.750 (sezione 4.1 Dichetopirrolopirroli), didascalia r.752_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Meccanismo di autocondensazione di Claisen del succinato in presenza di base, reazione parassita che porta a un derivato del cicloesandione. + +![[immagini/9cb4d6705cae60dc0e20d74685b5217ff70680872a3714cd00103f3561ad251b.jpg]] + +- Pannello: unico · file `9cb4d6705cae60dc0e20d74685b5217ff70680872a3714cd00103f3561ad251b.jpg` · 1126×407 · confidence high +- Descrizione: Il diestere succinico è deprotonato da una base; il carbanione attacca una seconda molecola con perdita di RO-; seconda condensazione intramolecolare (ancora con perdita di RO-) porta al 2,5-diosso-cicloesano-1,4-dicarbossilato (due COOR e due C=O). +- Testo visibile: Base · -RO- · RO · OR · COOR · O + +## Contesto nel testo +Spiega la reazione parassita dovuta a eccessiva concentrazione locale di succinato in condizioni basiche. + +Citata in tesi.md alle righe: 748 + +Esito revisione indipendente: descrizione: il prodotto e un 2,5-diosso-cicloesano-1,4-dicarbossilato (due C=O chetonici), non "diossi" + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-044.md b/wiki/figures/fig-044.md new file mode 100644 index 0000000..bdade10 --- /dev/null +++ b/wiki/figures/fig-044.md @@ -0,0 +1,45 @@ +--- +title: "Figura 44 - spettro 1H-NMR in DMSO del prodotto 1" +type: figure +id: fig-044 +tipo: spectrum_nmr +capitolo: "4" +sezione: "4.1" +tesi_loc: "§4.1 r.758" +composti: ["1"] +concetti: ["1h-nmr", "dmso", "dpp", "tiofene", "assegnazione"] +keywords: ["1H-NMR", "DMSO", "DPP", "tiofene", "assegnazione"] +confidence: medium +flags: [] +verifica: fix +derivata: true +--- + +# Figura 44 + +**Didascalia stampata (testo della tesi):** Figura 44 - spettro 1H-NMR in DMSO del prodotto 1 + +_Posizione: tesi.md §4.1 r.758 (sezione 4.1 Dichetopirrolopirroli), didascalia r.760_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Spettro 1H-NMR in DMSO del DPP 1 con assegnazione dei protoni tiofenici (pallini colorati). + +![[immagini/5b9c36eb3db1dae7d33d24a159eb75cd575f40a33dad1110ef83da17bffaa3d9.jpg]] + +- Pannello: unico · file `5b9c36eb3db1dae7d33d24a159eb75cd575f40a33dad1110ef83da17bffaa3d9.jpg` · 1223×829 · confidence medium +- Descrizione: Struttura del DPP 1 con protoni dei tiofeni marcati rosso, blu, verde. Asse ppm da 12 a 0. Segnali: rosso circa 8.2, blu circa 7.9, verde circa 7.3 ppm, integrali 1.00, 1.00, 1.01; NH largo a circa 11.2 ppm; due picchi a circa 3.5 e 3.3 ppm (acqua/impurezze), segnale intenso a circa 2.5 ppm (DMSO), picco minore a circa 1.9 ppm e riferimento a 0 ppm; picchi minori di impurezze tra 7.7 e 8.0 ppm. I valori ppm sono stimati dall'asse. +- Testo visibile: (ppm) · 12 · 11 · 10 · 9 · 8 · 7 · 6 · 5 · 4 · 3 · 2 · 1 · 0 · 1.00 · 1.00 · 1.01 + +## Contesto nel testo +La simmetria rende equivalenti diversi protoni, riducendo il numero di segnali rispetto agli idrogeni totali. + +Citata in tesi.md alle righe: 762 + +## Da verificare +I valori di ppm sono stimati dall'asse, non letti da etichette sui picchi. + +Esito revisione indipendente: descrizione omette il picco a ~3.5 ppm (alto quanto quello a 3.3) e quello a ~1.9 ppm; solo 3.3 e 2.5 attribuiti + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-045.md b/wiki/figures/fig-045.md new file mode 100644 index 0000000..5218a50 --- /dev/null +++ b/wiki/figures/fig-045.md @@ -0,0 +1,38 @@ +--- +title: "Figura 45 - spettro UV-Visibile e di emissione del prodotto 1 in THF" +type: figure +id: fig-045 +tipo: spectrum_uv_vis +capitolo: "4" +sezione: "4.1" +tesi_loc: "§4.1 r.766" +composti: ["1"] +concetti: ["uv-vis", "fluorescenza", "emissione", "dpp", "thf", "spettro-normalizzato"] +keywords: ["UV-Vis", "fluorescenza", "emissione", "DPP", "THF", "spettro normalizzato"] +confidence: high +flags: [] +verifica: ok +derivata: true +--- + +# Figura 45 + +**Didascalia stampata (testo della tesi):** Figura 45 - spettro UV-Visibile e di emissione del prodotto 1 in THF + +_Posizione: tesi.md §4.1 r.766 (sezione 4.1 Dichetopirrolopirroli), didascalia r.768_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Spettro di assorbimento UV-Visibile (linea continua) e di emissione (tratteggiata) normalizzati del prodotto 1 (DPP di partenza) in THF. + +![[immagini/ba9fb099eb33d86ffd10e40efffc19c6100dc56af328b2442f186b51e09433be.jpg]] + +- Pannello: unico · file `ba9fb099eb33d86ffd10e40efffc19c6100dc56af328b2442f186b51e09433be.jpg` · 1162×706 · confidence high +- Descrizione: Grafico con doppio asse y: assorbanza normalizzata (0-1) a sinistra e intensità normalizzata (0-1) a destra, ascisse lunghezza d'onda 400-700 nm. Curva continua rossa (UV-Visibile) con struttura vibronica: massimo a circa 531 nm, spalla/picco a circa 494 nm, spalla a circa 465 nm. Curva tratteggiata (emissione) con massimo a circa 543 nm e secondo picco a circa 584 nm, spalla a circa 640 nm. +- Testo visibile: Uv-Visibile · Emissione · Assorbanza normalizzata · Intensità normalizzata · Lunghezza d'onda (nm) · 400 · 450 · 500 · 550 · 600 · 650 · 700 + +## Contesto nel testo +Il testo descrive la banda di assorbimento con due massimi a circa 532 e 498 nm, caratteristici del core DPP, e lo spettro di emissione. + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-046.md b/wiki/figures/fig-046.md new file mode 100644 index 0000000..2f7aab1 --- /dev/null +++ b/wiki/figures/fig-046.md @@ -0,0 +1,42 @@ +--- +title: "Figura 46 - meccanismo della reazione di N-alchilazione" +type: figure +id: fig-046 +tipo: mechanism +capitolo: "4" +sezione: "4.1" +tesi_loc: "§4.1 r.778" +composti: ["DPP", "6-bromo-1-esanolo"] +concetti: ["n-alchilazione", "sostituzione-nucleofila-sn2", "t-buok", "6-bromo-1-esanolo", "lattame", "dpp"] +keywords: ["N-alchilazione", "sostituzione nucleofila SN2", "t-BuOK", "6-bromo-1-esanolo", "lattame", "DPP"] +confidence: high +flags: [] +verifica: fix +derivata: true +--- + +# Figura 46 + +**Didascalia stampata (testo della tesi):** Figura 46 - meccanismo della reazione di N-alchilazione + +_Posizione: tesi.md §4.1 r.778 (sezione 4.1 Dichetopirrolopirroli), didascalia r.780_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Meccanismo di N-alchilazione del DPP: deprotonazione del lattame con t-BuOK e attacco nucleofilo sul carbonio legato al bromo del 6-bromo-1-esanolo. + +![[immagini/9b67a0c4119927bb79c04800ab73ca66e034387467484976be81ef31499a5cfb.jpg]] + +- Pannello: unico · file `9b67a0c4119927bb79c04800ab73ca66e034387467484976be81ef31499a5cfb.jpg` · 1034×281 · confidence high +- Descrizione: Schema in tre stadi: DPP con due tiofeni (2-tienil) e due ammidi NH; freccia con t-BuOK verso l'anione amidato (carica negativa sull'azoto); freccia curva dall'azoto al carbonio legato a Br del 6-bromo-1-esanolo (Br-(CH2)6-OH, con freccia di uscita del bromuro); prodotto finale DPP mono-alchilato con catena (CH2)6-OH su un azoto e NH sull'altro. +- Testo visibile: t-BuOK · S · NH · O · Br · HO · OH · 6 · N · HN + +## Contesto nel testo +Il testo spiega che l'azoto ammidico, deprotonato da t-BuOK, attacca il carbonio adiacente al bromo. + +Citata in tesi.md alle righe: 776 + +Esito revisione indipendente: "tioleni" errato (sono tiofeni); alt_text mozzicato + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-047.md b/wiki/figures/fig-047.md new file mode 100644 index 0000000..4d5e8dc --- /dev/null +++ b/wiki/figures/fig-047.md @@ -0,0 +1,42 @@ +--- +title: "Figura 47 - reazione di ciclizzazione del 6-bromo-1-esanolo" +type: figure +id: fig-047 +tipo: reaction_scheme +capitolo: "4" +sezione: "4.1" +tesi_loc: "§4.1 r.784" +composti: ["6-bromo-1-esanolo"] +concetti: ["ciclizzazione-intramolecolare", "reazione-collaterale", "williamson", "base-forte", "ossepano"] +keywords: ["ciclizzazione intramolecolare", "reazione collaterale", "Williamson", "base forte", "ossepano"] +confidence: high +flags: [] +verifica: fix +derivata: true +--- + +# Figura 47 + +**Didascalia stampata (testo della tesi):** Figura 47 - reazione di ciclizzazione del 6-bromo-1-esanolo + +_Posizione: tesi.md §4.1 r.784 (sezione 4.1 Dichetopirrolopirroli), didascalia r.786_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Reazione collaterale di ciclizzazione intramolecolare del 6-bromo-1-esanolo in presenza di base forte, con formazione di ossepano (anello a 7 termini). + +![[immagini/de181218223f66cd046706d8723e5010aa9d7a8779b172c877562b47a100738d.jpg]] + +- Pannello: unico · file `de181218223f66cd046706d8723e5010aa9d7a8779b172c877562b47a100738d.jpg` · 1081×134 · confidence high +- Descrizione: HO-(CH2)6-Br con freccia 'Base forte' verso l'alcossido (O-) che attacca intramolecolarmente il carbonio legato a Br (freccia curva, uscita di Br-), con freccia '-Br-' verso un anello eterociclico a sette termini contenente ossigeno (ossepano). +- Testo visibile: HO · Br · Base forte · O- · -Br- · O + +## Contesto nel testo +Il testo avverte che un eccesso di base favorisce la ciclizzazione indesiderata del 6-bromo-1-esanolo. + +Citata in tesi.md alle righe: 782 + +Esito revisione indipendente: alt_text mozzicato con "…" + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-048.md b/wiki/figures/fig-048.md new file mode 100644 index 0000000..7c4a55e --- /dev/null +++ b/wiki/figures/fig-048.md @@ -0,0 +1,40 @@ +--- +title: "Figura 48 - spettro 1H-NMR in CDCl3 del prodotto 2" +type: figure +id: fig-048 +tipo: spectrum_nmr +capitolo: "4" +sezione: "4.1" +tesi_loc: "§4.1 r.792" +composti: ["2"] +concetti: ["1h-nmr", "cdcl3", "dpp-alchilato", "tiofene", "assegnazione-segnali"] +keywords: ["1H-NMR", "CDCl3", "DPP alchilato", "tiofene", "assegnazione segnali"] +confidence: high +flags: [] +verifica: ok +derivata: true +--- + +# Figura 48 + +**Didascalia stampata (testo della tesi):** Figura 48 - spettro 1H-NMR in CDCl3 del prodotto 2 + +_Posizione: tesi.md §4.1 r.792 (sezione 4.1 Dichetopirrolopirroli), didascalia r.794_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Spettro 1H-NMR in CDCl3 del prodotto 2 (DPP bis-alchilato con catene esanoliche), con assegnazione dei segnali a colori sulla struttura. + +![[immagini/d22ce85e035853dee124b1608b0cb176c370dc95ec3ab560926836261887394e.jpg]] + +- Pannello: unico · file `d22ce85e035853dee124b1608b0cb176c370dc95ec3ab560926836261887394e.jpg` · 1240×865 · confidence high +- Descrizione: Spettro 1H-NMR (asse ppm 12-0). Struttura del DPP con due tiofeni e due catene N-(CH2)6-OH, con protoni colorati. Segnali: rosso circa 8.9 ppm (doppietto, H tiofene vicino al core), blu circa 7.6 ppm, verde circa 7.3 ppm (sovrapposto al CHCl3 a 7.26), viola circa 4.1 ppm (NCH2, tripletto), arancione circa 3.65 ppm (CH2OH), giallo chiaro circa 1.4-1.8 ppm (CH2 centrali). Singoletto intenso del solvente a 7.26 ppm e TMS a 0. +- Testo visibile: HO · OH · 4 · ppm · 12 · 11 · 10 · 9 · 8 · 7 · 6 · 5 · 4 · 3 · 2 · 1 · 0 + +## Contesto nel testo +Il testo commenta la regione aromatica con tre segnali dei protoni tiofenici e il doppietto a circa 8.9 ppm. + +Citata in tesi.md alle righe: 796 + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-049.md b/wiki/figures/fig-049.md new file mode 100644 index 0000000..e5c8158 --- /dev/null +++ b/wiki/figures/fig-049.md @@ -0,0 +1,41 @@ +--- +title: "Figura 49 - spettro FT-IR del prodotto 2" +type: figure +id: fig-049 +tipo: spectrum_ir +capitolo: "4" +sezione: "4.1" +tesi_loc: "§4.1 r.798" +composti: ["2"] +concetti: ["ft-ir", "o-h-stretching", "c-o-lattame", "c-h-alifatici", "dpp"] +keywords: ["FT-IR", "O-H stretching", "C=O lattame", "C-H alifatici", "DPP"] +confidence: high +flags: ["cropped"] +verifica: ok +derivata: true +--- + +# Figura 49 + +**Didascalia stampata (testo della tesi):** Figura 49 - spettro FT-IR del prodotto 2 + +_Posizione: tesi.md §4.1 r.798 (sezione 4.1 Dichetopirrolopirroli), didascalia r.800_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Spettro FT-IR del prodotto 2 (DPP alchilato). + +![[immagini/f890cc2c6264ef44ec1b471578277dc04114da1baa30e1f6aa17bb7f674615e8.jpg]] + +- Pannello: unico · file `f890cc2c6264ef44ec1b471578277dc04114da1baa30e1f6aa17bb7f674615e8.jpg` · 1256×862 · confidence high +- Descrizione: Spettro in trasmittanza (0.40-0.90) vs numero d'onda 3800-500 cm-1 (asse etichettato 'Lunghezza d'onda [cm-1]'). Banda larga OH intorno a 3400 cm-1, segnale debole circa 3080 cm-1 (C-H aromatici), bande C-H alifatici circa 2920 e 2850 cm-1, assorbimento intenso a circa 1640 cm-1 (C=O lattame), numerosi picchi nella regione di impronta, tra cui circa 870 e 720 cm-1. +- Testo visibile: Trasmittanza · Lunghezza d'onda [cm-1] · 3800 · 3600 · 3400 · 3200 · 3000 · 2800 · 2600 · 2400 · 2200 · 2000 · 1800 · 1600 · 1400 · 1200 · 1000 · 800 · 600 +- Flag: cropped + +## Contesto nel testo +Il testo assegna la banda larga a 3400 cm-1 all'OH alcolico terminale e i segnali a 3100 cm-1 ai C-H aromatici. + +Citata in tesi.md alle righe: 802 + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-050.md b/wiki/figures/fig-050.md new file mode 100644 index 0000000..24ef3fe --- /dev/null +++ b/wiki/figures/fig-050.md @@ -0,0 +1,40 @@ +--- +title: "Figura 50 - spettro UV-Visibile e di emissione del prodotto2 in THF" +type: figure +id: fig-050 +tipo: spectrum_uv_vis +capitolo: "4" +sezione: "4.1" +tesi_loc: "§4.1 r.806" +composti: ["2"] +concetti: ["uv-vis", "fluorescenza", "spostamento-batocromico", "dpp-alchilato", "thf"] +keywords: ["UV-Vis", "fluorescenza", "spostamento batocromico", "DPP alchilato", "THF"] +confidence: high +flags: [] +verifica: ok +derivata: true +--- + +# Figura 50 + +**Didascalia stampata (testo della tesi):** Figura 50 - spettro UV-Visibile e di emissione del prodotto2 in THF + +_Posizione: tesi.md §4.1 r.806 (sezione 4.1 Dichetopirrolopirroli), didascalia r.808_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Spettro UV-Visibile e di emissione normalizzati del prodotto 2 in THF. + +![[immagini/75c7d0cf12baae0fe259352e5495ea053607717f5a57233f468098343f6693c7.jpg]] + +- Pannello: unico · file `75c7d0cf12baae0fe259352e5495ea053607717f5a57233f468098343f6693c7.jpg` · 1190×707 · confidence high +- Descrizione: Doppio asse y normalizzato (0-1), ascisse 420-650 nm. Curva continua verde (assorbimento) con massimo a circa 540 nm e spalla/picco a circa 505 nm; curva tratteggiata verde scuro (emissione) con massimo a circa 555 nm e secondo picco a circa 595 nm. +- Testo visibile: Uv-Visibile · Emissione · Assorbanza normalizzata · Intensità normalizzata · Lunghezza d'onda (nm) · 420 · 470 · 520 · 570 · 620 + +## Contesto nel testo +Il testo confronta il prodotto 2 con il 1, riportando spostamento batocromico del massimo da 531 a 541 nm dopo alchilazione. + +Citata in tesi.md alle righe: 804 + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-051.md b/wiki/figures/fig-051.md new file mode 100644 index 0000000..04cd6c0 --- /dev/null +++ b/wiki/figures/fig-051.md @@ -0,0 +1,40 @@ +--- +title: "Figura 51 - retta di calibrazione del fluoroforo 2 per il calcolo di ε" +type: figure +id: fig-051 +tipo: plot +capitolo: "4" +sezione: "4.1" +tesi_loc: "§4.1 r.821" +composti: ["2"] +concetti: ["legge-di-lambert-beer", "calibrazione", "coefficiente-di-estinzione-molare", "chcl3"] +keywords: ["legge di Lambert-Beer", "calibrazione", "coefficiente di estinzione molare", "CHCl3"] +confidence: high +flags: [] +verifica: ok +derivata: true +--- + +# Figura 51 + +**Didascalia stampata (testo della tesi):** Figura 51 - retta di calibrazione del fluoroforo 2 per il calcolo di ε + +_Posizione: tesi.md §4.1 r.821 (sezione 4.1 Dichetopirrolopirroli), didascalia r.823_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Retta di calibrazione assorbanza-concentrazione del fluoroforo 2 per il calcolo del coefficiente di estinzione molare ε. + +![[immagini/336837d03a78ea923cf3fa1ae976385b52eefe8ab91dccfdff63f3bb33ecfc6b.jpg]] + +- Pannello: unico · file `336837d03a78ea923cf3fa1ae976385b52eefe8ab91dccfdff63f3bb33ecfc6b.jpg` · 901×559 · confidence high +- Descrizione: Grafico a dispersione con 4 punti e retta di regressione tratteggiata. Asse x concentrazione (mol/L) 1E-06 - 5E-05, asse y assorbanza 0-0,8. Equazione y = 13218x + 0,0069, R² = 0,9981. Ultimo punto circa 0,67 a circa 4.9E-05 mol/L. +- Testo visibile: y = 13218x + 0,0069 · R² = 0,9981 · Assorbanza · Concentrazione (mol/L) · 1E-06 · 1E-05 · 2E-05 · 3E-05 · 4E-05 · 5E-05 + +## Contesto nel testo +Il testo spiega che ε è calcolato dalla pendenza della retta ottenuta con soluzioni di concentrazione nota in CHCl3. + +Citata in tesi.md alle righe: 819 + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-052.md b/wiki/figures/fig-052.md new file mode 100644 index 0000000..d244b5a --- /dev/null +++ b/wiki/figures/fig-052.md @@ -0,0 +1,40 @@ +--- +title: "Figura 52 - schema di reazione dei copolimeri coniugati" +type: figure +id: fig-052 +tipo: reaction_scheme +capitolo: "4" +sezione: "4.2" +tesi_loc: "§4.2 r.836" +composti: ["2", "3", "3HT"] +concetti: ["polimerizzazione-ossidativa", "fecl3", "3-esiltiofene", "copolimero", "dpp", "nitrometano"] +keywords: ["polimerizzazione ossidativa", "FeCl3", "3-esiltiofene", "copolimero", "DPP", "nitrometano"] +confidence: high +flags: [] +verifica: ok +derivata: true +--- + +# Figura 52 + +**Didascalia stampata (testo della tesi):** Figura 52 - schema di reazione dei copolimeri coniugati + +_Posizione: tesi.md §4.2 r.836 (sezione 4.2 Copolimeri coniugati), didascalia r.838_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Schema di reazione di polimerizzazione ossidativa del fluoroforo 2 con 3-esiltiofene (3HT) con FeCl3 catalitico, che porta al copolimero 3. + +![[immagini/0cc72ddb7b8a730785dfaeb2abb381f6ef486e86e068d50b5d0b0ac0e8bc220d.jpg]] + +- Pannello: unico · file `0cc72ddb7b8a730785dfaeb2abb381f6ef486e86e068d50b5d0b0ac0e8bc220d.jpg` · 1226×248 · confidence high +- Descrizione: Reagente 2 (DPP con due 2-tienil e due catene N-(CH2)6-OH) + 3-esiltiofene; sulla freccia: cat. FeCl3, CHCl3 / CHNO2, T_amb, 1 h. Prodotto 3: copolimero con unità [tiofene-DPP-tiofene]x e [3-esiltiofene (CH2)5CH3]y tra parentesi quadre, numero 3. +- Testo visibile: + · cat. FeCl3 · CHCl3 / CHNO2 · Tamb, 1 h · DPP · x · y · 5 · 2 · 3 · HO · OH + +## Contesto nel testo +Il testo introduce la polimerizzazione ossidativa del fluoroforo 2 con 3HT secondo lo schema di Figura 52. + +Citata in tesi.md alle righe: 834 + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-053.md b/wiki/figures/fig-053.md new file mode 100644 index 0000000..a182f93 --- /dev/null +++ b/wiki/figures/fig-053.md @@ -0,0 +1,42 @@ +--- +title: "Figura 53 - meccanismo di polimerizzazione ossidativa mediante tricloruro ferrico" +type: figure +id: fig-053 +tipo: mechanism +capitolo: "4" +sezione: "4.2" +tesi_loc: "§4.2 r.842" +composti: ["2", "3", "3HT"] +concetti: ["polimerizzazione-ossidativa", "fecl3", "radicale", "accoppiamento-ossidativo", "3-esiltiofene"] +keywords: ["polimerizzazione ossidativa", "FeCl3", "radicale", "accoppiamento ossidativo", "3-esiltiofene"] +confidence: high +flags: [] +verifica: fix +derivata: true +--- + +# Figura 53 + +**Didascalia stampata (testo della tesi):** Figura 53 - meccanismo di polimerizzazione ossidativa mediante tricloruro ferrico + +_Posizione: tesi.md §4.2 r.842 (sezione 4.2 Copolimeri coniugati), didascalia r.844_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Meccanismo di polimerizzazione ossidativa mediante FeCl3: ossidazione del DPP-tiofene a radicale, attacco del 3-esiltiofene e propagazione al copolimero 3. + +![[immagini/34cdcf9d6836a55ee2dd35ac99f5e80cd9dffb87cbfaf818b5257c5ccfed2b51.jpg]] + +- Pannello: unico · file `34cdcf9d6836a55ee2dd35ac99f5e80cd9dffb87cbfaf818b5257c5ccfed2b51.jpg` · 1256×312 · confidence high +- Descrizione: Il composto 2 (tiofene-DPP-tiofene) con Fe3+ / -Fe2+ forma un radicale sul tiofene; il radicale attacca 3-esiltiofene dando l'addotto tiofene-tiofene (con esile); doppia freccia verso il copolimero 3 con unità x e y. +- Testo visibile: Fe3+ · -Fe2+ · DPP · S · 2 · 3 · x · y · 5 + +## Contesto nel testo +Il testo descrive il primo stadio governato dalla reattività di FeCl3 come ossidante in eccesso e il ruolo del nitrometano. + +Citata in tesi.md alle righe: 840 + +Esito revisione indipendente: alt_text mozzicato con "…" + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-054.md b/wiki/figures/fig-054.md new file mode 100644 index 0000000..19ea713 --- /dev/null +++ b/wiki/figures/fig-054.md @@ -0,0 +1,40 @@ +--- +title: "Figura 54 - spettro 1H-NMR del copolimero 3a in CDCl3" +type: figure +id: fig-054 +tipo: spectrum_nmr +capitolo: "4" +sezione: "4.2" +tesi_loc: "§4.2 r.886" +composti: ["3a"] +concetti: ["1h-nmr", "cdcl3", "composizione-copolimero", "integrazione", "3ht", "dpp"] +keywords: ["1H-NMR", "CDCl3", "composizione copolimero", "integrazione", "3HT", "DPP"] +confidence: high +flags: [] +verifica: ok +derivata: true +--- + +# Figura 54 + +**Didascalia stampata (testo della tesi):** Figura 54 - spettro 1H-NMR del copolimero 3a in CDCl3 + +_Posizione: tesi.md §4.2 r.886 (sezione 4.2 Copolimeri coniugati), didascalia r.888_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Spettro 1H-NMR del copolimero 3a in CDCl3, con integrali usati per stimare la composizione DPP/3HT. + +![[immagini/a182a55cad5ef042b39852288ff9f6ae3b5f9c0fd758fd0815f0366e77b09a8e.jpg]] + +- Pannello: unico · file `a182a55cad5ef042b39852288ff9f6ae3b5f9c0fd758fd0815f0366e77b09a8e.jpg` · 1073×851 · confidence high +- Descrizione: Spettro 1H-NMR (ppm 10-0). Segnali aromatici/tiofenici 6.9-7.3 ppm, singoletto intenso a circa 3.45 ppm, segnali a 2.6 (CH2 alfa al tiofene), 1.6, 1.3 e 0.9 ppm (CH3 esile). Integrali evidenziati: 3.44 (circa 4.1 ppm, NCH2 DPP) e 96.56 (circa 0.9 ppm, CH3 3HT). Segnale del solvente a 7.26 ppm. +- Testo visibile: 3.44 · 96.56 · ppm · 10 · 9 · 8 · 7 · 6 · 5 · 4 · 3 · 2 · 1 · 0 + +## Contesto nel testo +Il testo spiega il calcolo della percentuale reale di DPP dai rapporti di aree integrate; i risultati sono in Tabella 6. + +Citata in tesi.md alle righe: 872 + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-055.md b/wiki/figures/fig-055.md new file mode 100644 index 0000000..a55637f --- /dev/null +++ b/wiki/figures/fig-055.md @@ -0,0 +1,40 @@ +--- +title: "Figura 55 - spettro 1H-NMR del copolimero 3b in CDCl3" +type: figure +id: fig-055 +tipo: spectrum_nmr +capitolo: "4" +sezione: "4.2" +tesi_loc: "§4.2 r.890" +composti: ["3b"] +concetti: ["1h-nmr", "cdcl3", "composizione-copolimero", "integrazione"] +keywords: ["1H-NMR", "CDCl3", "composizione copolimero", "integrazione"] +confidence: high +flags: [] +verifica: ok +derivata: true +--- + +# Figura 55 + +**Didascalia stampata (testo della tesi):** Figura 55 - spettro 1H-NMR del copolimero 3b in CDCl3 + +_Posizione: tesi.md §4.2 r.890 (sezione 4.2 Copolimeri coniugati), didascalia r.892_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Spettro 1H-NMR del copolimero 3b in CDCl3, con integrali per il calcolo della composizione. + +![[immagini/5ab89fc3cc83f82abb39c0bfd40b1f0da53a8f88a4ca771e00621a476cf8901d.jpg]] + +- Pannello: unico · file `5ab89fc3cc83f82abb39c0bfd40b1f0da53a8f88a4ca771e00621a476cf8901d.jpg` · 1121×837 · confidence high +- Descrizione: Spettro 1H-NMR (ppm 10-0). Segnali aromatici deboli 6.5-9 ppm (circa 8.9, 8.3, 7.6), segnale a circa 4.1 ppm (NCH2), 3.6 ppm (CH2OH), multipletti 1.2-1.8 ppm, CH3 a circa 0.9 ppm. Integrali: 17.59 (circa 4.1 ppm) e 82.41 (circa 0.9 ppm). Solvente a 7.26 e TMS a 0. +- Testo visibile: 17.59 · 82.41 · ppm · 10 · 9 · 8 · 7 · 6 · 5 · 4 · 3 · 2 · 1 · 0 + +## Contesto nel testo +Il testo riporta gli spettri NMR dei tre copolimeri per determinare la percentuale reale di DPP. + +Citata in tesi.md alle righe: 872 + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-056.md b/wiki/figures/fig-056.md new file mode 100644 index 0000000..2acfb66 --- /dev/null +++ b/wiki/figures/fig-056.md @@ -0,0 +1,40 @@ +--- +title: "Figura 56 - spettro 1H-NMR del copolimero 3c in CDCl3" +type: figure +id: fig-056 +tipo: spectrum_nmr +capitolo: "4" +sezione: "4.2" +tesi_loc: "§4.2 r.894" +composti: ["3c"] +concetti: ["1h-nmr", "cdcl3", "composizione-copolimero", "integrazione"] +keywords: ["1H-NMR", "CDCl3", "composizione copolimero", "integrazione"] +confidence: high +flags: [] +verifica: ok +derivata: true +--- + +# Figura 56 + +**Didascalia stampata (testo della tesi):** Figura 56 - spettro 1H-NMR del copolimero 3c in CDCl3 + +_Posizione: tesi.md §4.2 r.894 (sezione 4.2 Copolimeri coniugati), didascalia r.896_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Spettro 1H-NMR del copolimero 3c in CDCl3, con integrali per il calcolo della composizione. + +![[immagini/f078dd5e0992c244123ad8fcbd08d2f2235bffb15f21adcee16bef8ed40a1f4e.jpg]] + +- Pannello: unico · file `f078dd5e0992c244123ad8fcbd08d2f2235bffb15f21adcee16bef8ed40a1f4e.jpg` · 1090×809 · confidence high +- Descrizione: Spettro 1H-NMR (ppm 10-0). Segnali aromatici a circa 8.9, 8.3, 7.6, 7.2, 6.9 ppm; NCH2 circa 4.1 ppm; singoletto intenso circa 3.45 ppm; CH2OH circa 3.6 ppm; multipletti 1.2-1.8 e CH3 circa 0.9 ppm. Integrali: 41.52 (circa 4.1 ppm) e 58.48 (circa 0.9 ppm). +- Testo visibile: 41.52 · 58.48 · ppm · 10 · 9 · 8 · 7 · 6 · 5 · 4 · 3 · 2 · 1 · 0 + +## Contesto nel testo +Ultimo dei tre spettri NMR dei copolimeri; il testo successivo passa a FT-IR, UV-Vis, GPC e DSC. + +Citata in tesi.md alle righe: 872 + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-057.md b/wiki/figures/fig-057.md new file mode 100644 index 0000000..1c3ca89 --- /dev/null +++ b/wiki/figures/fig-057.md @@ -0,0 +1,46 @@ +--- +title: "Figura 57 - spettro FT-IR dei copolimeri 3a (blu), 3b (verde), 3c (rosso)" +type: figure +id: fig-057 +tipo: spectrum_ir +capitolo: "4" +sezione: "4.2" +tesi_loc: "§4.2 r.900" +composti: ["3a", "3b", "3c"] +concetti: ["ft-ir", "copolimeri", "c-h-alifatici", "3-esiltiofene", "c-o"] +keywords: ["FT-IR", "copolimeri", "C-H alifatici", "3-esiltiofene", "C=O"] +confidence: medium +flags: ["caption_mismatch"] +verifica: fix +derivata: true +--- + +# Figura 57 + +**Didascalia stampata (testo della tesi):** Figura 57 - spettro FT-IR dei copolimeri 3a (blu), 3b (verde), 3c (rosso) + +_Posizione: tesi.md §4.2 r.900 (sezione 4.2 Copolimeri coniugati), didascalia r.902_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Spettri FT-IR sovrapposti dei copolimeri 3a, 3b e 3c. + +![[immagini/4b81d4490846b8b0f24cd7ae9e1ed776036c588345475c519334bef4eb76a684.jpg]] + +- Pannello: unico · file `4b81d4490846b8b0f24cd7ae9e1ed776036c588345475c519334bef4eb76a684.jpg` · 1229×848 · confidence medium +- Descrizione: Tre tracce (blu, rosso, verde) in trasmittanza (tick da 0.0 a 1.0) vs numero d'onda 4000-400 cm-1. Banda larga 3600-3200 cm-1 (più intensa nella traccia verde), C-H alifatici a circa 2920 e 2850 cm-1, forte assorbimento a circa 1650-1700 cm-1 (C=O), bande intense a circa 1030 e 720 cm-1 e piccole bande attorno a 820-860 cm-1. Nessuna legenda nell'immagine; l'assegnazione dei colori ai copolimeri è riportata solo nella didascalia (e in modo diverso nel testo). +- Testo visibile: Trasmittanza · Lunghezza d'onda [cm-1] · 3500 · 3000 · 2500 · 2000 · 1500 · 1000 · 500 · 1.0 · 0.9 · 0.8 · 0.7 · 0.6 · 0.5 · 0.4 · 0.3 · 0.2 · 0.1 · 0.0 +- Flag: caption_mismatch + +## Contesto nel testo +Il testo conferma la copolimerizzazione e cita gli stretching C-H a 2920 e 2850 e il segnale a 820 cm-1 del 3-esiltiofene. + +Citata in tesi.md alle righe: 904 + +## Da verificare +Didascalia (3a blu, 3b verde, 3c rosso) e testo (3a verde, 3b rossa, 3c blu) discordano sui colori; nessuna legenda in immagine. + +Esito revisione indipendente: asse x va da 4000 a 400 cm-1 (non 3900); asse y mostra tick 0.0-1.0 completi; picchi forti a circa 1030 e 720 cm-1; il segnale a 820 e solo una piccola banda (~820-860); colori didascalia (3a blu, 3b verde, 3c rosso) in conflitto con il testo (3a verde, 3b rossa, 3c blu): non verificabile dall'immagine, nessuna legenda + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-058.md b/wiki/figures/fig-058.md new file mode 100644 index 0000000..c0a9663 --- /dev/null +++ b/wiki/figures/fig-058.md @@ -0,0 +1,40 @@ +--- +title: "Figura 58 - spettro UV-Visibile e di emissione del copolimero 3a in THF" +type: figure +id: fig-058 +tipo: spectrum_uv_vis +capitolo: "4" +sezione: "4.2" +tesi_loc: "§4.2 r.908" +composti: ["3a"] +concetti: ["uv-vis", "fluorescenza", "copolimero", "thf"] +keywords: ["UV-Vis", "fluorescenza", "copolimero", "THF"] +confidence: high +flags: [] +verifica: ok +derivata: true +--- + +# Figura 58 + +**Didascalia stampata (testo della tesi):** Figura 58 - spettro UV-Visibile e di emissione del copolimero 3a in THF + +_Posizione: tesi.md §4.2 r.908 (sezione 4.2 Copolimeri coniugati), didascalia r.910_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Spettro UV-Visibile e di emissione normalizzati del copolimero 3a in THF. + +![[immagini/585dc7627f409d974b2dda6d2db2fc8d1febafb609faba20d707f941b23f851c.jpg]] + +- Pannello: unico · file `585dc7627f409d974b2dda6d2db2fc8d1febafb609faba20d707f941b23f851c.jpg` · 1193×693 · confidence high +- Descrizione: Doppio asse normalizzato, ascisse 400-700 nm. Curva continua blu (UV-Visibile): massimo a circa 540 nm, spalla a circa 505 nm, minimo a circa 425 nm con assorbanza 0,25; coda a lunghe lunghezze d'onda. Curva tratteggiata blu scuro (emissione): massimo a circa 548 nm, spalla a circa 590 nm. Senza titolo nel grafico. +- Testo visibile: UV-Visibile · Emissione · Assorbanza normalizzata · Intensità normalizzata · Lunghezza d'onda (nm) · 400 · 450 · 500 · 550 · 600 · 650 · 700 + +## Contesto nel testo +Il testo afferma che i tre copolimeri hanno profili quasi identici, con λmax 540-545 nm. + +Citata in tesi.md alle righe: 906, 920 + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-059.md b/wiki/figures/fig-059.md new file mode 100644 index 0000000..f4e04be --- /dev/null +++ b/wiki/figures/fig-059.md @@ -0,0 +1,40 @@ +--- +title: "Figura 59 - spettro UV-Visibile e di emissione del copolimero 3b in THF" +type: figure +id: fig-059 +tipo: spectrum_uv_vis +capitolo: "4" +sezione: "4.2" +tesi_loc: "§4.2 r.912" +composti: ["3b"] +concetti: ["uv-vis", "fluorescenza", "copolimero", "thf"] +keywords: ["UV-Vis", "fluorescenza", "copolimero", "THF"] +confidence: high +flags: [] +verifica: ok +derivata: true +--- + +# Figura 59 + +**Didascalia stampata (testo della tesi):** Figura 59 - spettro UV-Visibile e di emissione del copolimero 3b in THF + +_Posizione: tesi.md §4.2 r.912 (sezione 4.2 Copolimeri coniugati), didascalia r.914_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Spettro UV-Visibile e di emissione normalizzati del copolimero 3b in THF. + +![[immagini/f8b0852a6a485472cb2438e024374bb56e26d87d86831f40903fd0be201d0771.jpg]] + +- Pannello: unico · file `f8b0852a6a485472cb2438e024374bb56e26d87d86831f40903fd0be201d0771.jpg` · 1196×831 · confidence high +- Descrizione: Titolo 'Copolimero 3b'. Doppio asse normalizzato, ascisse 420-700 nm circa. Curva arancione continua: massimo a circa 540 nm, spalla a circa 505 nm. Curva tratteggiata (emissione): massimo a circa 550 nm, spalla a circa 590 nm. +- Testo visibile: Copolimero 3b · UV-Visibile · Emissione · Assorbanza normalizzata · Intensità normalizzata · Lunghezza d'onda (nm) · 420 · 470 · 520 · 570 · 620 · 670 + +## Contesto nel testo +Insieme a Figure 58 e 60 mostra profili fotofisici simili al DPP di partenza. + +Citata in tesi.md alle righe: 906, 920 + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-060.md b/wiki/figures/fig-060.md new file mode 100644 index 0000000..821bed6 --- /dev/null +++ b/wiki/figures/fig-060.md @@ -0,0 +1,40 @@ +--- +title: "Figura 60 - spettro UV-Visibile e di emissione del copolimero 3c in THF" +type: figure +id: fig-060 +tipo: spectrum_uv_vis +capitolo: "4" +sezione: "4.2" +tesi_loc: "§4.2 r.916" +composti: ["3c"] +concetti: ["uv-vis", "fluorescenza", "copolimero", "thf"] +keywords: ["UV-Vis", "fluorescenza", "copolimero", "THF"] +confidence: high +flags: [] +verifica: ok +derivata: true +--- + +# Figura 60 + +**Didascalia stampata (testo della tesi):** Figura 60 - spettro UV-Visibile e di emissione del copolimero 3c in THF + +_Posizione: tesi.md §4.2 r.916 (sezione 4.2 Copolimeri coniugati), didascalia r.918_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Spettro UV-Visibile e di emissione normalizzati del copolimero 3c in THF. + +![[immagini/2b34f5439b53ddcf7aeff01949aba8f61aa554f29849c81d7c3922f06dd3bba9.jpg]] + +- Pannello: unico · file `2b34f5439b53ddcf7aeff01949aba8f61aa554f29849c81d7c3922f06dd3bba9.jpg` · 1196×837 · confidence high +- Descrizione: Titolo 'Copolimero 3c'. Curva magenta continua: massimo a circa 540 nm, spalla a circa 505 nm, assorbanza a 420 nm circa 0,23. Curva tratteggiata (emissione): massimo a circa 552 nm, spalla a circa 592 nm. Ascisse 420-700 nm. +- Testo visibile: Copolimero 3c · UV-Visibile · Emissione · Assorbanza normalizzata · Intensità normalizzata · Lunghezza d'onda (nm) · 420 · 470 · 520 · 570 · 620 · 670 + +## Contesto nel testo +Il testo osserva che 3a, 3b e 3c in THF mostrano profili quasi identici con λmax 540-545 nm. + +Citata in tesi.md alle righe: 906, 920 + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-061.md b/wiki/figures/fig-061.md new file mode 100644 index 0000000..18fc113 --- /dev/null +++ b/wiki/figures/fig-061.md @@ -0,0 +1,41 @@ +--- +title: "Figura 61 - film solidi dei copolimeri sotto lampada UV, in ordine copolimero 3a, 3b, 3c" +type: figure +id: fig-061 +tipo: photo +capitolo: "4" +sezione: "4.2" +tesi_loc: "§4.2 r.932" +composti: ["3a", "3b", "3c"] +concetti: ["film-solidi", "lampada-uv", "quenching", "aggregazione", "fluorescenza-stato-solido"] +keywords: ["film solidi", "lampada UV", "quenching", "aggregazione", "fluorescenza stato solido"] +confidence: high +flags: ["low_resolution"] +verifica: ok +derivata: true +--- + +# Figura 61 + +**Didascalia stampata (testo della tesi):** Figura 61 - film solidi dei copolimeri sotto lampada UV, in ordine copolimero 3a, 3b, 3c + +_Posizione: tesi.md §4.2 r.932 (sezione 4.2 Copolimeri coniugati), didascalia r.934_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Film solidi dei copolimeri 3a, 3b e 3c sotto lampada UV: l'emissione risulta praticamente assente (quenching da aggregazione). + +![[immagini/efcc22eae8c7e8ff910d35fa7c018b13417126c67a70da70eed1784a889d6d32.jpg]] + +- Pannello: unico · file `efcc22eae8c7e8ff910d35fa7c018b13417126c67a70da70eed1784a889d6d32.jpg` · 1020×343 · confidence high +- Descrizione: Tre fotografie affiancate di film su fondo blu scuro quasi nero, ciascuna con un cerchio giallo tratteggiato che indica l'area del film, senza emissione visibile. Etichette gialle: DPP-3HT (80:20), (50:50), (20:80). +- Testo visibile: DPP-3HT (80:20) · DPP-3HT (50:50) · DPP-3HT (20:80) +- Flag: low_resolution + +## Contesto nel testo +Il testo spiega che allo stato solido l'aggregazione porta a quenching emissivo, criticità per i sistemi lineari. + +Citata in tesi.md alle righe: 930 + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-062.md b/wiki/figures/fig-062.md new file mode 100644 index 0000000..2fa7757 --- /dev/null +++ b/wiki/figures/fig-062.md @@ -0,0 +1,44 @@ +--- +title: "Figura 62 - effetto dell'intensità dello stacking π-π sull'emissione luminosa" +type: figure +id: fig-062 +tipo: diagram +capitolo: "4" +sezione: "4.3" +tesi_loc: "§4.3 r.961" +composti: [] +concetti: ["stacking", "bottle-brush", "quenching", "emissione", "catene-laterali"] +keywords: ["π-π stacking", "bottle brush", "quenching", "emissione", "catene laterali"] +confidence: medium +flags: ["caption_mismatch"] +verifica: ok +derivata: true +--- + +# Figura 62 + +**Didascalia stampata (testo della tesi):** Figura 62 - effetto dell'intensità dello stacking π-π sull'emissione luminosa + +_Posizione: tesi.md §4.3 r.961 (sezione 4.3 Polimeri bottle brush), didascalia r.963_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Schema dell'effetto dell'intensità dello stacking π-π sull'emissione luminosa. + +![[immagini/a3ecc2457962649d36b1824710784bec90b0e52d32275fc154743f9bf9f62339.jpg]] + +- Pannello: unico · file `a3ecc2457962649d36b1824710784bec90b0e52d32275fc154743f9bf9f62339.jpg` · 1021×471 · confidence medium +- Descrizione: Due pannelli. Sinistra: due catene coniugate parallele e vicine (anelli arancioni = tiofeni, esagoni viola = DPP), lampadina barrata, testo 'Deboli interazioni π-π stacking'. Destra: catene con catene laterali verdi ondulate che le tengono distanziate, lampadina accesa, testo 'Forti interazioni π-π stacking'. +- Testo visibile: Deboli interazioni π-π stacking · Forti interazioni π-π stacking +- Flag: caption_mismatch + +## Contesto nel testo +Introduce l'architettura bottle brush per limitare l'impaccamento intermolecolare delle catene. + +## Da verificare +Nel disegno la lampadina barrata sta sotto 'Deboli interazioni' e quella accesa sotto 'Forti interazioni'; il testo non lo spiega. + +Esito revisione indipendente: descrizione fedele; nota: nell'immagine la lampadina accesa e le catene laterali sono associate all'etichetta 'Forti interazioni', in apparente contrasto con il testo (le catene laterali riducono lo stacking): non modificato + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-063.md b/wiki/figures/fig-063.md new file mode 100644 index 0000000..dbd3057 --- /dev/null +++ b/wiki/figures/fig-063.md @@ -0,0 +1,42 @@ +--- +title: "Figura 63 - meccanismo di reazione della ROP con gruppo alcolico come iniziatore" +type: figure +id: fig-063 +tipo: mechanism +capitolo: "4" +sezione: "4.3" +tesi_loc: "§4.3 r.971" +composti: ["PCL", "Sn(Oct)2", "ε-caprolattone"] +concetti: ["rop", "coordinazione-inserzione", "sn-oct-2", "pcl", "caprolattone", "iniziatore-alcolico"] +keywords: ["ROP", "coordinazione-inserzione", "Sn(Oct)2", "PCL", "caprolattone", "iniziatore alcolico"] +confidence: high +flags: [] +verifica: fix +derivata: true +--- + +# Figura 63 + +**Didascalia stampata (testo della tesi):** Figura 63 - meccanismo di reazione della ROP con gruppo alcolico come iniziatore + +_Posizione: tesi.md §4.3 r.971 (sezione 4.3 Polimeri bottle brush), didascalia r.973_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Meccanismo di polimerizzazione per apertura d'anello (ROP) dell'ε-caprolattone con iniziatore alcolico e Sn(Oct)2 (coordinazione-inserzione). + +![[immagini/86add528de15d390b0a228d524bbd008d318d4ae0e85530a063f2df5ddf904ee.jpg]] + +- Pannello: unico · file `86add528de15d390b0a228d524bbd008d318d4ae0e85530a063f2df5ddf904ee.jpg` · 1254×387 · confidence high +- Descrizione: Sn(Oct)2 (2-etilesanoato di stagno, struttura disegnata) + R-OH con perdita di acido 2-etilesanoico (struttura disegnata, con '-') dà l'alcossido Sn-OR; coordinazione dell'ε-caprolattone al centro metallico M (X-M-OR) con stato di transizione indicato da linee tratteggiate rossa e blu e frecce curve; attacco nucleofilo con intermedio tetraedrico (RO, O-M-X); apertura dell'anello a X-M-O-(CH2)5-C(=O)-O-R, quindi propagazione verso la catena [O-(CH2)5-C(=O)]n. +- Testo visibile: Sn · R-OH · X · M · OR · RO · R · O · OH · n + +## Contesto nel testo +Il testo descrive il meccanismo di coordinazione-inserzione catalizzato da stagno ottanoato. + +Citata in tesi.md alle righe: 969 + +Esito revisione indipendente: alt_text troncato con '...'; visible_text '- 2-etilesanoico' non presente come testo: l'acido 2-etilesanoico è disegnato come struttura, con solo '-' e 'OH'; mancano nel visible_text R, RO, OH; descrizione omette frecce curve e linee tratteggiate rosso/blu dello stato di transizione + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-064.md b/wiki/figures/fig-064.md new file mode 100644 index 0000000..3acc3e6 --- /dev/null +++ b/wiki/figures/fig-064.md @@ -0,0 +1,42 @@ +--- +title: "Figura 64 - spettro 1H-NMR del polimero 3.1b in CDCl3" +type: figure +id: fig-064 +tipo: spectrum_nmr +capitolo: "4" +sezione: "4.3" +tesi_loc: "§4.3 r.1002" +composti: ["3.1b", "PCL"] +concetti: ["1h-nmr", "cdcl3", "pcl", "bottle-brush", "rop"] +keywords: ["1H-NMR", "CDCl3", "PCL", "bottle brush", "ROP"] +confidence: high +flags: [] +verifica: fix +derivata: true +--- + +# Figura 64 + +**Didascalia stampata (testo della tesi):** Figura 64 - spettro 1H-NMR del polimero 3.1b in CDCl3 + +_Posizione: tesi.md §4.3 r.1002 (sezione 4.3 Polimeri bottle brush), didascalia r.1004_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Spettro 1H-NMR del polimero bottle brush 3.1b in CDCl3, con i segnali caratteristici del PCL assegnati sulla struttura. + +![[immagini/aae4bec55b3a0f29e1dfa6231c86c1d0295d5d38f2f2e9f0af6a69eba8aa0231.jpg]] + +- Pannello: unico · file `aae4bec55b3a0f29e1dfa6231c86c1d0295d5d38f2f2e9f0af6a69eba8aa0231.jpg` · 1092×721 · confidence high +- Descrizione: Spettro (ppm 12-0). Struttura: DPP con due gruppi 2-tienile e catene N-(CH2)5-O-C(=O)-CH2-(CH2)4-OH (PCL). Punto blu: OCH2 a circa 4.05 ppm (tripletto intenso); punto verde: CH2 alfa al carbonile a circa 2.3 ppm; multipletti a circa 1.65 e 1.38 ppm; piccolo segnale a 3.65 (CH2OH terminale); CHCl3 a 7.26; piccoli segnali a circa 0 ppm. +- Testo visibile: HO · OH · S · N · O · 4 · 5 · ppm · 12 · 11 · 10 · 9 · 8 · 7 · 6 · 5 · 4 · 3 · 2 · 1 · 0 + +## Contesto nel testo +Il testo verifica la polimerizzazione del caprolattone dalla comparsa dei segnali caratteristici del PCL. + +Citata in tesi.md alle righe: 1000 + +Esito revisione indipendente: visible_text incompleto: nella struttura sono leggibili anche S (tiofeni), N, O, i numeri 4 e 5 e due volte HO/OH; il grafico mostra anche segnali a circa 0 ppm (riferimento/impurezze) oltre a 3.65 e 7.26 ppm + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-065.md b/wiki/figures/fig-065.md new file mode 100644 index 0000000..9921ef4 --- /dev/null +++ b/wiki/figures/fig-065.md @@ -0,0 +1,46 @@ +--- +title: "Figura 65 - spettri FT-IR dei polimeri bottle brush ottenuti a partire dal copolimero 3b (verde)" +type: figure +id: fig-065 +tipo: spectrum_ir +capitolo: "4" +sezione: "4.3" +tesi_loc: "§4.3 r.1012" +composti: ["3b", "3.1b", "3.2b", "3.3b", "PCL"] +concetti: ["ft-ir", "pcl", "c-o-estere", "bottle-brush", "oh"] +keywords: ["FT-IR", "PCL", "C=O estere", "bottle brush", "OH"] +confidence: medium +flags: ["caption_mismatch"] +verifica: fix +derivata: true +--- + +# Figura 65 + +**Didascalia stampata (testo della tesi):** Figura 65 - spettri FT-IR dei polimeri bottle brush ottenuti a partire dal copolimero 3b (verde) + +_Posizione: tesi.md §4.3 r.1012 (sezione 4.3 Polimeri bottle brush), didascalia r.1014_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Spettri FT-IR sovrapposti dei polimeri bottle brush derivati dal copolimero 3b (precursore, verde) e dei polimeri 3.1b (arancione), 3.2b (rosa), 3.3b (azzurro). + +![[immagini/4cd08436660a2e3a6f913e54d196a0d183b780c3f5f915be6d22a563771d3e43.jpg]] + +- Pannello: unico · file `4cd08436660a2e3a6f913e54d196a0d183b780c3f5f915be6d22a563771d3e43.jpg` · 1174×829 · confidence medium +- Descrizione: Quattro tracce in trasmittanza (asse y da -0,1 a 1,5) vs 4000-400 cm-1. La traccia verde (precursore 3b) ha banda OH larga a 3600-3200 e C=O attorno a 1650; le tre tracce in alto (arancione 3.1b, magenta 3.2b, blu 3.3b secondo la sottodidascalia) mostrano C-H a 2940 e 2860 cm-1, C=O molto intenso e stretto a circa 1725 cm-1 (estere PCL) e bande C-O a circa 1240 e 1170 cm-1, simili al PCL. Nessuna legenda nell'immagine. +- Testo visibile: Trasmittanza · Lunghezza d'onda [cm-1] · 3500 · 3000 · 2500 · 2000 · 1500 · 1000 · 500 · -0.1 · 0.0 · 0.1 · 0.2 · 0.3 · 0.4 · 0.5 · 0.6 · 0.7 · 0.8 · 0.9 · 1.0 · 1.1 · 1.2 · 1.3 · 1.4 · 1.5 +- Flag: caption_mismatch + +## Contesto nel testo +Il testo evidenzia la scomparsa dell'OH e la crescita dei segnali PCL con l'aumentare delle catene laterali. + +Citata in tesi.md alle righe: 1006 + +## Da verificare +Nessuna legenda in immagine; i colori non combaciano chiaramente con la didascalia. + +Esito revisione indipendente: asse y con tick da -0,1 a 1,5 non riportato; assegnazione colori (arancione 3.1b, rosa 3.2b, azzurro 3.3b) presente nella sottodidascalia del testo ma non in caption/description; il testo dice 'traccia rossa' per il precursore mentre in immagine è verde + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-066.md b/wiki/figures/fig-066.md new file mode 100644 index 0000000..1315a1d --- /dev/null +++ b/wiki/figures/fig-066.md @@ -0,0 +1,46 @@ +--- +title: "Figura 66 - spettri FT-IR dei polimeri bottle brush ottenuti a partire dal copolimero 3c (verde)" +type: figure +id: fig-066 +tipo: spectrum_ir +capitolo: "4" +sezione: "4.3" +tesi_loc: "§4.3 r.1018" +composti: ["3c", "3.1c", "3.2c", "3.3c", "PCL"] +concetti: ["ft-ir", "pcl", "bottle-brush", "c-o-estere"] +keywords: ["FT-IR", "PCL", "bottle brush", "C=O estere"] +confidence: medium +flags: ["caption_mismatch"] +verifica: fix +derivata: true +--- + +# Figura 66 + +**Didascalia stampata (testo della tesi):** Figura 66 - spettri FT-IR dei polimeri bottle brush ottenuti a partire dal copolimero 3c (verde) + +_Posizione: tesi.md §4.3 r.1018 (sezione 4.3 Polimeri bottle brush), didascalia r.1020_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Spettri FT-IR sovrapposti dei polimeri bottle brush derivati dal copolimero 3c (precursore, verde) e dei polimeri 3.1c (arancione), 3.2c (rosa), 3.3c (azzurro). + +![[immagini/d5559d2ff37ffb2861c2ac8eecbade7c09f8fc905c8363be4f48c06a0afae72e.jpg]] + +- Pannello: unico · file `d5559d2ff37ffb2861c2ac8eecbade7c09f8fc905c8363be4f48c06a0afae72e.jpg` · 1176×873 · confidence medium +- Descrizione: Quattro tracce come in Figura 65 (asse y da 0.0 a 1.2): precursore verde con OH largo a 3600-3200 e C=O a circa 1650, e tre tracce in alto (arancione 3.1c, magenta 3.2c, blu 3.3c secondo la sottodidascalia) con C-H a 2940/2860, C=O intenso a circa 1725 cm-1 e picchi C-O a 1240/1170 cm-1. Nessuna legenda. +- Testo visibile: Trasmittanza · Lunghezza d'onda [cm-1] · 3500 · 3000 · 2500 · 2000 · 1500 · 1000 · 500 · 0.0 · 0.1 · 0.2 · 0.3 · 0.4 · 0.5 · 0.6 · 0.7 · 0.8 · 0.9 · 1.0 · 1.1 · 1.2 +- Flag: caption_mismatch + +## Contesto nel testo +Seconda serie di polimeri bottle brush a confronto con il precursore. + +Citata in tesi.md alle righe: 1006 + +## Da verificare +Nessuna legenda in immagine; i colori non combaciano chiaramente con la didascalia. + +Esito revisione indipendente: asse y con tick da 0.0 a 1.2 non riportato; assegnazione colori (arancione 3.1c, rosa 3.2c, azzurro 3.3c) dalla sottodidascalia assente in caption/description + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-067.md b/wiki/figures/fig-067.md new file mode 100644 index 0000000..9802f0d --- /dev/null +++ b/wiki/figures/fig-067.md @@ -0,0 +1,40 @@ +--- +title: "Figura 67 - spettri UV-Visibile (linea continua) e di emissione (linea tratteggiata) dei polimeri bottle brush in THF" +type: figure +id: fig-067 +tipo: spectrum_fluorescence +capitolo: "4" +sezione: "4.3" +tesi_loc: "§4.3 r.1026" +composti: ["3.1b", "3.2b", "3.3b", "3.1c", "3.2c", "3.3c"] +concetti: ["uv-vis", "fluorescenza", "bottle-brush", "thf"] +keywords: ["UV-Vis", "fluorescenza", "bottle brush", "THF"] +confidence: high +flags: [] +verifica: ok +derivata: true +--- + +# Figura 67 + +**Didascalia stampata (testo della tesi):** Figura 67 - spettri UV-Visibile (linea continua) e di emissione (linea tratteggiata) dei polimeri bottle brush in THF + +_Posizione: tesi.md §4.3 r.1026 (sezione 4.3 Polimeri bottle brush), didascalia r.1028_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Spettri UV-Visibile (continua) ed emissione (tratteggiata) normalizzati dei sei polimeri bottle brush 3.1b-3.3b e 3.1c-3.3c in THF. + +![[immagini/be53b102694fafa8036962962c8c0a3735cc1ec95cf721f163b7d25bdd7099fb.png]] + +- Pannello: unico · file `be53b102694fafa8036962962c8c0a3735cc1ec95cf721f163b7d25bdd7099fb.png` · 1005×1235 · confidence high +- Descrizione: Pannello 3x2 con sei grafici a doppio asse (assorbanza e intensità normalizzate, ascisse 400-700 nm): Polimero 3.1b (magenta), 3.1c (verde), 3.2b (arancione), 3.2c (rosso), 3.3b (blu), 3.3c (viola). In ciascuno l'assorbimento ha massimo a circa 545-555 nm con spalla a circa 510 nm e l'emissione ha massimo a circa 557-564 nm con spalla a circa 600-610 nm. +- Testo visibile: Polimero 3.1b · Polimero 3.1c · Polimero 3.2b · Polimero 3.2c · Polimero 3.3b · Polimero 3.3c · Assorbanza normalizzata · Intensità normalizzata · Lunghezza d'onda (nm) + +## Contesto nel testo +Il testo riporta massimi di assorbimento 544-554 nm ed emissione 557-564 nm (Tabella 10). + +Citata in tesi.md alle righe: 1024 + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-068.md b/wiki/figures/fig-068.md new file mode 100644 index 0000000..2ee04cc --- /dev/null +++ b/wiki/figures/fig-068.md @@ -0,0 +1,43 @@ +--- +title: "Figura 68 - esempio di termogramma dei polimeri bottle brush realizzati (in figura l'analisi del campione 3.1c)" +type: figure +id: fig-068 +tipo: plot +capitolo: "4" +sezione: "4.3" +tesi_loc: "§4.3 r.1095" +composti: ["3.1c", "PCL"] +concetti: ["dsc", "fusione", "cristallizzazione", "pcl", "bottle-brush", "termogramma"] +keywords: ["DSC", "fusione", "cristallizzazione", "PCL", "bottle brush", "termogramma"] +confidence: high +flags: [] +verifica: fix +derivata: true +--- + +# Figura 68 + +**Didascalia stampata (testo della tesi):** Figura 68 - esempio di termogramma dei polimeri bottle brush realizzati (in figura l'analisi del campione 3.1c) + +_Posizione: tesi.md §4.3 r.1095 (sezione 4.3 Polimeri bottle brush), didascalia r.1097_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Termogramma DSC del polimero bottle brush 3.1c, con picco di fusione e picco di cristallizzazione del PCL. + +![[immagini/d2ed44d32060aa9ee04e73304940b111e53bf65cf115a93ace696933048e308b.jpg]] + +- Pannello: unico · file `d2ed44d32060aa9ee04e73304940b111e53bf65cf115a93ace696933048e308b.jpg` · 1210×554 · confidence high +- Descrizione: Curva DSC: Heat Flow (W/g) da -4 a 6 vs Temperature (°C) da -20 a 100, convenzione 'Exo Down'. Picco positivo a circa 64 °C (circa 4.8 W/g) e picco negativo a circa 24 °C (circa -2.6 W/g); con Exo Down il primo corrisponde a un processo endotermico (fusione) e il secondo a esotermico (cristallizzazione). Indicato 'Universal V4.5A'. +- Testo visibile: Heat Flow (W/g) · Temperature (°C) · Exo Down · Universal V4.5A · -20 · 0 · 20 · 40 · 60 · 80 · 100 · 6 · 4 · 2 · 0 · -2 · -4 + +## Contesto nel testo +Il testo afferma che le transizioni termiche sono dominate dalle catene di PCL e sono simili per tutti i polimeri. + +## Da verificare +Assegnazione dei picchi (~64 C fusione, ~24 C cristallizzazione) dedotta da 'Exo Down' e dal contesto, non da diciture in immagine. + +Esito revisione indipendente: visible_text omette i tick dell'asse y (-4, -2, 0, 2, 4, 6) + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-069.md b/wiki/figures/fig-069.md new file mode 100644 index 0000000..9723863 --- /dev/null +++ b/wiki/figures/fig-069.md @@ -0,0 +1,40 @@ +--- +title: "Figura 69 - voltammogramma ciclico del polimero 3.2.c registrato a una velocità di scansione di 0,05 V/s in soluzione di THF con TBAPF6 0,1 M" +type: figure +id: fig-069 +tipo: cv_voltammogram +capitolo: "4" +sezione: "4.4.2" +tesi_loc: "§4.4.2 r.1128" +composti: ["3.2c"] +concetti: ["ciclovoltammetria", "potenziale-di-onset", "thf", "tbapf6", "homo-lumo", "0-05-v-s"] +keywords: ["ciclovoltammetria", "potenziale di onset", "THF", "TBAPF6", "HOMO-LUMO", "0.05 V/s"] +confidence: high +flags: [] +verifica: ok +derivata: true +--- + +# Figura 69 + +**Didascalia stampata (testo della tesi):** Figura 69 - voltammogramma ciclico del polimero 3.2.c registrato a una velocità di scansione di 0,05 V/s in soluzione di THF con TBAPF6 0,1 M + +_Posizione: tesi.md §4.4.2 r.1128 (sezione 4.4.2 Metodologie di analisi voltammetrica), didascalia r.1130_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Voltammogramma ciclico del polimero 3.2c a 0.05 V/s in THF con TBAPF6 0.1 M, con tangenti per la determinazione dei potenziali di onset. + +![[immagini/6afc0d601841f25b1c02e27bc6b1616abc101c5f1ceaa0ba9d30ed0f965ebed2.jpg]] + +- Pannello: unico · file `6afc0d601841f25b1c02e27bc6b1616abc101c5f1ceaa0ba9d30ed0f965ebed2.jpg` · 1190×754 · confidence high +- Descrizione: Curva blu corrente (A, da -0,0002 a 0,0002) vs potenziale (V, da -2,5 a 1). Finestra da circa -2,17 a circa +0,63 V. Onda anodica crescente verso +0,5 V (picco circa 0,00017 A), onde catodiche a circa -1,5 e -1,8 V, picco di riduzione a circa +0,2 V. Quattro rette di costruzione per onset: verde e arancione (ossidazione, intorno a 0 V), magenta e gialla (riduzione, intorno a -1,3 V). +- Testo visibile: Corrente (A) · Potenziale (V) · 0,0002 · 0,00015 · 0,0001 · 0,00005 · 0 · -0,00005 · -0,0001 · -0,00015 · -0,0002 · -2,5 · -2 · -1,5 · -1 · -0,5 · 0 · 0,5 · 1 + +## Contesto nel testo +Esempio della procedura di determinazione dei potenziali di onset applicata a tutti i materiali. + +Citata in tesi.md alle righe: 1126, 1148 + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-070.md b/wiki/figures/fig-070.md new file mode 100644 index 0000000..4d87bae --- /dev/null +++ b/wiki/figures/fig-070.md @@ -0,0 +1,40 @@ +--- +title: "Figura 70 - voltammogramma ciclico del polimero 3.2.c registrato a diverse velocità di scansione" +type: figure +id: fig-070 +tipo: cv_voltammogram +capitolo: "4" +sezione: "4.4.2" +tesi_loc: "§4.4.2 r.1136" +composti: ["3.2c"] +concetti: ["ciclovoltammetria", "velocita-di-scansione", "reversibilita", "thf"] +keywords: ["ciclovoltammetria", "velocità di scansione", "reversibilità", "THF"] +confidence: high +flags: [] +verifica: ok +derivata: true +--- + +# Figura 70 + +**Didascalia stampata (testo della tesi):** Figura 70 - voltammogramma ciclico del polimero 3.2.c registrato a diverse velocità di scansione + +_Posizione: tesi.md §4.4.2 r.1136 (sezione 4.4.2 Metodologie di analisi voltammetrica), didascalia r.1138_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Voltammogrammi ciclici del polimero 3.2c a diverse velocità di scansione (0.05, 0.1, 0.5, 1 V/s). + +![[immagini/5491a0651d00b47f168b335586b4f144e1b25834ff74113ff26b1d3a2c8cc991.jpg]] + +- Pannello: unico · file `5491a0651d00b47f168b335586b4f144e1b25834ff74113ff26b1d3a2c8cc991.jpg` · 1076×704 · confidence high +- Descrizione: Quattro CV sovrapposti, corrente (A) vs potenziale (V), da circa -2,17 a +0,63 V. Legenda: 0.05 V/s (arancione), 0.1 V/s (verde), 0.5 V/s (magenta), 1 V/s (azzurro). Le correnti diminuiscono al crescere della velocità; la traccia a 0.05 V/s mostra le onde più marcate (anodica a circa +0,5 V, riduzioni a circa -1,5 e -1,8 V). +- Testo visibile: Corrente (A) · Potenziale (V) · 0.05 V/s · 0.1 V/s · 0.5 V/s · 1 V/s · 0,0002 · -0,0002 · -2,5 · 1 + +## Contesto nel testo +Il testo osserva l'assenza di onde di scarica simmetriche al ritorno e la progressiva diminuzione delle correnti con la velocità. + +Citata in tesi.md alle righe: 1140 + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-071.md b/wiki/figures/fig-071.md new file mode 100644 index 0000000..5ebac8a --- /dev/null +++ b/wiki/figures/fig-071.md @@ -0,0 +1,40 @@ +--- +title: "Figura 71 - correlazione tra bandgap elettrochimico e frazione reale di DPP nei copolimeri sintetizzati" +type: figure +id: fig-071 +tipo: plot +capitolo: "4" +sezione: "4.4.3" +tesi_loc: "§4.4.3 r.1193" +composti: ["DPP"] +concetti: ["ciclovoltammetria", "bandgap-elettrochimico", "frazione-reale-dpp", "copolimeri-lineari"] +keywords: ["ciclovoltammetria", "bandgap elettrochimico", "frazione reale DPP", "copolimeri lineari"] +confidence: high +flags: [] +verifica: ok +derivata: true +--- + +# Figura 71 + +**Didascalia stampata (testo della tesi):** Figura 71 - correlazione tra bandgap elettrochimico e frazione reale di DPP nei copolimeri sintetizzati + +_Posizione: tesi.md §4.4.3 r.1193 (sezione 4.4.3 Proprietà elettrochimiche dei copolimeri lienari), didascalia r.1195_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Correlazione tra bandgap elettrochimico (eV) e frazione reale di DPP nei copolimeri sintetizzati: il bandgap cresce con il contenuto di DPP. + +![[immagini/6c7bd8393eb8c1a329f65b7fc74e5f338a866e514455c0122a43d13ca340ded5.jpg]] + +- Pannello: unico · file `6c7bd8393eb8c1a329f65b7fc74e5f338a866e514455c0122a43d13ca340ded5.jpg` · 940×570 · confidence high +- Descrizione: Grafico a dispersione con tre punti blu e linea di tendenza lineare tratteggiata. Asse x: Frazione reale DPP (0,24-0,36); asse y: Bandgap elettrochimico (eV) (0,8-1,5). Punti approssimativi: (0,25; ~0,97), (0,32; ~1,32), (0,35; ~1,37). Andamento crescente. +- Testo visibile: Bandgap elettrochimico (eV) · Frazione reale DPP · 0,24 · 0,26 · 0,28 · 0,3 · 0,32 · 0,34 · 0,36 · 0,8 · 0,9 · 1 · 1,1 · 1,2 · 1,3 · 1,4 · 1,5 + +## Contesto nel testo +Il testo illustra la correlazione sperimentale tra ampiezza del bandgap e frazione reale di DPP: all'aumentare del DPP il bandgap si allarga. + +Citata in tesi.md alle righe: 1191 + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-072.md b/wiki/figures/fig-072.md new file mode 100644 index 0000000..6bf70f4 --- /dev/null +++ b/wiki/figures/fig-072.md @@ -0,0 +1,38 @@ +--- +title: "Figura 72 - correlazione tra Epicco e frazione reale di DPP nei copolimeri sintetizzati" +type: figure +id: fig-072 +tipo: plot +capitolo: "4" +sezione: "4.4.3" +tesi_loc: "§4.4.3 r.1205" +composti: ["DPP"] +concetti: ["ciclovoltammetria", "potenziale-di-picco", "drogaggio-n", "ossidazione-riduzione"] +keywords: ["ciclovoltammetria", "potenziale di picco", "drogaggio n", "ossidazione/riduzione"] +confidence: high +flags: [] +verifica: ok +derivata: true +--- + +# Figura 72 + +**Didascalia stampata (testo della tesi):** Figura 72 - correlazione tra Epicco e frazione reale di DPP nei copolimeri sintetizzati + +_Posizione: tesi.md §4.4.3 r.1205 (sezione 4.4.3 Proprietà elettrochimiche dei copolimeri lienari), didascalia r.1207_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Potenziali di picco anodico e catodico in funzione della frazione reale di DPP nei copolimeri sintetizzati. + +![[immagini/d7a3694f2d97dcaa84465aeed07d8d26adca6a8f8ed64f7ea2bf86943b918b66.jpg]] + +- Pannello: unico · file `d7a3694f2d97dcaa84465aeed07d8d26adca6a8f8ed64f7ea2bf86943b918b66.jpg` · 937×584 · confidence high +- Descrizione: Grafico a dispersione, asse x Frazione reale DPP (0,22-0,36), asse y Epicco (V) da -2 a 0,5. Serie anodica (verde): ~0,38 V a 0,25, ~0,20 a 0,32, ~0,23 a 0,35. Serie catodica (magenta): ~-1,02 V a 0,25, ~-1,81 a 0,32, ~-1,63 a 0,35. Valori approssimati dal grafico. +- Testo visibile: Epicco (V) · Frazione reale DPP · E picco anodico · E picco catodico · 0,5 · 0 · -0,5 · -1 · -1,5 · -2 · 0,22 · 0,36 + +## Contesto nel testo +Il testo commenta che il potenziale di picco catodico si sposta verso valori molto più negativi all'aumentare del DPP, mentre quello anodico varia meno. + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-073.md b/wiki/figures/fig-073.md new file mode 100644 index 0000000..364a214 --- /dev/null +++ b/wiki/figures/fig-073.md @@ -0,0 +1,40 @@ +--- +title: "Figura 73 - correlazione tra Eonset e frazione reale di DPP nei copolimeri sintetizzati" +type: figure +id: fig-073 +tipo: plot +capitolo: "4" +sezione: "4.4.3" +tesi_loc: "§4.4.3 r.1217" +composti: ["DPP"] +concetti: ["ciclovoltammetria", "potenziale-di-onset", "homo-lumo"] +keywords: ["ciclovoltammetria", "potenziale di onset", "HOMO/LUMO"] +confidence: high +flags: [] +verifica: ok +derivata: true +--- + +# Figura 73 + +**Didascalia stampata (testo della tesi):** Figura 73 - correlazione tra Eonset e frazione reale di DPP nei copolimeri sintetizzati + +_Posizione: tesi.md §4.4.3 r.1217 (sezione 4.4.3 Proprietà elettrochimiche dei copolimeri lienari), didascalia r.1219_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Potenziali di onset anodico e catodico in funzione della frazione reale di DPP nei copolimeri sintetizzati. + +![[immagini/b2931ebedd31df7df3b344c25fcbb4a64aceb7b356181adecf39363e49dcb0fe.jpg]] + +- Pannello: unico · file `b2931ebedd31df7df3b344c25fcbb4a64aceb7b356181adecf39363e49dcb0fe.jpg` · 945×587 · confidence high +- Descrizione: Grafico a dispersione, asse x Frazione reale DPP (0,22-0,36), asse y Eonset (V) da -1,5 a 0,5. Serie anodica (verde): ~0,24 V a 0,25, ~0,05 a 0,32, ~0,00 a 0,35. Serie catodica (magenta): ~-0,73 V a 0,25, ~-1,26 a 0,32, ~-1,37 a 0,35. Valori approssimati. +- Testo visibile: Eonset (V) · Frazione reale DPP · Eonset anodico · E onset catodico · 0,5 · 0 · -0,5 · -1 · -1,5 · 0,22 · 0,36 + +## Contesto nel testo +Il testo indica che l'onset catodico (LUMO) si sposta fortemente verso valori negativi, in linea con i potenziali di picco. + +Citata in tesi.md alle righe: 1221 + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-074.md b/wiki/figures/fig-074.md new file mode 100644 index 0000000..506adf6 --- /dev/null +++ b/wiki/figures/fig-074.md @@ -0,0 +1,42 @@ +--- +title: "Figura 74 - confronto tra spettri UV-Vis (in nero) ed emissione (in rosso) del polimero 3.2.b in soluzione (linea continua) e allo stato solido (linea tratteggiata)" +type: figure +id: fig-074 +tipo: spectrum_uv_vis +capitolo: "4" +sezione: "4.5" +tesi_loc: "§4.5 r.1268" +composti: ["3.2b"] +concetti: ["uv-vis", "fluorescenza", "stato-solido", "soluzione", "bottle-brush", "red-shift"] +keywords: ["UV-Vis", "fluorescenza", "stato solido", "soluzione", "bottle brush", "red shift"] +confidence: high +flags: [] +verifica: fix +derivata: true +--- + +# Figura 74 + +**Didascalia stampata (testo della tesi):** Figura 74 - confronto tra spettri UV-Vis (in nero) ed emissione (in rosso) del polimero 3.2.b in soluzione (linea continua) e allo stato solido (linea tratteggiata) + +_Posizione: tesi.md §4.5 r.1268 (sezione 4.5 Caratterizzazione spettroscopica allo stato solido), didascalia r.1270_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Spettri UV-Vis (nero) ed emissione (rosso) del polimero 3.2b in soluzione (linea continua) e allo stato solido (tratteggio). + +![[immagini/04f625a8b25744bf2d07d569e55558174b59a5cb564c8bdd0a53c704dfbde545.jpg]] + +- Pannello: unico · file `04f625a8b25744bf2d07d569e55558174b59a5cb564c8bdd0a53c704dfbde545.jpg` · 965×648 · confidence high +- Descrizione: Doppio asse y: Normalized Absorbance (sinistra, 0-1) e Normalized Intensity (destra, rosso), asse x Wavelength (nm) 400-900. Assorbimento LS (nero continuo): massimo ~550 nm con spalla ~510 nm; SS (nero tratteggiato): massimo ~550 nm (circa 0.95) e secondo massimo ~580 nm (circa 0.8), con assorbimento nullo oltre ~650 nm. Emissione LS (rossa continua): massimo ~562 nm e spalla ~605 nm; emissione SS (rossa tratteggiata): massimo ~655 nm, spalle a ~580 e ~800 nm, nettamente spostata verso il rosso. Legenda LS (continua), SS (tratteggio). +- Testo visibile: Normalized Absorbance · Normalized Intensity · Wavelength (nm) · LS · SS · 400 · 500 · 600 · 700 · 800 · 900 + +## Contesto nel testo +Confronto delle proprietà ottiche in soluzione (LS) e allo stato solido (SS) per il polimero bottle brush 3.2.b per valutare l'effetto dell'impaccamento. + +Citata in tesi.md alle righe: 1266 + +Esito revisione indipendente: nome composto '3.2.b' incoerente con '3.2b' usato nelle altre figure/tabelle; emissione SS ha spalle a circa 580 nm (~0.28) e a circa 790-800 nm (~0.27); descrizione cita solo 800; assorbimento SS: massimo ~550 nm (0.95) e secondo massimo ~580 nm (0.81); il testo parla di massimo a 570-580 nm: discrepanza testo/immagine + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-x-136800.md b/wiki/figures/fig-x-136800.md new file mode 100644 index 0000000..7976267 --- /dev/null +++ b/wiki/figures/fig-x-136800.md @@ -0,0 +1,44 @@ +--- +title: "fig-x-136800 - composizione dei polimeri bottle brush" +type: figure +id: fig-x-136800 +tipo: reaction_scheme +capitolo: "3" +sezione: "3.2" +tesi_loc: "§3.2 r.648" +composti: ["3b", "3c", "PCL", "caprolattone"] +concetti: ["rop", "poli-epsilon-caprolattone", "sn-oct-2", "bottle-brush", "grafting-from"] +keywords: ["ROP", "poli(epsilon-caprolattone)", "Sn(Oct)2", "bottle brush", "grafting from"] +confidence: high +flags: ["caption_mismatch"] +verifica: fix +derivata: true +--- + +# fig-x-136800 + +**Didascalia stampata (testo della tesi):** Tabella 4 - composizione dei polimeri bottle brush + +_Posizione: tesi.md §3.2 r.648 (sezione 3.2 Sintesi e procedure), didascalia r.661_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Polimerizzazione ad apertura di anello di epsilon-caprolattone sui gruppi OH dei copolimeri DPP-3HT per ottenere i polimeri bottle brush con catene di PCL. + +![[immagini/136800375cf0b441570672093e255d90a47c45a009bd254929fb74b1f17b382d.jpg]] + +- Pannello: unico · file `136800375cf0b441570672093e255d90a47c45a009bd254929fb74b1f17b382d.jpg` · 1256×229 · confidence high +- Descrizione: Copolimero con unità DPP (catene (CH2)6-OH) e 3-esiltiofene + epsilon-caprolattone, Sn(Oct)2, toluene anidro, N2, 110 C, 4 h; prodotto con catene O-[C(=O)-(CH2)5-O]n-H innestate sui bracci (CH2)6. +- Testo visibile: Sn(Oct)2, PhMe anidro · N2, 110 °C, 4h · 6 · 5 · HO · OH · O · S +- Flag: caption_mismatch + +## Contesto nel testo +Il testo parla di sintesi di bottle brush da 3b e 3c; la Tabella 4 stampata è riportata come testo mentre questo file è lo schema di reazione. + +## Da verificare +Il testo della tesi (riga ~663) indica 24 h di reflusso, lo schema riporta 4 h; la descrizione segue l'immagine. + +Esito revisione indipendente: alt_text mozzicato con "…" + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-x-185efd.md b/wiki/figures/fig-x-185efd.md new file mode 100644 index 0000000..a79ea5d --- /dev/null +++ b/wiki/figures/fig-x-185efd.md @@ -0,0 +1,40 @@ +--- +title: "fig-x-185efd" +type: figure +id: fig-x-185efd +tipo: reaction_scheme +capitolo: "3" +sezione: "3.2" +tesi_loc: "§3.2 r.590" +composti: ["1"] +concetti: ["sintesi-dpp", "pseudo-stobbe", "diisopropil-succinato", "t-amona", "fecl3"] +keywords: ["sintesi DPP", "pseudo-Stobbe", "diisopropil succinato", "t-AmONa", "FeCl3"] +confidence: high +flags: [] +verifica: fix +derivata: true +--- + +# fig-x-185efd + +**Didascalia stampata (testo della tesi):** n/d + +_Posizione: tesi.md §3.2 r.590 (sezione 3.2 Sintesi e procedure)_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Sintesi del DPP 1 da 2-tiofencarbonitrile e diisopropil succinato in t-AmOH/t-AmONa con FeCl3 catalitico. + +![[immagini/185efd9de96189fb7fefd271e19709d672e7eda09572a645d13092c3196248e1.jpg]] + +- Pannello: unico · file `185efd9de96189fb7fefd271e19709d672e7eda09572a645d13092c3196248e1.jpg` · 1148×312 · confidence high +- Descrizione: 2-tiofencarbonitrile + diisopropil succinato, condizioni 110 °C, 18 h, t-AmOH/t-AmONa, FeCl3 cat.; prodotto 1: 3,6-di(tiofen-2-il)-2,5-diidropirrolo[3,4-c]pirrolo-1,4-dione con due NH e due C=O. +- Testo visibile: C≡N · 110°C, 18h · t-AmOH/t-AmONa · FeCl3 cat. · 1 · S · NH · O + +## Contesto nel testo +Parte sperimentale: sintesi del composto 1 in pallone con Na, t-AmOH e FeCl3 catalitico a 80 C, poi aggiunta di succinato. + +Esito revisione indipendente: '110 C' senza simbolo di grado nella description + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-x-cc3f54.md b/wiki/figures/fig-x-cc3f54.md new file mode 100644 index 0000000..80f7908 --- /dev/null +++ b/wiki/figures/fig-x-cc3f54.md @@ -0,0 +1,39 @@ +--- +title: "fig-x-cc3f54 - composizione dei copolimeri" +type: figure +id: fig-x-cc3f54 +tipo: reaction_scheme +capitolo: "3" +sezione: "3.2" +tesi_loc: "§3.2 r.630" +composti: ["2", "3a", "3b", "3c", "3HT"] +concetti: ["polimerizzazione-ossidativa", "fecl3", "p3ht", "copolimero-dpp-3ht"] +keywords: ["polimerizzazione ossidativa", "FeCl3", "P3HT", "copolimero DPP-3HT"] +confidence: high +flags: ["caption_mismatch"] +verifica: ok +derivata: true +--- + +# fig-x-cc3f54 + +**Didascalia stampata (testo della tesi):** Tabella 3 - composizione dei copolimeri + +_Posizione: tesi.md §3.2 r.630 (sezione 3.2 Sintesi e procedure), didascalia r.640_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Copolimerizzazione ossidativa del DPP 2 con 3-esiltiofene (3HT) con FeCl3 per dare i copolimeri 3a/3b/3c. Il file è uno schema, non la Tabella 3. + +![[immagini/cc3f5409e11922aee7835c8eb96ff0f9826afea68af08f1473159279af625b8a.jpg]] + +- Pannello: unico · file `cc3f5409e11922aee7835c8eb96ff0f9826afea68af08f1473159279af625b8a.jpg` · 1215×259 · confidence high +- Descrizione: DPP 2 + 3-esiltiofene; cat. FeCl3, CHCl3/CHNO2, T ambiente, 1 h. Prodotto: copolimero con unità tiofene-DPP-tiofene (x) e unità 3-esiltiofene (y, catena laterale con (CH2)5), etichettato 3a/3b/3c. +- Testo visibile: cat. FeCl3 · CHCl3 / CHNO2 · Tamb, 1 h · 2 · 3a / 3b / 3c · DPP · x · y · 5 +- Flag: caption_mismatch + +## Contesto nel testo +Il testo cita la Tabella 3 (composizione dei copolimeri) ma l'immagine è lo schema di sintesi; la tabella è riportata come testo. + +## Collegamenti +- [[tesi]] diff --git a/wiki/figures/fig-x-f6eeb1.md b/wiki/figures/fig-x-f6eeb1.md new file mode 100644 index 0000000..e974a2f --- /dev/null +++ b/wiki/figures/fig-x-f6eeb1.md @@ -0,0 +1,40 @@ +--- +title: "fig-x-f6eeb1" +type: figure +id: fig-x-f6eeb1 +tipo: reaction_scheme +capitolo: "3" +sezione: "3.2" +tesi_loc: "§3.2 r.610" +composti: ["1", "2"] +concetti: ["n-alchilazione", "6-bromoesanolo", "dmso", "t-buok"] +keywords: ["N-alchilazione", "6-bromoesanolo", "DMSO", "t-BuOK"] +confidence: high +flags: [] +verifica: fix +derivata: true +--- + +# fig-x-f6eeb1 + +**Didascalia stampata (testo della tesi):** n/d + +_Posizione: tesi.md §3.2 r.610 (sezione 3.2 Sintesi e procedure)_ + +> Sotto: contenuto generato guardando l'immagine, non verificato una per una. + +**Didascalia generata:** Alchilazione del DPP 1 con 6-bromoesan-1-olo (DMSO, t-BuOK, 40 °C, 16 h) a dare il DPP 2 con due catene idrossiesiliche. + +![[immagini/f6eeb10de88591bd0358f146073c675489133b4c8bb70f71131b343bb8a25794.jpg]] + +- Pannello: unico · file `f6eeb10de88591bd0358f146073c675489133b4c8bb70f71131b343bb8a25794.jpg` · 1298×270 · confidence high +- Descrizione: DPP 1 + 2 equivalenti di Br-(CH2)6-OH; condizioni 40 °C, 16 h, DMSO, t-BuOK; prodotto 2 con due catene N-(CH2)6-OH sugli azoti. +- Testo visibile: 1 · 2 · + 2 · Br · OH · 40°C, 16h · DMSO, t-BuOK · HO · S + +## Contesto nel testo +Parte sperimentale: sintesi del 2,5-bis(6-idrossiesil)-3,6-di(tiofen-2-il)DPP (2) a partire da 1 in DMSO. + +Esito revisione indipendente: '40 C' senza simbolo di grado in caption/alt_text/description + +## Collegamenti +- [[tesi]] diff --git a/wiki/overview.md b/wiki/overview.md new file mode 100644 index 0000000..6ba7626 --- /dev/null +++ b/wiki/overview.md @@ -0,0 +1,19 @@ +--- +title: Overview +type: overview +tags: [overview] +created: 2026-10-09 +updated: 2026-10-09 +sources: +status: draft +--- + +# Overview + +Tema e research question: _da definire alla prima ingest._ + +## Stato della sintesi +Nessuna fonte ancora ingerita. + +## Collegamenti +- [[index]] diff --git a/wiki/techniques/.gitkeep b/wiki/techniques/.gitkeep new file mode 100644 index 0000000..e69de29 diff --git a/wiki/tesi.md b/wiki/tesi.md new file mode 100644 index 0000000..122b5d3 --- /dev/null +++ b/wiki/tesi.md @@ -0,0 +1,25 @@ +--- +title: Tesi - mappa +type: overview +tags: [tesi, mappa] +created: 2026-10-09 +updated: 2026-10-09 +tesi_loc: "r.1-1411" +status: draft +--- + +# Tesi - mappa + +Sintesi e caratterizzazione di copolimeri bottle brush foto-elettro attivi (Aurora Luzi, rel. Stefano Scurti, a.a. 2025-2026). Sorgente: `raw/tesi.md`. + +| Capitolo | Riga | Sezioni | Pagine wiki | +|---|---|---|---| +| 1 Introduzione | 66 | 1.1 Dichetopirrolopirroli (69), 1.2 Fluorescenza (376), 1.3 Fluorofori in materiali polimerici (479), 1.4 Applicazioni (502) | da fare | +| 2 Scopo | 545 | - | da fare | +| 3 Procedure sperimentali | 562 | 3.1 Materiali e metodi (565), 3.2 Sintesi e procedure (586), 3.3 Principi teorici della ciclovoltammetria (666), 3.4 Procedure voltammetriche (702) | da fare | +| 4 Discussione dei risultati | 717 | 4.1 DPP (722), 4.2 Copolimeri coniugati (826), 4.3 Bottle brush (957), 4.4 Ciclovoltammetrie (1100), 4.5 Caratterizzazione spettroscopica allo stato solido (1254) | da fare | +| 5 Conclusioni | 1279 | - | da fare | + +## Collegamenti +- [[overview]] +- [[index]] From af88e23d3aa32ed5a9b3f5ece2a0cba24cec6aaa Mon Sep 17 00:00:00 2001 From: Davide Grilli Date: Fri, 9 Oct 2026 19:21:52 +0200 Subject: [PATCH 2/5] Ingest della tesi: concetti, composti, tecniche, difetti noti e bibliografia - Aggiunge 10 pagine concetto, 5 composti e 6 tecniche, riorganizzate per argomento con tesi_loc e righe di raw/tesi.md - Incorpora le figure (embed e link alle note) nelle pagine pertinenti - Aggiunge overview, mappa wiki/tesi.md, difetti-noti (incoerenze rilevate) e bibliografia generata (scripts/gen_bibliografia.py) - Rigenera le note figura con avviso per caption_mismatch; aggiorna CLAUDE.md, index.md e log.md Co-Authored-By: Claude Sonnet 5.5 --- .obsidian/graph.json | 2 +- CLAUDE.md | 10 +- index.md | 31 +++- log.md | 13 ++ scripts/gen_bibliografia.py | 29 +++ scripts/gen_figures.py | 2 + wiki/analyses/difetti-noti.md | 66 +++++++ wiki/bibliografia.md | 79 +++++++++ wiki/compounds/bottle-brush-3-x.md | 137 ++++++++++++++ wiki/compounds/copolimeri-3a-3b-3c.md | 120 +++++++++++++ wiki/compounds/dpp-1.md | 91 ++++++++++ wiki/compounds/dpp-2.md | 102 +++++++++++ wiki/compounds/reagenti-e-materiali.md | 41 +++++ wiki/concepts/acq-e-stato-solido.md | 70 ++++++++ wiki/concepts/bottle-brush.md | 57 ++++++ wiki/concepts/dpp-reattivita.md | 128 ++++++++++++++ wiki/concepts/dpp-sintesi-letteratura.md | 123 +++++++++++++ wiki/concepts/dpp-struttura-e-proprieta.md | 84 +++++++++ wiki/concepts/fluorescenza.md | 102 +++++++++++ wiki/concepts/fluorofori-in-polimeri.md | 51 ++++++ ...optoelettronica-oled-donatore-accettore.md | 62 +++++++ .../polimerizzazione-ossidativa-fecl3.md | 61 +++++++ wiki/concepts/rop-pcl.md | 54 ++++++ wiki/figures/fig-009.md | 2 + wiki/figures/fig-026.md | 2 + wiki/figures/fig-027.md | 2 + wiki/figures/fig-029.md | 2 + wiki/figures/fig-057.md | 2 + wiki/figures/fig-062.md | 2 + wiki/figures/fig-065.md | 2 + wiki/figures/fig-066.md | 2 + wiki/figures/fig-x-136800.md | 2 + wiki/figures/fig-x-cc3f54.md | 2 + wiki/overview.md | 41 ++++- wiki/techniques/ciclovoltammetria.md | 167 ++++++++++++++++++ wiki/techniques/dsc.md | 31 ++++ wiki/techniques/ft-ir.md | 41 +++++ wiki/techniques/gpc.md | 40 +++++ wiki/techniques/nmr-1h.md | 61 +++++++ wiki/techniques/uv-vis-fluorescenza.md | 48 +++++ wiki/tesi.md | 53 ++++-- 41 files changed, 1994 insertions(+), 23 deletions(-) create mode 100644 scripts/gen_bibliografia.py create mode 100644 wiki/analyses/difetti-noti.md create mode 100644 wiki/bibliografia.md create mode 100644 wiki/compounds/bottle-brush-3-x.md create mode 100644 wiki/compounds/copolimeri-3a-3b-3c.md create mode 100644 wiki/compounds/dpp-1.md create mode 100644 wiki/compounds/dpp-2.md create mode 100644 wiki/compounds/reagenti-e-materiali.md create mode 100644 wiki/concepts/acq-e-stato-solido.md create mode 100644 wiki/concepts/bottle-brush.md create mode 100644 wiki/concepts/dpp-reattivita.md create mode 100644 wiki/concepts/dpp-sintesi-letteratura.md create mode 100644 wiki/concepts/dpp-struttura-e-proprieta.md create mode 100644 wiki/concepts/fluorescenza.md create mode 100644 wiki/concepts/fluorofori-in-polimeri.md create mode 100644 wiki/concepts/optoelettronica-oled-donatore-accettore.md create mode 100644 wiki/concepts/polimerizzazione-ossidativa-fecl3.md create mode 100644 wiki/concepts/rop-pcl.md create mode 100644 wiki/techniques/ciclovoltammetria.md create mode 100644 wiki/techniques/dsc.md create mode 100644 wiki/techniques/ft-ir.md create mode 100644 wiki/techniques/gpc.md create mode 100644 wiki/techniques/nmr-1h.md create mode 100644 wiki/techniques/uv-vis-fluorescenza.md diff --git a/.obsidian/graph.json b/.obsidian/graph.json index 42a46ec..be925e9 100644 --- a/.obsidian/graph.json +++ b/.obsidian/graph.json @@ -17,6 +17,6 @@ "repelStrength": 10, "linkStrength": 1, "linkDistance": 250, - "scale": 1, + "scale": 0.25883865621816243, "close": true } \ No newline at end of file diff --git a/CLAUDE.md b/CLAUDE.md index 06aef50..7803cc9 100644 --- a/CLAUDE.md +++ b/CLAUDE.md @@ -32,10 +32,11 @@ Convenzioni di `tesi.md`: decimali con la virgola; codici composto con il punto CLAUDE.md index.md log.md raw/ immutabile (vedi sopra) scripts/gen_figures.py genera wiki/figures/ da raw/immagini.json +scripts/gen_bibliografia.py genera wiki/bibliografia.md da raw/bibliografia.json wiki/ overview.md sintesi evolutiva, research question, risultati tesi.md mappa capitolo/sezione → pagine wiki (unica pagina "source" della tesi) - bibliografia.md i 59 riferimenti raggruppati per tema, con link alle schede raw/fonti/ + bibliografia.md i 59 riferimenti (GENERATA dallo script), con link alle schede raw/fonti/ concepts/ meccanismi, ROP, ACQ, bottle brush, π-stacking, ciclovoltammetria… compounds/ un file per composto numerato (composto-32.md) o polimero/campione techniques/ NMR, FT-IR, GPC, UV-Vis, fluorescenza, DSC, CV: condizioni usate nella tesi @@ -72,11 +73,16 @@ status: draft | stable - **Sicurezza:** niente procedure di sintesi pericolose oltre quanto riporta la tesi; riporta i pericoli noti dei reagenti se citati. ## Figure -- `wiki/figures/*.md` sono **derivate**: `python scripts/gen_figures.py` le rigenera da `raw/immagini.json`, riportando ogni campo (didascalie, descrizioni e testo visibile per pannello, composti, concetti, contesto, righe di citazione, note di revisione) senza riassumere. Eccezione alla regola "solo l'LLM scrive in `wiki/`"; non modificarle a mano, correggi `raw/immagini.json` solo se l'utente lo chiede e poi rigenera. +- `wiki/figures/*.md` e `wiki/bibliografia.md` sono **derivate**: `python scripts/gen_figures.py` le rigenera da `raw/immagini.json`, riportando ogni campo (didascalie, descrizioni e testo visibile per pannello, composti, concetti, contesto, righe di citazione, note di revisione) senza riassumere. Eccezione alla regola "solo l'LLM scrive in `wiki/`"; non modificarle a mano, correggi `raw/immagini.json` solo se l'utente lo chiede e poi rigenera. - **Attendibilità:** solo `caption_printed` è testo della tesi. Descrizioni, `visible_text` e didascalia generata derivano dall'immagine e non sono verificati: valori letti da grafici o schemi (rese, picchi, potenziali) vanno confermati sull'immagine/tesi prima di riusarli. - Le pagine concept/compound/technique richiamano le figure con `[[fig-026]]` o con l'embed `![[immagini/]]` (da `panels[].embed`). Le figure con `flags` o `review_notes` (Figure 26, 27, 29, 57, 62, 65, 66, 68 hanno discrepanze didascalia/testo) vanno citate con l'avvertenza. - `compounds` nel catalogo sono numeri della tesi; `concepts` sono slug candidati, non nomi definitivi: crea la pagina solo se la regola dei ≥2 usi è soddisfatta. +## Regole di organizzazione dei dati +- Una tabella o un dato sta in **una sola pagina**: quella dove la tesi lo discute (per es. Tab. 5 in `dpp-2`, Tab. 13-14 in `ciclovoltammetria`). Le altre pagine rimandano con wikilink; fanno eccezione i riepiloghi comparativi (es. in `uv-vis-fluorescenza`), che citano la tabella di origine. +- Le pagine riorganizzano per argomento, non per capitolo, senza eliminare informazioni: procedure con quantità in tabella, condizioni, assegnazioni e ragionamenti della tesi restano, con `tesi_loc` e righe. +- Composti sperimentali: `dpp-1`, `dpp-2`, `copolimeri-3a-3b-3c`, `bottle-brush-3-x`. La numerazione dei composti del cap. 1 (1-48) è un'altra: non confonderle. + ## Difetti noti della tesi Raccolti in `wiki/analyses/difetti-noti.md` (una sola pagina; le altre rimandano lì): bibliografia con voce 44 duplicata della 1; voci 20, 22, 36, 53 incomplete; DOI errati nelle voci 47, 48 (corretto 10.1080/15583720802231833) e 49; voci 47, 49, 53 non identificabili; segnaposto "paragrafo XX (XX)" in 4.4.4; discrepanze figura/testo sopra elencate. diff --git a/index.md b/index.md index 1fdccb9..e3707b4 100644 --- a/index.md +++ b/index.md @@ -1,20 +1,43 @@ # Indice della wiki -_Catalogo di tutte le pagine. Aggiornato a ogni ingest/query. Pagine curate: 2 · Figure generate: 78_ +_Catalogo di tutte le pagine. Aggiornato a ogni ingest/query. Pagine curate: 25 · Figure generate: 78 · Fonti ingerite: 1 (la tesi)_ ## Overview -- [[overview]] — sintesi evolutiva della tesi (da compilare) +- [[overview]] — problema, strategia, risultati dichiarati e limiti della tesi ## Tesi e bibliografia -- [[tesi]] — mappa capitolo/sezione → pagine wiki +- [[bibliografia]] — i 59 riferimenti con link alle schede in `raw/fonti/` (generata) +- [[tesi]] — mappa sezione → pagine wiki → figure ## Concetti +- [[acq-e-stato-solido]] — ACQ, evidenza sui film, aggregati H/J, misura sul polimero 3.2b +- [[bottle-brush]] — logica di progetto, sequenza di sintesi, cosa dimostrano i dati +- [[dpp-reattivita]] — siti reattivi, N-alchilazione, cross-coupling, arilazioni, litiazione, SNAr +- [[dpp-sintesi-letteratura]] — Farnum, Iqbal, Closs-Gompper, Sprake, Langhals +- [[dpp-struttura-e-proprieta]] — struttura, impaccamento, Tab. 2, lavoro precedente del gruppo +- [[fluorescenza]] — Jablonski, Stokes, resa quantica, tempi di vita (Eq. 1-5) +- [[fluorofori-in-polimeri]] — host-guest, main-chain, side-chain, cross-linked +- [[optoelettronica-oled-donatore-accettore]] — OLED, approccio D-A, scelta DPP+3HT +- [[polimerizzazione-ossidativa-fecl3]] — meccanismo SET, ruolo di nitrometano e CHCl3, work-up +- [[rop-pcl]] — ROP del caprolattone con Sn(Oct)2, grafting-from ## Composti +- [[bottle-brush-3-x]] — i sei bottle brush 3.1b-3.3c (Tab. 4, 9-12, procedura) +- [[copolimeri-3a-3b-3c]] — copolimeri DPP-3HT (Tab. 3, 6-8, procedura) +- [[dpp-1]] — DPP tiofenico (procedura, pseudo-Stobbe, spettri) +- [[dpp-2]] — monomero bis-idrossiesil (procedura, N-alchilazione, Tab. 5) +- [[reagenti-e-materiali]] — reagenti per passaggio e trattamento dei solventi ## Tecniche +- [[ciclovoltammetria]] — teoria (Eq. 6-8), procedura, metodo (Eq. 11-12), Tab. 13-14 +- [[dsc]] — programma termico e risultati +- [[ft-ir]] — bande diagnostiche +- [[gpc]] — condizioni e interpretazione della sottostima +- [[nmr-1h]] — %DPP (Eq. 9) e peso molecolare (Eq. 10) +- [[uv-vis-fluorescenza]] — riepilogo dei dati ottici in soluzione ## Figure -- [[wiki/figures]] — 78 note generate da `raw/immagini.json` (28 reaction_scheme, 11 diagram, 8 mechanism, 7 spectrum_uv_vis, 6 spectrum_nmr, 5 chemical_structure, 5 plot, 4 spectrum_ir, 2 cv_voltammogram, 1 photo, 1 spectrum_fluorescence) +- `wiki/figures/` — 78 note generate da `raw/immagini.json` (28 reaction_scheme, 11 diagram, 8 mechanism, 7 spectrum_uv_vis, 6 spectrum_nmr, 5 chemical_structure, 5 plot, 4 spectrum_ir, 2 cv_voltammogram, 1 photo, 1 spectrum_fluorescence); elenco per sezione in [[tesi]] ## Analisi +- [[difetti-noti]] — difetti noti della tesi e incoerenze rilevate nell'ingest diff --git a/log.md b/log.md index 07baf42..e3a904a 100644 --- a/log.md +++ b/log.md @@ -16,3 +16,16 @@ _Append-only. Formato: `## [YYYY-MM-DD] tipo | titolo`_ - Figure: `scripts/gen_figures.py` genera 78 note in `wiki/figures/` da `raw/immagini.json` (derivate, senza riassunti) ## [2026-10-09] setup | Generate le 78 note figura e wiki/tesi.md (mappa) + +## [2026-10-09] ingest | Tesi completa (cap. 1-5, bibliografia, figure) +- Fonte: `raw/tesi.md` (r.1-1411) + `raw/immagini.json` + `raw/bibliografia.json`. Nessun riassunto: contenuto riorganizzato per argomento +- Concetti (10): dpp-struttura-e-proprieta, dpp-sintesi-letteratura, dpp-reattivita, fluorescenza, fluorofori-in-polimeri, optoelettronica-oled-donatore-accettore, acq-e-stato-solido, polimerizzazione-ossidativa-fecl3, rop-pcl, bottle-brush +- Composti (5): dpp-1, dpp-2, copolimeri-3a-3b-3c, bottle-brush-3-x, reagenti-e-materiali +- Tecniche (6): nmr-1h, ft-ir, gpc, uv-vis-fluorescenza, dsc, ciclovoltammetria +- Analisi: difetti-noti (bibliografia, segnaposto, frase troncata, figure, 10 incoerenze rilevate: ottici di 1 e 2, integrali NMR, fusione, bandgap nelle conclusioni, Tab. 12, aritmetica CV) +- Overview, wiki/tesi.md (mappa sezioni -> pagine -> figure), wiki/bibliografia.md (script gen_bibliografia.py); figure incorporate con embed e link alle 78 note +- Controlli: 161 embed e tutti i wikilink risolti, nessuna pagina orfana + +## [2026-10-09] schema | Regole di organizzazione dati e script bibliografia +- CLAUDE.md: una tabella in una sola pagina; script `gen_bibliografia.py`; `bibliografia.md` derivata + diff --git a/scripts/gen_bibliografia.py b/scripts/gen_bibliografia.py new file mode 100644 index 0000000..fe40ca9 --- /dev/null +++ b/scripts/gen_bibliografia.py @@ -0,0 +1,29 @@ +"""Genera wiki/bibliografia.md da raw/bibliografia.json (una voce per riferimento, link alla scheda in raw/fonti/). +Uso: python scripts/gen_bibliografia.py (rigenera tutto; pagina derivata, non si modifica a mano).""" +import json +from pathlib import Path + +root = Path(__file__).resolve().parent.parent +refs = json.loads((root / "raw/bibliografia.json").read_text(encoding="utf8"))["references"] + +out = [ + "---", "title: Bibliografia", "type: overview", "tags: [bibliografia]", + "created: 2026-10-09", "updated: 2026-10-09", 'tesi_loc: "r.1293-1411"', "derivata: true", "status: draft", "---", "", + "# Bibliografia", "", + "Elenco dei 59 riferimenti della tesi (`text` = testo originale). Ogni voce rimanda alla scheda in `raw/fonti/` e alle righe/sezioni di `raw/tesi.md` in cui è citata. Difetti noti: [[difetti-noti]].", "", + "| N | Riferimento (testo della tesi) | Citato in (sezioni; righe) | Scheda | Stato | DOI verificato | Flag |", + "| --- | --- | --- | --- | --- | --- | --- |", +] +for r in refs: + f = r["fonte"] + card = Path(f["file"]).stem + text = r["text"].replace("|", "\\|") + secs = ", ".join(r["cited_in_sections"]) or "-" + lines = ", ".join(map(str, r["cited_in_md_lines"])) or "-" + out.append( + f"| {r['id']} | {text} | §{secs}; r.{lines} | [[{card}\\|{r['id']}]] | {f.get('stato', '-')} | " + f"{f.get('doi_verificato') or '-'} | {', '.join(r.get('quality_flags', [])) or '-'} |" + ) +out += ["", "## Collegamenti", "- [[tesi]]", ""] +(root / "wiki/bibliografia.md").write_text("\n".join(out), encoding="utf8") +print(f"{len(refs)} voci") diff --git a/scripts/gen_figures.py b/scripts/gen_figures.py index 68c0603..8902375 100644 --- a/scripts/gen_figures.py +++ b/scripts/gen_figures.py @@ -45,6 +45,8 @@ for f in cat["figures"]: body += [f"**Didascalia stampata (testo della tesi):** {f.get('caption_printed') or 'n/d'}", ""] cap = f", didascalia r.{loc['caption_md_line']}" if loc.get("caption_md_line") else "" body += [f"_Posizione: tesi.md {tesi_loc} (sezione {loc['section']} {loc['section_title']}){cap}_", ""] + if "caption_mismatch" in qual.get("flags", []): + body += ["> ⚠ Flag `caption_mismatch`: la didascalia stampata qui sopra è quella attribuita dal catalogo e potrebbe non descrivere l'immagine (vedi «Didascalia generata» e «Da verificare»).", ""] body += ["> Sotto: contenuto generato guardando l'immagine, non verificato una per una.", ""] body += [f"**Didascalia generata:** {f['caption']}", ""] for p in f["panels"]: diff --git a/wiki/analyses/difetti-noti.md b/wiki/analyses/difetti-noti.md new file mode 100644 index 0000000..7454b57 --- /dev/null +++ b/wiki/analyses/difetti-noti.md @@ -0,0 +1,66 @@ +--- +title: Difetti noti, incoerenze e punti da verificare +type: analysis +tags: [qualità, discrepanze, verifica] +created: 2026-10-09 +updated: 2026-10-09 +tesi_loc: "varie (indicate per voce)" +refs: [1, 20, 22, 36, 44, 47, 48, 49, 53] +figures: ["fig-004", "fig-009", "fig-010", "fig-026", "fig-027", "fig-029", "fig-033", "fig-034", "fig-049", "fig-057", "fig-061", "fig-062", "fig-065", "fig-066", "fig-068", "fig-x-cc3f54", "fig-x-136800"] +status: draft +--- + +# Difetti noti, incoerenze e punti da verificare + +Pagina unica: le altre pagine rimandano qui. Regola: **segnalare, non correggere**. Sezioni A-D = difetti già noti (CLAUDE.md, catalogo immagini); sezione E = incoerenze rilevate durante questo ingest, confrontando testo, tabelle e conclusioni di `raw/tesi.md` (le righe sono di quel file). Dove indicato, è stato fatto un controllo aritmetico o sul PDF originale. + +## A. Bibliografia (da `raw/bibliografia.json`, `raw/fonti/`) +| Voce | Problema | Stato | +|---|---|---| +| 44 | duplica la voce 1 (Bao 2020, Front. Chem.) | `duplicate_entry` | +| 20 (Lenz), 22 (Zambounis & Iqbal), 36 (Stokes), 53 (Paganin, Bizzarri, Lanzi) | incomplete già nel testo originale (`incomplete_in_source`) | 20 e 36 identificate; 22 candidata; 53 non risolta | +| 47 (Li, 2014), 49 (Hendriks, 2013) | DOI errati/non registrati; voci non identificabili | `non_risolta` | +| 48 (Kroon, 2008) | DOI errato; il DOI corretto è **10.1080/15583720802231833** | `verificata_con_correzioni` | + +Schede in `raw/fonti/`. La voce 53 è citata a r.840 per il meccanismo di trasferimento mono-elettronico (SET) nella polimerizzazione ossidativa ([[53-paganin-nd|53]]); la sua scheda la dà come non risolta (senza anno, rivista o DOI). + +## B. Segnaposto non risolto +- **«paragrafo XX (XX)»** in §4.4.4 (r.1247): il confronto con i copolimeri lineari doveva rimandare a §4.4.3. + +## C. Frase troncata nel testo (anche nel PDF originale) +- §1.1.2, r.235: «...qualsiasi modifica strutturale si traduce, in Il comportamento allo stato solido appare, invece, ...». La frase è interrotta anche nel testo di `tesi.pdf` (controllato nella versione in cronologia git): non è un errore di estrazione. [[dpp-struttura-e-proprieta]]. + +## D. Discrepanze figura/testo (dal catalogo `raw/immagini.json`) +| Figura | Nota | +|---|---| +| [[fig-026\|Fig. 26]] | Didascalia («DPP di-bromurati con diversi areni») non coincide col testo, che cita i prodotti 38(a-h) della Figura 25; l'immagine mostra l'arilazione di 32 e 37 con tiofeni sostituiti | +| [[fig-027\|Fig. 27]] | Il testo cita il prodotto «45a», l'immagine mostra 42a-c: numerazione composti incoerente | +| [[fig-029\|Fig. 29]] | Nell'immagine **45** è il derivato SnMe3; controllare la numerazione col testo | +| [[fig-057\|Fig. 57]] | Didascalia (3a blu, 3b verde, 3c rosso) e testo (3a verde, 3b rossa, 3c blu) discordano sui colori; nessuna legenda in immagine | +| [[fig-062\|Fig. 62]] | Lampadina barrata sotto «Deboli interazioni» e accesa sotto «Forti interazioni»; il testo non lo spiega | +| [[fig-065\|Fig. 65]], [[fig-066\|Fig. 66]] | Nessuna legenda in immagine; i colori non combaciano chiaramente con la didascalia | +| [[fig-068\|Fig. 68]] | Assegnazione dei picchi (~64 °C fusione, ~24 °C cristallizzazione) dedotta da «Exo Down» e dal contesto | +| [[fig-x-136800\|schema bottle brush]] | Schema: reflusso **4 h**; testo (r.663): **24 h**. Il file catalogato come «Tabella 4» è in realtà lo schema della ROP | +| [[fig-x-cc3f54\|schema copolimeri]] | Il file catalogato come «Tabella 3» è lo schema della copolimerizzazione | +| [[fig-009\|Fig. 9]] | La didascalia riportava «Gloss» (refuso), corretto in «Closs» | +| [[fig-044\|Fig. 44]] | I ppm sono stimati dall'asse, non letti da etichette | +| [[fig-004\|Fig. 4]], [[fig-010\|Fig. 10]], [[fig-034\|Fig. 34]], [[fig-061\|Fig. 61]] | bassa risoluzione | +| [[fig-033\|Fig. 33]], [[fig-049\|Fig. 49]] | ritagliata (e [[fig-033\|Fig. 33]] multi-pannello) | + +Anche: la didascalia di [[fig-004|Fig. 4]] dice «sale di zinco derivato dall'intermedio **3**», mentre il testo (r.114) lo riferisce all'intermedio **1** (il DPP è il 3). _(osservazione dalla lettura del testo)_ + +## E. Incoerenze rilevate nell'ingest +1. **Numerazione dei composti doppia.** Nel cap. 1 i numeri 1-48 indicano composti di letteratura; nei cap. 3-4 «1» e «2» sono i DPP sperimentali ([[dpp-1]], [[dpp-2]]). Nel testo di r.287 si dice che «il DPP **26** si può ottenere più semplicemente dal 4-bromobenzonitrile»: nel contesto 26 è il solfonato, il prodotto bromurato è 27 _(possibile refuso, inferenza)_. +2. **Dati ottici di [[dpp-1]].** §3.2 (r.604-606): UV-Vis 532 e 498 nm, fluorescenza **490 nm**. §4.1 (r.770): massimo di emissione **543 nm** (spalla 585 nm). Tabella 5: λabs **531**, λex **542**, Stokes 11. Il valore 490 nm è inferiore al massimo di assorbimento. +3. **Dati ottici di [[dpp-2]].** §3.2 (r.624-626): UV-Vis 541 nm, fluorescenza **540 nm**. Tabella 5: λabs 541, λex **555**, Stokes 14. Inoltre il testo (r.810) dice «Stokes shift ... simile per entrambi i fluorofori e vale circa 14 nm», mentre la tabella dà 11 nm per 1 e 14 nm per 2. +4. **Integrazioni ¹H-NMR in §3.2.** Per **1** (r.602): 4H + 4H + 4H = 12H, mentre il DPP 1 ha 6 H tiofenici (più 2 NH, non riportati nella lista). Per **2** (r.620): aromatici 1H + 1H + 2H = 4H, mentre i tiofeni sono 6 H. _(verifica sulla struttura; i dati originali non sono disponibili in `raw/`)_ +5. **Fusione dei copolimeri lineari.** §4.2 (r.954): DSC senza transizioni di fusione, Tg ≈ −10 °C. Conclusioni (r.1283): «transizioni vetrose intorno a −10 °C e temperature di fusione superiori a 110 °C». Vedi [[dsc]]. +6. **Bandgap nelle Conclusioni.** r.1289: correlazione lineare con R² = 0,9719 «tra la percentuale reale di DPP ... e l'allargamento del bandgap (da 3,42 eV a oltre 4,30 eV)». Tabella 13 ([[ciclovoltammetria]]): 0,970 / 1,316 / 1,371 eV. R² non compare altrove nel testo. +7. **Pesi molecolari via ¹H-NMR (Tab. 12).** Il testo (r.1078) li definisce «molto più vicini ai valori teorici» rispetto alla GPC, ma 3.3b = 88000 Da vs 34500 teorico (≈2,5×), 3.1c = 18200 vs 10000, 3.3c = 41300 vs 55000 (inferiore al teorico). Vedi [[bottle-brush-3-x]]. +8. **Aritmetica CV.** Le Tabelle 13 e 14 sono state ricalcolate con le Eq. 11-12 (HOMO = −(Eonsetox + 4,8), LUMO = −(Eonsetred + 4,8), Eg = LUMO − HOMO): tutte le righe tornano entro l'arrotondamento, **tranne 3c** (Tab. 13), dove Eonsetox = 0,0006 V darebbe HOMO ≈ −4,8006 eV (tabella: −4,799) e Eg ≈ 1,373 eV (tabella: 1,371). Differenza di pochi millielettronvolt. _(controllo eseguito in questo ingest)_ +9. **Tabelle UV.** Gli Stokes shift delle Tabelle 7 e 10 coincidono con la differenza λex − λabs (controllato). +10. **Refusi nei titoli e nelle didascalie.** «copolimeri lienari» (titolo §4.4.3), «Reformtskij» (didascalia [[fig-005|Fig. 5]]), «di-brorumati» (didascalia [[fig-026|Fig. 26]]), «prepare» (r.862). + +## Collegamenti +- [[tesi]] · [[bibliografia]] +- [[dpp-struttura-e-proprieta]] · [[dpp-reattivita]] · [[dpp-1]] · [[dpp-2]] · [[ciclovoltammetria]] · [[bottle-brush-3-x]] · [[dsc]] diff --git a/wiki/bibliografia.md b/wiki/bibliografia.md new file mode 100644 index 0000000..7ed3807 --- /dev/null +++ b/wiki/bibliografia.md @@ -0,0 +1,79 @@ +--- +title: Bibliografia +type: overview +tags: [bibliografia] +created: 2026-10-09 +updated: 2026-10-09 +tesi_loc: "r.1293-1411" +derivata: true +status: draft +--- + +# Bibliografia + +Elenco dei 59 riferimenti della tesi (`text` = testo originale). Ogni voce rimanda alla scheda in `raw/fonti/` e alle righe/sezioni di `raw/tesi.md` in cui è citata. Difetti noti: [[difetti-noti]]. + +| N | Riferimento (testo della tesi) | Citato in (sezioni; righe) | Scheda | Stato | DOI verificato | Flag | +| --- | --- | --- | --- | --- | --- | --- | +| 1 | Bao, W. W. *et al.* Diketopyrrolopyrrole (DPP)-Based Materials and Its Applications: A Review. *Front. Chem.* **8**, 679 (2020). | §1.1; r.77 | [[01-bao-2020\|1]] | verificata | 10.3389/fchem.2020.00679 | - | +| 2 | Shaikh, S. A. L. *et al.* A minireview on diketopyrrolopyrrole chemistry: Historical perspective and recent developments. *Results Chem.* **4**, 100473 (2022). | §1.1, 1.1.1, 1.1.2; r.81, 86, 90, 253 | [[02-shaikh-2022\|2]] | verificata | 10.1016/j.rechem.2022.100473 | - | +| 3 | Auwalu, M. A. & Cheng, S. Diketopyrrolopyrrole Fluorescent Probes, Photophysical and Biological Applications. *Chemosensors* **9**, 44 (2021). | §1.1; r.81 | [[03-auwalu-2021\|3]] | verificata | 10.3390/chemosensors9030044 | - | +| 4 | Zhang, B. *et al.* Diketopyrrolopyrrole-based fluorescent probe for visualizing over-expressed carboxylesterase in fever via ratiometric imaging. *Talanta* **266**, 124971 (2024). | §1.1; r.81 | [[04-zhang-2024\|4]] | verificata | 10.1016/j.talanta.2023.124971 | - | +| 5 | Iqbal, A. *et al.* The synthesis and properties of 1,4-diketo-pyrrolo[3,4-C]pyrroles. *Bull. Sociétés Chim. Belg.* **97**, 615–644 (1988). | §1.1.1, 1.1.2, 4.1; r.94, 150, 168, 271, 742 | [[05-iqbal-1988\|5]] | verificata | 10.1002/bscb.19880970804 | - | +| 6 | Sprake, J. M. & Watson, K. D. Addition products of 2-(N-arylformimidoyl)pyridines and carbanions, and their reduction to octahydroindolizine derivatives. *J. Chem. Soc. Perkin 1* 5 (1976) doi:10.1039/p19760000005. | §1.1.1; r.138, 174, 178 | [[06-sprake-1976\|6]] | verificata | 10.1039/p19760000005 | - | +| 7 | Grzybowski, M. & Gryko, D. T. Diketopyrrolopyrroles: Synthesis, Reactivity, and Optical Properties. *Adv. Opt. Mater.* **3**, 280–320 (2015). | §1.1.1, 1.1.2, 4.1; r.150, 247, 301, 305, 742, 748 | [[07-grzybowski-2015\|7]] | verificata | 10.1002/adom.201400559 | - | +| 8 | Closs, F. & Gompper, R. 2,5-Diazapentalenes. *Angew. Chem. Int. Ed. Engl.* **26**, 552–554 (1987). | §1.1.1; r.160 | [[08-closs-1987\|8]] | verificata | 10.1002/anie.198705521 | - | +| 9 | Stas, S., Sergeyev, S. & Geerts, Y. Synthesis of diketopyrrolopyrrole (DPP) derivatives comprising bithiophene moieties. *Tetrahedron* **66**, 1837–1845 (2010). | §1.1.1; r.180 | [[09-stas-2010\|9]] | verificata | 10.1016/j.tet.2010.01.027 | - | +| 10 | Avcıbaşi, N. *et al.* Synthesis and in vitro evaluation of dioxopyrrolopyrroles as potential low-affinity fluorescent Ca2+ indicators. *Int. J. Photoenergy* **6**, 159–167 (2004). | §1.1.1; r.180 | [[10-avcbasi-2004\|10]] | verificata | 10.1155/s1110662x04000200 | - | +| 11 | Riggs, R. L. *et al.* Synthetic studies related to diketopyrrolopyrrole (DPP) pigments. Part 3: Syntheses of tri- and tetra-aryl DPPs. *Tetrahedron* **61**, 11230–11243 (2005). | §1.1.1; r.180 | [[11-riggs-2005\|11]] | verificata | 10.1016/j.tet.2005.09.005 | - | +| 12 | Qian, G. & Wang, Z. Y. Near-Infrared Thermochromic Diazapentalene Dyes. *Adv. Mater.* **24**, 1582–1588 (2012). | §1.1.1; r.180 | [[12-qian-2012\|12]] | verificata | 10.1002/adma.201104711 | - | +| 13 | Langhals, H., Grundei, T., Potrawa, T. & Polborn, K. Highly Photostable Organic Fluorescent Pigments – A Simple Synthesis of *N* -Arylpyrrolopyrrolediones (DPP). *Liebigs Ann.* **1996**, 679–682 (1996). | §1.1.1; r.182 | [[13-langhals-1996\|13]] | verificata | 10.1002/jlac.199619960506 | - | +| 14 | De Luca, L., Giacomelli, G. & Porcheddu, A. A Mild and Efficient Alternative to the Classical Swern Oxidation. *J. Org. Chem.* **66**, 7907–7909 (2001). | §1.1.1; r.184 | [[14-de-luca-2001\|14]] | verificata | 10.1021/jo015935s | - | +| 15 | Harris, J. M., Liu, Y., Chai, S., Andrews, M. D. & Vederas, J. C. Modification of the Swern Oxidation: Use of a Soluble Polymer-Bound, Recyclable, and Odorless Sulfoxide. *J. Org. 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Chem.* **65**, 477–500 (2014). | §4.5; r.1262 | [[59-spano-2014\|59]] | verificata | 10.1146/annurev-physchem-040513-103639 | - | + +## Collegamenti +- [[tesi]] diff --git a/wiki/compounds/bottle-brush-3-x.md b/wiki/compounds/bottle-brush-3-x.md new file mode 100644 index 0000000..28d10a6 --- /dev/null +++ b/wiki/compounds/bottle-brush-3-x.md @@ -0,0 +1,137 @@ +--- +title: Polimeri bottle brush DPP-3HT-g-PCL (3.1b-3.3c) +type: compound +aliases: ["3.1b", "3.2b", "3.3b", "3.1c", "3.2c", "3.3c", "3.1.b", "3.2.c", "polimeri bottle brush"] +tags: [bottle-brush, pcl, rop, serie-b, serie-c] +created: 2026-10-09 +updated: 2026-10-09 +tesi_loc: "§3.2 r.646-663; §4.3 r.957-1097; §4.4.4 r.1230-1251; §4.5 r.1254-1276" +refs: [55, 56, 57] +figures: ["fig-x-136800", "fig-062", "fig-063", "fig-064", "fig-065", "fig-066", "fig-067", "fig-068"] +status: draft +--- + +# Polimeri bottle brush DPP-3HT-g-PCL (3.1b-3.3c) + +Sei polimeri in due serie, ottenuti per [[rop-pcl]] dai macroiniziatori **3b** e **3c** ([[copolimeri-3a-3b-3c]]), con catene laterali di PCL a Mn teorico **1500, 5000, 10000 Da**. Codici composto con il punto (`3.1b`); nel §4.4 compaiono anche come 3.1.b, 3.2.c ecc. (stessa cosa). Strategia: [[bottle-brush]]. + +![[immagini/136800375cf0b441570672093e255d90a47c45a009bd254929fb74b1f17b382d.jpg|560]] +*schema bottle brush (didascalia generata dal catalogo): Polimerizzazione ad apertura di anello di epsilon-caprolattone sui gruppi OH dei copolimeri DPP-3HT per ottenere i polimeri bottle brush con catene di PCL.* · [[fig-x-136800|nota figura]] + +> Nota del catalogo: lo schema riporta reflusso di **4 h**, la procedura del testo **24 h**; la descrizione del catalogo segue l'immagine. La didascalia «Tabella 4» attribuita al file è un'attribuzione errata ([[difetti-noti]]). + +## Quantità di caprolattone (§3.2, r.650-661) +La quantità di ε-caprolattone è fissata in base agli equivalenti di gruppi -OH del derivato DPP, considerati iniziatori attivi per la ROP. + +**Tabella 4** - *composizione dei polimeri bottle brush* +| Copolimero | Mn teorico | Caprolattone V (ml) | Caprolattone mol | +| --- | --- | --- | --- | +| 3b | 1500 Da (**3.1b**) | 1,06 | 0,01 | +| 3b | 5000 Da (**3.2b**) | 4,65 | 0,04 | +| 3b | 10000 Da (**3.3b**) | 9,29 | 0,09 | +| 3c | 1500 Da (**3.1c**) | 1,72 | 0,02 | +| 3c | 5000 Da (**3.2c**) | 7,43 | 0,07 | +| 3c | 10000 Da (**3.3c**) | 14,87 | 0,1 | + +**Tabella 9** - *lunghezza delle catene in PCL nei polimeri bottle brush* (r.981-990): 3.1b/3.1c = 1500 Da; 3.2b/3.2c = 5000 Da; 3.3b/3.3c = 10000 Da (coincide con Tab. 4). + +### Formula del volume di caprolattone (r.992-998) +$$ +V_{CL}=\frac{\frac{m_{backbone}}{MW_{backbone}}\times DP_{backbone}\times \chi _{DPP}\times 2\times Mn_{teorico}}{\rho _{CL}} +$$ +- $V_{CL}$: volume di caprolattone da prelevare (mL). +- $m_{backbone}$ (g) / $MW_{backbone}$ (g/mol, dalla GPC) = moli di backbone. +- $DP_{backbone}$: grado di polimerizzazione del copolimero lineare di partenza. +- $\chi_{DPP}$: frazione molare delle unità DPP. +- $2$: gruppi -OH per ogni unità DPP. +- $Mn_{teorico}$ (Da): peso molecolare teorico desiderato per la singola catena laterale di PCL. +- $\rho_{CL}$ (g/mL): densità dell'ε-caprolattone liquido alla temperatura di prelievo, per convertire la massa in volume. + +## Procedura (identica per tutti, r.663) +1. Pallone da **30 mL** con rubinetto: copolimero (quantitativi di Tab. 4) sciolto in THF; riscaldamento con bagno ad olio siliconico; solvente rimosso a pressione ridotta con pompa a membrana. +2. Residuo secco in **atmosfera inerte di azoto**. +3. Aggiunta di **2 mL di toluene** e della quantità di caprolattone di Tab. 4. +4. Soluzione portata a **110 °C**; aggiunta di **Sn(Oct)2** in quantità catalitica. +5. **Reflusso per 24 h**. +6. Purificazione: precipitazione in non-solvente (**metanolo freddo**); polimero recuperato per filtrazione su Büchner ed essiccato all'aria sotto cappa aspirante. + +Perché metanolo freddo e meccanismo: [[rop-pcl]]. + +## Verifica dell'innesto +### ¹H-NMR ([[fig-064|Fig. 64]], r.1000) +Comparsa dei segnali del PCL: **tripletto a ~4,0 ppm** (-CH2-O-, adiacente all'ossigeno estereo) e segnale a **2,3 ppm** (protoni in α al carbonile). Spettri analoghi per tutta la serie, differiscono per i valori di integrazione in funzione del peso molecolare: [[fig-064|Fig. 64]] è lo spettro rappresentativo di **3.1b**. + +![[immagini/aae4bec55b3a0f29e1dfa6231c86c1d0295d5d38f2f2e9f0af6a69eba8aa0231.jpg|560]] +*Figura 64 - spettro 1H-NMR del polimero 3.1b in CDCl3* · [[fig-064|nota figura]] + +### FT-IR ([[fig-065|Fig. 65]], [[fig-066|Fig. 66]], r.1006-1010) +Spettri sovrapposti per le due serie con la traccia del macroiniziatore alla base. +- Precursore: assorbimento largo **3600-3200 cm⁻¹** (O-H terminale). Dopo la polimerizzazione la banda è **assente** nei bottle brush: l'ossidrile ha fatto da sito iniziatore. +- Compare un picco molto stretto e intenso a ~**1720 cm⁻¹** (C=O estereo delle unità di caprolattone). +- Maggiore definizione dello stretching C-H alifatici (**2950-2860 cm⁻¹**); forti segnali C-O-C nel fingerprint (**1240-1160 cm⁻¹**). +- All'aumentare del peso molecolare delle catene laterali il profilo tende a coincidere con quello del PCL omopolimero: la massa delle catene copre i segnali meno intensi del backbone. +- Le legende dei colori nelle immagini non sono presenti e non combaciano chiaramente con la didascalia ([[difetti-noti]]). + +![[immagini/4cd08436660a2e3a6f913e54d196a0d183b780c3f5f915be6d22a563771d3e43.jpg|560]] +*Figura 65 - spettri FT-IR dei polimeri bottle brush ottenuti a partire dal copolimero 3b (verde)* · [[fig-065|nota figura]] + +![[immagini/d5559d2ff37ffb2861c2ac8eecbade7c09f8fc905c8363be4f48c06a0afae72e.jpg|560]] +*Figura 66 - spettri FT-IR dei polimeri bottle brush ottenuti a partire dal copolimero 3c (verde)* · [[fig-066|nota figura]] + +## UV-Vis ed emissione in THF ([[fig-067|Fig. 67]], r.1024-1043) +- Massimi di assorbimento dell'intera libreria: **544-554 nm**; massimi di emissione: **557-564 nm**. Le fluttuazioni nelle due serie non seguono un andamento lineare con il peso molecolare del PCL e sono trascurabili → l'ingombro sterico non perturba livelli energetici e natura delle transizioni del core DPP. +- Stokes shift **8-14 nm**, conferma del design: i domini flessibili di PCL allontanano le catene principali (meno impaccamento, più mobilità) senza introdurre distorsioni alla geometria del backbone; il basso Stokes shift indica che il core conserva la conformazione planare senza rilassamenti nel passaggio allo stato eccitato. + +**Tabella 10** - *dati spettroscopici dei polimeri sintetizzati* +| Polimero | λmax, abs (nm) | λmax, ex (nm) | Stokes shift (nm) | +| --- | --- | --- | --- | +| 3.1b | 554 | 562 | 8 | +| 3.2b | 550 | 564 | 14 | +| 3.3b | 553 | 563 | 10 | +| 3.1c | 547 | 561 | 14 | +| 3.2c | 544 | 557 | 13 | +| 3.3c | 553 | 564 | 11 | + +![[immagini/be53b102694fafa8036962962c8c0a3735cc1ec95cf721f163b7d25bdd7099fb.png|560]] +*Figura 67 - spettri UV-Visibile (linea continua) e di emissione (linea tratteggiata) dei polimeri bottle brush in THF* · [[fig-067|nota figura]] + +Stato solido (solo 3.2b): [[acq-e-stato-solido]]. + +## GPC (r.1045-1062) → [[gpc]] +**Tabella 11** - *pesi molecolari e polidispersità dei polimeri bottle brush determinati mediante GPC* +| Polimero | Massa molecolare media numerale (Da) | Massa molecolare media ponderale (Da) | Polidispersità (PD) | +| --- | --- | --- | --- | +| 3.1b | 12188 | 18536 | 1,521 | +| 3.2b | 17302 | 22737 | 1,314 | +| 3.3b | 21269 | 26328 | 1,238 | +| 3.1c | 13999 | 18219 | 1,301 | +| 3.2c | 19119 | 24376 | 1,275 | +| 3.3c | 14445 | 19521 | 1,351 | + +Interpretazione della tesi (sottostima per volume idrodinamico, outlier 3.3c): [[gpc]]. + +## Peso molecolare da ¹H-NMR (r.1064-1089) → [[nmr-1h]] +**Tabella 12** - *pesi molecolari dei polimeri bottle brush determinati via ¹H-NMR* +| Polimero | Peso Molecolare teorico (Da) | Peso Molecolare da ¹H-NMR (Da) | +| --- | --- | --- | +| 3.1b | 6500 | 8900 | +| 3.2b | 18000 | 20500 | +| 3.3b | 34500 | 88000 | +| 3.1c | 10000 | 18200 | +| 3.2c | 28500 | 35500 | +| 3.3c | 55000 | 41300 | + +Il testo afferma che questi valori sono «una stima molto più vicina ai valori teorici» (rispetto alla GPC). Osservazione dai numeri: per 3.3b il valore da NMR (88000 Da) è circa 2,5 volte il teorico (34500 Da) e per 3.3c è inferiore al teorico ([[difetti-noti]]). + +## DSC (r.1091-1097) → [[dsc]] +Transizioni principali pressoché costanti per tutti i polimeri, dominate dal PCL: **Tm 55-60 °C**, **Tc 25-35 °C**. Esempio di termogramma: campione 3.1c ([[fig-068|Fig. 68]]). + +![[immagini/d2ed44d32060aa9ee04e73304940b111e53bf65cf115a93ace696933048e308b.jpg|560]] +*Figura 68 - esempio di termogramma dei polimeri bottle brush realizzati (in figura l'analisi del campione 3.1c)* · [[fig-068|nota figura]] + +## Ciclovoltammetria (§4.4.4) → [[ciclovoltammetria]] +Tabella 14: bandgap 0,929-1,521 eV. + +## Collegamenti +- [[copolimeri-3a-3b-3c]] · [[rop-pcl]] · [[bottle-brush]] · [[acq-e-stato-solido]] · [[nmr-1h]] · [[ft-ir]] · [[uv-vis-fluorescenza]] · [[gpc]] · [[dsc]] · [[ciclovoltammetria]] · [[reagenti-e-materiali]] +- [[tesi]] · [[bibliografia]] diff --git a/wiki/compounds/copolimeri-3a-3b-3c.md b/wiki/compounds/copolimeri-3a-3b-3c.md new file mode 100644 index 0000000..2477505 --- /dev/null +++ b/wiki/compounds/copolimeri-3a-3b-3c.md @@ -0,0 +1,120 @@ +--- +title: Copolimeri coniugati DPP-3HT (3a, 3b, 3c) +type: compound +aliases: ["3a", "3b", "3c", "copolimeri lineari", "macroiniziatori", "copolimeri statistici"] +tags: [copolimeri, dpp-3ht, polimerizzazione-ossidativa, macroiniziatore] +created: 2026-10-09 +updated: 2026-10-09 +tesi_loc: "§3.2 r.628-644; §4.2 r.826-954" +refs: [52, 53, 54] +figures: ["fig-x-cc3f54", "fig-052", "fig-053", "fig-054", "fig-055", "fig-056", "fig-057", "fig-058", "fig-059", "fig-060", "fig-061"] +status: draft +--- + +# Copolimeri coniugati DPP-3HT (3a, 3b, 3c) + +Copolimeri **statistici (random)** del monomero [[dpp-2]] con **3-esiltiofene (3HT)**, sintetizzati per [[polimerizzazione-ossidativa-fecl3]] (FeCl3/nitrometano, cloroformio). Servono da scheletri/macroiniziatori ([[bottle-brush-3-x]]). Perché 3HT e perché questo metodo (§4.2, r.828-832): [[polimerizzazione-ossidativa-fecl3]]. + +![[immagini/cc3f5409e11922aee7835c8eb96ff0f9826afea68af08f1473159279af625b8a.jpg|560]] +*schema copolimeri (didascalia generata dal catalogo): Copolimerizzazione ossidativa del DPP 2 con 3-esiltiofene (3HT) con FeCl3 per dare i copolimeri 3a/3b/3c. Il file è uno schema, non la Tabella 3.* · [[fig-x-cc3f54|nota figura]] + +> Nota: il catalogo delle figure attribuisce a questo file lo schema (copolimerizzazione ossidativa del DPP 2 con 3HT) e la didascalia «Tabella 3» è un'attribuzione errata (flag *caption_mismatch*). + +## Composizione di reazione (§3.2) +**Tabella 3** - *composizione dei copolimeri* (r.634-640) +| Copolimero | DPP (mmol) | DPP (eq) | 3HT (mmol) | 3HT (eq) | +| --- | --- | --- | --- | --- | +| 3a | 0,2 | 0,2 | 0,8 | 0,8 | +| 3b | 0,5 | 0,5 | 0,5 | 0,5 | +| 3c | 0,8 | 0,8 | 0,2 | 0,2 | + +## Procedura (identica per i tre, r.642-644) +1. Pallone a tre colli sotto azoto: **40 mL di CHCl3 anidro** e i due monomeri nelle proporzioni di Tab. 3; solubilizzazione di **2** favorita dal **sonicatore**. +2. In parallelo: **818 mg di FeCl3 (5,05 mmol, 5 eq)** in **10 mL di nitrometano**, in sonicatore per alcuni minuti. +3. Soluzione ossidante sgocciolata nel pallone; agitazione per **1 h**. Aggiunta di **30 mL di THF sbiancato**; altri **30 min** di agitazione. +4. Grezzo in imbuto separatore: lavaggi con **HCl 0,6 M** fino a saggio negativo del tiocianato (colore rosso = tracce di FeCl3; test dal terzo lavaggio). +5. Estrazione della fase organica con soluzione satura di NaCl; anidrificazione; evaporazione al rotavapor. +6. Precipitazione in non-solvente per rimuovere sottoprodotti (poli-3HT) e molecole a basso peso molecolare: solido nella minima quantità di THF, gocciolato in **150 mL di metanolo freddo**; precipitato filtrato e soluzione portata a secco al rotavapor. + +Motivazioni dei singoli passaggi: [[polimerizzazione-ossidativa-fecl3]]. + +## Composizione reale e limite del DPP (§4.2, r.860-884) +- Obiettivo: serie di materiali per studiare l'andamento delle proprietà al variare dell'architettura, da maggioranza tiofenica a sistema equimolare o dominato da DPP. +- **Problematiche di reazione hanno limitato l'integrazione di DPP a un massimo del 35%**. Causa indicata: differenza nei rapporti di reattività dei comonomeri, influenzata dall'ingombro sterico del nucleo DPP; il tiofene, più reattivo e meno voluminoso, addiziona preferenzialmente. +- Libreria: **3a** (minime quantità di DPP) → **3b** → **3c** (più arricchito), sempre con rapporto molare a favore del 3HT. + +**Tabella 6** - *composizione dei copolimeri coniugati* +| Copolimero | moli DPP **2** | moli 3HT | % DPP teorica (mol/mol) | % DPP reale (mol/mol) | +| --- | --- | --- | --- | --- | +| 3a | 0,2 | 0,8 | 20 | 25,2 | +| 3b | 0,5 | 0,5 | 50 | 32,6 | +| 3c | 0,8 | 0,2 | 80 | 35,3 | + +La % reale è determinata da ¹H-NMR ([[nmr-1h]], Equazione 9) sul rapporto fra il segnale CH3 del 3HT e i CH2 adiacenti agli OH del DPP. + +![[immagini/a182a55cad5ef042b39852288ff9f6ae3b5f9c0fd758fd0815f0366e77b09a8e.jpg|560]] +*Figura 54 - spettro 1H-NMR del copolimero 3a in CDCl3* · [[fig-054|nota figura]] + +![[immagini/5ab89fc3cc83f82abb39c0bfd40b1f0da53a8f88a4ca771e00621a476cf8901d.jpg|560]] +*Figura 55 - spettro 1H-NMR del copolimero 3b in CDCl3* · [[fig-055|nota figura]] + +![[immagini/f078dd5e0992c244123ad8fcbd08d2f2235bffb15f21adcee16bef8ed40a1f4e.jpg|560]] +*Figura 56 - spettro 1H-NMR del copolimero 3c in CDCl3* · [[fig-056|nota figura]] + +## FT-IR ([[fig-057|Fig. 57]], r.904) +- Conferma la copolimerizzazione. In tutti gli spettri: C-H alifatici (~2920 e ~2850 cm⁻¹); segnale a ~820 cm⁻¹ dell'anello del 3-esiltiofene. +- Incorporazione del DPP: intenso picco del **carbonile lattamico (C=O) a ~1650 cm⁻¹** e **stretching C-O a ~1050 cm⁻¹**. +- Banda degli ossidrili terminali (3300-3400 cm⁻¹) evidente in **3b** e **3c**, meno intensa in **3a** (minore contenuto di DPP). +- Colori: la didascalia dice 3a blu, 3b verde, 3c rosso; il testo dice 3a verde, 3b rossa, 3c blu: discordanza non risolta in immagine ([[difetti-noti]]). + +![[immagini/4b81d4490846b8b0f24cd7ae9e1ed776036c588345475c519334bef4eb76a684.jpg|560]] +*Figura 57 - spettro FT-IR dei copolimeri 3a (blu), 3b (verde), 3c (rosso)* · [[fig-057|nota figura]] + +## UV-Vis ed emissione in THF ([[fig-058|Fig. 58]]-[[fig-060|Fig. 60]], r.906-920) +Profili pressoché identici tra i tre copolimeri e simili a quello del monomero DPP: ampia banda di assorbimento (transizione π→π\*, λmax ≈ **540-545 nm**) ed emissione con λmax ≈ **550 nm**. Stokes shift estremamente ridotto → forte sovrapposizione assorbimento/emissione → notevole rigidità dello scheletro, minima riorganizzazione conformazionale. + +**Tabella 7** - *dati spettroscopici dei copolimeri sintetizzati* +| copolimero | λmax, abs (nm) | λmax, ecc (nm) | Stokes shift (nm) | +| --- | --- | --- | --- | +| 3a | 540 | 547 | 7 | +| 3b | 544 | 550 | 6 | +| 3c | 542 | 552 | 10 | + +![[immagini/585dc7627f409d974b2dda6d2db2fc8d1febafb609faba20d707f941b23f851c.jpg|560]] +*Figura 58 - spettro UV-Visibile e di emissione del copolimero 3a in THF* · [[fig-058|nota figura]] + +![[immagini/f8b0852a6a485472cb2438e024374bb56e26d87d86831f40903fd0be201d0771.jpg|560]] +*Figura 59 - spettro UV-Visibile e di emissione del copolimero 3b in THF* · [[fig-059|nota figura]] + +![[immagini/2b34f5439b53ddcf7aeff01949aba8f61aa554f29849c81d7c3922f06dd3bba9.jpg|560]] +*Figura 60 - spettro UV-Visibile e di emissione del copolimero 3c in THF* · [[fig-060|nota figura]] + +## Stato solido +I film su vetrino sotto lampada UV non mostrano emissione apprezzabile ([[fig-061|Fig. 61]]): vedi [[acq-e-stato-solido]]. Ne discende la necessità del design [[bottle-brush]]. + +![[immagini/efcc22eae8c7e8ff910d35fa7c018b13417126c67a70da70eed1784a889d6d32.jpg|560]] +*Figura 61 - film solidi dei copolimeri sotto lampada UV, in ordine copolimero 3a, 3b, 3c* · [[fig-061|nota figura]] + +## GPC (r.938-952) → [[gpc]] +Mn 1400-2150 Da. Dati: + +**Tabella 8** - *pesi molecolari e polidispersità determinati mediante GPC* +| Copolimero | Massa molecolare media numerica (Da) | Massa molecolare media ponderale (Da) | Polidispersità (PD) | +| --- | --- | --- | --- | +| 3a | 2149 | 5526 | 2,571 | +| 3b | 1402 | 6439 | 4,592 | +| 3c | 2134 | 4223 | 1,979 | + +- **3a** e **3c**: Mn equiparabili (2149 e 2134 Da); **3c** ha la distribuzione più omogenea della serie (PD = 1,979). +- PD attorno a 2 o superiori sono attesi per polimerizzazione non controllata: distribuzione più probabile di Flory (rif. [[54-odian-2004|54]]). +- **3b**: Mn più basso (1402 Da) ma Mw più alta (6439 Da) → PD = 4,592; indica una frazione significativa di oligomeri a catena corta (abbassano Mn) e una porzione di macromolecole a peso molecolare più elevato (aumentano Mw). + +## DSC (r.954) → [[dsc]] +Per tutti i campioni **Tg intorno a −10 °C**; a differenza del 3HT **nessuna transizione di fusione**: conferma il copolimero **random**; l'elevato disordine impedisce la cristallizzazione nonostante i bassi pesi molecolari. (Le Conclusioni parlano invece di «temperature di fusione superiori a 110 °C»: [[difetti-noti]].) + +## Ciclovoltammetria → [[ciclovoltammetria]] +Tabella 13 (bandgap 0,970 / 1,316 / 1,371 eV per 3a/3b/3c). + +## Collegamenti +- [[dpp-2]] · [[polimerizzazione-ossidativa-fecl3]] · [[bottle-brush-3-x]] · [[bottle-brush]] · [[nmr-1h]] · [[ft-ir]] · [[uv-vis-fluorescenza]] · [[gpc]] · [[dsc]] · [[ciclovoltammetria]] · [[reagenti-e-materiali]] +- [[tesi]] · [[bibliografia]] diff --git a/wiki/compounds/dpp-1.md b/wiki/compounds/dpp-1.md new file mode 100644 index 0000000..4845657 --- /dev/null +++ b/wiki/compounds/dpp-1.md @@ -0,0 +1,91 @@ +--- +title: DPP 1 - 3,6-di(tiofen-2-il)-2,5-diidropirrolo[3,4-c]pirrolo-1,4-dione +type: compound +aliases: ["composto 1", "DPP tiofenico", "prodotto 1"] +tags: [dpp, fluoroforo, pseudo-stobbe, sintesi] +created: 2026-10-09 +updated: 2026-10-09 +tesi_loc: "§3.2 r.588-606; §4.1 r.742-770" +refs: [5, 7, 51] +figures: ["fig-x-185efd", "fig-042", "fig-043", "fig-044", "fig-045"] +status: draft +--- + +# DPP 1 - 3,6-di(tiofen-2-il)-2,5-diidropirrolo[3,4-c]pirrolo-1,4-dione + +Fluoroforo DPP con anelli tiofenici, base del monomero [[dpp-2]]. Numerazione sperimentale (cap. 3-4), da non confondere con i composti 1-48 del cap. 1 ([[difetti-noti]]). Aspetto: **solido rosso scuro/violaceo** (r.598). + +![[immagini/185efd9de96189fb7fefd271e19709d672e7eda09572a645d13092c3196248e1.jpg|560]] +*schema DPP 1 (didascalia generata dal catalogo): Sintesi del DPP 1 da 2-tiofencarbonitrile e diisopropil succinato in t-AmOH/t-AmONa con FeCl3 catalitico.* · [[fig-x-185efd|nota figura]] + +## Procedura (§3.2, r.592-596) +Pallone a tre colli da 25 mL con ancoretta magnetica e refrigerante, sotto flusso di azoto. + +| Reagente | Quantità | mmol | eq | +|---|---|---|---| +| Na(s) | 475 mg | 20,7 | 3,5 | +| alcol tert-amilico (t-AmOH) | 12 mL | 109,7 | 16,6 | +| FeCl3 | quantità catalitica | - | - | +| 2-cianotiofene (2-CNTh) | 1,9 mL | 20 | 3 | +| diisopropil succinato | 1,36 mL | 6,66 | 1,13 | + +1. Na, t-AmOH e FeCl3 catalitico: scaldati a **80 °C** (bagno d'olio), sotto agitazione fino a dissoluzione del sodio (formazione di t-AmONa). +2. Aggiunta goccia a goccia del 2-cianotiofene; temperatura a **110 °C**. +3. Gocciolamento del diisopropil succinato; reazione per **16 h**. +4. Quench: raffreddamento e aggiunta di acido acetico diluito in acqua (rapporto **1:9 V/V**). +5. Filtrazione su Büchner; lavaggi ripetuti con acqua distillata e metanolo; essiccamento in stufa a **85 °C**. + +## Caratterizzazione (§3.2, r.600-606) +| Tecnica | Dato (verbatim) | +|---|---| +| 1H NMR (400 MHz, d6-DMSO) | δ = 8.24 – 8.18 (dd, *J* = 3.8, 1.2 Hz, 4H), 8.00 – 7.93 (dd, *J* = 5.0, 1.1 Hz, 4H), 7.38 – 7.25 (m, 4H) | +| UV-Vis (THF) | 532 nm, 498 nm | +| Fluorescenza (THF) | 490 nm | + +Altri dati: λmax,abs 531 nm, λmax,ex 542 nm, Stokes shift 11 nm, ε 28000 M⁻¹ cm⁻¹ (rif. [[51-wang-2022|51]]) → Tabella 5 in [[dpp-2]]. Coerenza dei valori fra §3.2, testo di §4.1 e Tab. 5: vedi [[difetti-noti]]. + +## Meccanismo di formazione: ciclizzazione pseudo-Stobbe (§4.1, r.742, [[fig-042|Fig. 42]]) +Procedura basata sulla letteratura (rif. [[05-iqbal-1988|5]], [[07-grzybowski-2015|7]]): il derivato tiofenico reagisce con un estere succinico (qui diisopropil succinato). +1. **Base forte**: deprotona l'estere succinico in α al carbonile: il **teramilato di sodio (t-AmONa)**, ottenuto per salificazione dell'alcol ter-amilico con sodio e FeCl3 catalitico. +2. Il carbanione attacca il carbonio nitrilico del tiofene → composto imminico → tautomerizza a **enammina**. +3. L'ammina attacca il carbonile estereo in modo intramolecolare → chiusura del **primo anello a cinque termini**. +4. Seconda deprotonazione e attacco di una seconda molecola di tiofene → nuova enammina → attacco sul carbonile estereo → **secondo anello** e struttura DPP. + +![[immagini/b8095b77f46fe9daaa5430cabef072a05c35605430fd6ff6af09c38553a33d1c.jpg|560]] +*Figura 42 - meccanismo di reazione proposto per la formazione dei DPP* · [[fig-042|nota figura]] + +### Scelte di processo (r.748, [[fig-043|Fig. 43]]) +- Il tiofene è introdotto direttamente nell'ambiente di reazione **dopo la formazione dell'alcolato**. +- Il succinato è **gocciolato lentamente**: una concentrazione locale troppo alta in condizioni basiche induce reazioni parassite di **autocondensazione** (Claisen, [[fig-043|Fig. 43]]). +- Scelto il **diisopropil succinato** per aumentare l'ingombro intorno al carbonile e ridurre la possibilità di autocondensazione di Claisen e successiva ciclizzazione (rif. [[07-grzybowski-2015|7]]). Sul trend R vedi [[dpp-sintesi-letteratura]]. + +![[immagini/9cb4d6705cae60dc0e20d74685b5217ff70680872a3714cd00103f3561ad251b.jpg|560]] +*Figura 43 - meccanismo di autocondensazione di Claisen* · [[fig-043|nota figura]] + +### Purificazione (r.754) +Sfrutta la netta differenza di solubilità tra reagenti e prodotto; dopo isolamento, numerosi lavaggi con acqua e metanolo per eliminare solvente e reagenti residui. + +## Spettri e assegnazioni +### ¹H-NMR in DMSO ([[fig-044|Fig. 44]], r.762-764) +La simmetria rende equivalenti diversi gruppi di protoni → meno segnali del totale degli H. +- ~**11 ppm**: singoletto allargato dei due **protoni ammidici** dei due anelli lattamici; marcatamente deschermato per richiamo elettronico dei carbonili adiacenti, esteso sistema π-coniugato e legami a idrogeno intermolecolari con il solvente. +- Regione aromatica: segnali dei due anelli tiofenici laterali. Il **doppietto più deschermato** = protoni più vicini al core DPP. Procedendo a campi più alti, secondo doppietto = protoni adiacenti all'**eteroatomo di zolfo** (effetto induttivo). Il segnale a campi ancora maggiori, **doppietto di doppietti**, = protoni centrali dell'anello tiofenico, accoppiati con entrambi i protoni vicinali. +- Nota del catalogo: i ppm in [[fig-044|Fig. 44]] sono stimati dall'asse, non letti da etichette. + +![[immagini/5b9c36eb3db1dae7d33d24a159eb75cd575f40a33dad1110ef83da17bffaa3d9.jpg|560]] +*Figura 44 - spettro 1H-NMR in DMSO del prodotto 1* · [[fig-044|nota figura]] + +### UV-Vis ed emissione in THF ([[fig-045|Fig. 45]], r.768-770) +- Banda di assorbimento ben definita con due massimi a circa **532 nm** e **498 nm** (sistema coniugato e planare del core DPP). +- Spettro di emissione pressoché simmetrico a quello di assorbimento: massimo principale **543 nm** e spalla secondaria a circa **585 nm**. +- **Stokes shift di soli 11 nm**: l'elevata rigidità riduce i riarrangiamenti fra fondamentale ed eccitato, limitando i decadimenti non radiativi. + +![[immagini/ba9fb099eb33d86ffd10e40efffc19c6100dc56af328b2442f186b51e09433be.jpg|560]] +*Figura 45 - spettro UV-Visibile e di emissione del prodotto 1 in THF* · [[fig-045|nota figura]] + +## Ruolo nel progetto +Substrato della N-alchilazione che dà il monomero ortogonale [[dpp-2]]; poco solubile (legami a idrogeno ammidici, [[dpp-reattivita]]). Sequenza completa: [[bottle-brush]]. + +## Collegamenti +- [[dpp-2]] · [[dpp-sintesi-letteratura]] · [[dpp-struttura-e-proprieta]] · [[nmr-1h]] · [[uv-vis-fluorescenza]] · [[reagenti-e-materiali]] +- [[tesi]] · [[bibliografia]] diff --git a/wiki/compounds/dpp-2.md b/wiki/compounds/dpp-2.md new file mode 100644 index 0000000..7cf565e --- /dev/null +++ b/wiki/compounds/dpp-2.md @@ -0,0 +1,102 @@ +--- +title: DPP 2 - 2,5-bis(6-idrossiesil)-3,6-di(tiofen-2-il)-2,5-diidropirrolo[3,4-c]pirrolo-1,4-dione +type: compound +aliases: ["composto 2", "DPP bis-alchilato", "monomero ortogonale", "prodotto 2"] +tags: [dpp, monomero, n-alchilazione, ossidrile] +created: 2026-10-09 +updated: 2026-10-09 +tesi_loc: "§3.2 r.608-626; §4.1 r.772-823" +refs: [51] +figures: ["fig-x-f6eeb1", "fig-046", "fig-047", "fig-048", "fig-049", "fig-050", "fig-051"] +status: draft +--- + +# DPP 2 - 2,5-bis(6-idrossiesil)-3,6-di(tiofen-2-il)-2,5-diidropirrolo[3,4-c]pirrolo-1,4-dione + +Monomero «ortogonale e tetrafunzionale» (§4.1, r.772): anelli tiofenici per la polimerizzazione ossidativa, due -OH come unità diolica o iniziatori per ROP ([[bottle-brush]]). Ottenuto da [[dpp-1]]. Numerazione sperimentale. + +![[immagini/f6eeb10de88591bd0358f146073c675489133b4c8bb70f71131b343bb8a25794.jpg|560]] +*schema DPP 2 (didascalia generata dal catalogo): Alchilazione del DPP 1 con 6-bromoesan-1-olo (DMSO, t-BuOK, 40 °C, 16 h) a dare il DPP 2 con due catene idrossiesiliche.* · [[fig-x-f6eeb1|nota figura]] + +## Procedura (§3.2, r.612-616) +Pallone a 3 colli da 50 mL con ancoretta e refrigerante. + +| Reagente | Quantità | mmol | eq | +|---|---|---|---| +| DPP **1** | 1 g | 3,32 | 1 | +| DMSO | 18,75 mL (6,25 mL/mmol di DPP) | - | - | +| t-BuOK | 1,1 g | 0,01 mol (come riportato) | 3 | +| 6-bromoesanolo | 1,08 mL | 8,3 | 1,25 | + +1. Inertizzazione con cicli vuoto/azoto; aggiunta di t-BuOK; miscela a **40 °C**. +2. Dopo **10 min**, gocciolamento di 6-bromoesanolo; reazione per **16 h**. +3. Work-up: grezzo in imbuto separatore da 250 mL con **100 mL di DCM**; fase organica lavata **3 volte con 100 mL di soluzione satura di KCl**; anidrificazione con Na2SO4; filtrazione su filtro a pieghe; evaporazione al rotavapor. +4. Purificazione per **cristallizzazione in etanolo**: solido sciolto a caldo nella minima quantità di solvente; **freezer a −20 °C per 24 h**; precipitato scuro = DPP bis-alchilato **2**; stufa a **85 °C** fino a eliminazione del solvente. + +## Caratterizzazione (§3.2, r.618-626) +| Tecnica | Dato (verbatim) | +|---|---| +| 1H NMR (400 MHz, CDCl3) | δ 8.96 – 8.84 (m, 1H), 7.67 – 7.58 (m, 1H), 7.33 – 7.19 (m, 2H), 4.17 – 4.04 (m, 2H), 3.73 – 3.59 (t, *J* = 6.4 Hz, 2H), 1.82 – 1.20 (m, 9H) | +| IR (ATR) | 3350, 3070, 2920, 2850, 1645, 1555, 1495, 1440, 1390, 820, 730 cm⁻¹ | +| UV-Vis (THF) | 541 nm | +| Fluorescenza (THF) | 540 nm | + +Per la coerenza dei valori fra §3.2 e Tabella 5 vedi [[difetti-noti]]. + +## Reazione di N-alchilazione (§4.1, r.772-790) +- Sfrutta la reattività descritta in [[dpp-reattivita]] (§1.1.2, «Reazioni su gruppi ammidici come nucleofili») su **entrambi gli azoti ammidici**, con **6-bromo-1-esanolo**. +- Meccanismo ([[fig-046|Fig. 46]]): sostituzione nucleofila; l'azoto ammidico, deprotonato da **t-BuOK**, attacca il carbonio alifatico adiacente al bromo. +- **Controllo della base** (r.782, [[fig-047|Fig. 47]]): un eccesso di base favorisce una reazione collaterale di **ciclizzazione del 6-bromo-1-esanolo**. +- Work-up: estrazioni liquido-liquido per allontanare impurezze idrosolubili (sali inorganici, eccessi di base, tracce di solvente); fase organica in DCM lavata con KCl saturo, essiccata su Na2SO4 anidro e filtrata; poi purificazione. +- Purificazione per cristallizzazione in etanolo: grezzo sciolto a caldo nella minima quantità di etanolo; precipitazione lenta con raffreddamento prolungato a −20 °C; le impurità restano nelle acque madri; il **precipitato scuro** (DPP bis-alchilato) è recuperato per filtrazione. Caratterizzato con NMR e FT-IR. + +![[immagini/9b67a0c4119927bb79c04800ab73ca66e034387467484976be81ef31499a5cfb.jpg|560]] +*Figura 46 - meccanismo della reazione di N-alchilazione* · [[fig-046|nota figura]] + +![[immagini/de181218223f66cd046706d8723e5010aa9d7a8779b172c877562b47a100738d.jpg|560]] +*Figura 47 - reazione di ciclizzazione del 6-bromo-1-esanolo* · [[fig-047|nota figura]] + +## ¹H-NMR in CDCl3 ([[fig-048|Fig. 48]], r.796) +- Regione aromatica: tre segnali distinti dei protoni tiofenici. Il più indicativo è un **doppietto a ~8,9 ppm**, protoni fortemente deschermati dai carbonili adiacenti del core DPP; gli altri due a **7,6 ppm** e **7,3 ppm**. +- Avvenuta N-alchilazione: due multipletti alifatici: **4,1 ppm** (metileni legati all'azoto lattamico, più deschermati) e **3,6 ppm** (metileni adiacenti all'ossidrile terminale). +- Gli altri metileni della catena: multipletti fra **1 e 2 ppm**. + +![[immagini/d22ce85e035853dee124b1608b0cb176c370dc95ec3ab560926836261887394e.jpg|560]] +*Figura 48 - spettro 1H-NMR in CDCl3 del prodotto 2* · [[fig-048|nota figura]] + +## FT-IR ([[fig-049|Fig. 49]], r.802) +| Numero d'onda | Assegnazione | +|---|---| +| ~3400 cm⁻¹ (banda larga) | stretching O-H dei gruppi alcolici terminali | +| ~3100 cm⁻¹ (segnali deboli) | stretching C-H aromatici degli anelli tiofenici | +| 2930 e 2850 cm⁻¹ (picchi netti) | stretching asimmetrico e simmetrico dei C-H alifatici dei metileni | +| ~1650 cm⁻¹ (molto intensa) | stretching C=O dei lattami in sistemi coniugati, tipica dei DPP (segnale più indicativo) | +| 1500-1400 cm⁻¹ | stretching C=C degli anelli aromatici e del core | +| fingerprint | picchi compatibili con stretching C-O degli alcoli primari e bending dei C-H tiofenici | + +(La nota del catalogo segnala [[fig-049|Fig. 49]] come ritagliata.) + +![[immagini/f890cc2c6264ef44ec1b471578277dc04114da1baa30e1f6aa17bb7f674615e8.jpg|560]] +*Figura 49 - spettro FT-IR del prodotto 2* · [[fig-049|nota figura]] + +## Proprietà foto-fisiche e Tabella 5 (r.804-823) +- Dopo l'alchilazione: **spostamento batocromico** del massimo di assorbimento, da **531 nm (1)** a **541 nm (2)**. Spiegazione: effetto induttivo elettron-donatore delle catene alifatiche, che arricchiscono la densità elettronica sugli azoti → **destabilizzazione dell'HOMO** → restringimento del bandgap ottico. Lo Stokes shift è simile per entrambi (nel testo «circa 14 nm»; in tabella 11 e 14 nm). + +| Prodotto | λmax, abs (nm) | λmax, ex (nm) | Stokes shift (nm) | ε (M-1 cm-1) | +| --- | --- | --- | --- | --- | +| 1 | 531 | 542 | 11 | 28000 (rif. [[51-wang-2022\|51]]) | +| 2 | 541 | 555 | 14 | 13218 | + +**Tabella 5** - *dati spettroscopici dei fluorofori sintetizzati* + +![[immagini/75c7d0cf12baae0fe259352e5495ea053607717f5a57233f468098343f6693c7.jpg|560]] +*Figura 50 - spettro UV-Visibile e di emissione del prodotto2 in THF* · [[fig-050|nota figura]] + +- **Coefficiente di estinzione molare di 2**: retta di calibrazione dall'assorbanza (spettrofotometria) di soluzioni di fluoroforo in **CHCl3** a concentrazione nota; per Lambert-Beer la pendenza è ε: **13218 M⁻¹ cm⁻¹** ([[fig-051|Fig. 51]]). + +![[immagini/336837d03a78ea923cf3fa1ae976385b52eefe8ab91dccfdff63f3bb33ecfc6b.jpg|560]] +*Figura 51 - retta di calibrazione del fluoroforo 2 per il calcolo di ε* · [[fig-051|nota figura]] + +## Collegamenti +- [[dpp-1]] · [[dpp-reattivita]] · [[bottle-brush]] · [[copolimeri-3a-3b-3c]] · [[nmr-1h]] · [[ft-ir]] · [[uv-vis-fluorescenza]] · [[reagenti-e-materiali]] +- [[tesi]] · [[bibliografia]] diff --git a/wiki/compounds/reagenti-e-materiali.md b/wiki/compounds/reagenti-e-materiali.md new file mode 100644 index 0000000..382303e --- /dev/null +++ b/wiki/compounds/reagenti-e-materiali.md @@ -0,0 +1,41 @@ +--- +title: Reagenti, solventi e materiali +type: compound +tags: [reagenti, solventi, materiali-e-metodi] +created: 2026-10-09 +updated: 2026-10-09 +tesi_loc: "§3.1 r.567-569; §3.2 r.588-663; §3.4 r.704-714" +refs: [] +figures: [] +status: draft +--- + +# Reagenti, solventi e materiali + +Riepilogo dei reagenti citati nella parte sperimentale (dove sono usati e con quale ruolo). Le quantità sono nelle pagine dei composti. + +## Trattamento dei solventi (§3.1, r.569) +Reagenti e solventi commerciali ad elevato grado di purezza, **usati senza ulteriori purificazioni** salvo: +- **CHCl3**: anidrificato per distillazione in apparato **Claisen** con **calcio idruro**. +- **THF**: purificato a pressione ridotta con evaporatore rotante per rimuovere lo stabilizzante («THF sbiancato»). + +## Reagenti per passaggio +| Passaggio | Reagente | Ruolo | Pagina | +|---|---|---|---| +| DPP **1** | Na, t-AmOH, FeCl3 (cat.) | formazione di t-AmONa (base) | [[dpp-1]] | +| DPP **1** | 2-cianotiofene (2-CNTh) | fonte dell'anello tiofenico e del nitrile | [[dpp-1]] | +| DPP **1** | diisopropil succinato | estere succinico, gocciolato lentamente | [[dpp-1]] | +| DPP **1** | acido acetico diluito in acqua (1:9 V/V) | quench; poi lavaggi con acqua e metanolo | [[dpp-1]] | +| DPP **2** | DMSO, t-BuOK | solvente, base | [[dpp-2]] | +| DPP **2** | 6-bromoesanolo | agente alchilante con -OH | [[dpp-2]] | +| DPP **2** | DCM, KCl sat., Na2SO4, etanolo | work-up e cristallizzazione | [[dpp-2]] | +| 3a-c | 3-esiltiofene (3HT) | comonomero donatore | [[copolimeri-3a-3b-3c]] | +| 3a-c | FeCl3, nitrometano, CHCl3 anidro | ossidante, legante moderatore, solvente | [[polimerizzazione-ossidativa-fecl3]] | +| 3a-c | THF sbiancato, HCl 0,6 M, NaCl sat., metanolo freddo | quench, rimozione Fe, anidrificazione, precipitazione | [[copolimeri-3a-3b-3c]] | +| bottle brush | ε-caprolattone, toluene, Sn(Oct)2 | monomero, solvente, catalizzatore | [[bottle-brush-3-x]], [[rop-pcl]] | +| CV | THF, TBAPF6 0,1 M, ferrocene | solvente, elettrolita, standard interno | [[ciclovoltammetria]] | + +Strumenti: [[nmr-1h]], [[ft-ir]], [[gpc]], [[uv-vis-fluorescenza]], [[dsc]], [[ciclovoltammetria]]. + +## Collegamenti +- [[tesi]] diff --git a/wiki/concepts/acq-e-stato-solido.md b/wiki/concepts/acq-e-stato-solido.md new file mode 100644 index 0000000..6491a83 --- /dev/null +++ b/wiki/concepts/acq-e-stato-solido.md @@ -0,0 +1,70 @@ +--- +title: ACQ e comportamento ottico allo stato solido +type: concept +tags: [acq, aggregazione, pi-stacking, stato-solido, aggregati-h, aggregati-j, eccimeri] +created: 2026-10-09 +updated: 2026-10-09 +tesi_loc: "§2 r.549-553; §4.2 r.930-936; §4.3 r.959-963; §4.5 r.1254-1276; §5 r.1287" +refs: [58, 59] +figures: ["fig-061", "fig-062", "fig-074"] +status: draft +--- + +# ACQ e comportamento ottico allo stato solido + +**ACQ = Aggregation-Caused Quenching**: spegnimento dell'emissione indotto dall'aggregazione. È il problema che la tesi vuole superare ([[bottle-brush]]). + +## Definizione e problema (§2, r.549-553; Abstract r.27) +- I materiali semiconduttori π-coniugati spesso perdono le proprietà ottiche allo stato solido. Causa: natura altamente **planare** dello scheletro molecolare → forti interazioni di **π-stacking** tra catene adiacenti → drastico smorzamento della fluorescenza (e dissipazione non radiativa dell'energia). +- Obiettivo del progetto: semiconduttori polimerici emissivi che superino l'ACQ con architetture a spazzola, per **separare fisicamente i segmenti planari coniugati**, ripristinando le proprietà emissive allo stato solido e preservando integrità elettrochimica e stabilità. +- Origine nel DPP: legami a idrogeno e π-π stacking a 0,334 nm → [[dpp-struttura-e-proprieta]]. + +## Evidenza sperimentale sui copolimeri lineari (§4.2, r.930-936) +- In soluzione diluita (THF) i copolimeri [[copolimeri-3a-3b-3c]] mantengono eccellenti caratteristiche emissive (λmax abs ~540-545 nm, em ~550 nm, Stokes shift ridotto). +- Allo stato solido il comportamento è drasticamente diverso: l'intenso impaccamento delle catene forma aggregati che disattivano i fluorofori per decadimento non radiativo. I film su vetrino sotto lampada UV **non mostrano emissione apprezzabile** ([[fig-061|Fig. 61]]). +- Questa tendenza è «la principale criticità per l'impiego di tali sistemi lineari in dispositivi optoelettronici» e giustifica il passaggio al design bottle brush. + +![[immagini/efcc22eae8c7e8ff910d35fa7c018b13417126c67a70da70eed1784a889d6d32.jpg|560]] +*Figura 61 - film solidi dei copolimeri sotto lampada UV, in ordine copolimero 3a, 3b, 3c* · [[fig-061|nota figura]] + +## Razionale dell'effetto sterico (§4.3, r.959-963) +- Scopo del design bottle brush: limitare l'impaccamento intermolecolare tra le catene dei copolimeri; l'ingombro sterico delle catene laterali isola i backbone, migliora le proprietà spettroscopiche, limita il quenching da aggregazione e favorisce mobilità e flessibilità delle catene. +- [[fig-062|Fig. 62]] illustra l'effetto dell'intensità dello stacking π-π sull'emissione. Nel disegno la lampadina barrata sta sotto «Deboli interazioni» e quella accesa sotto «Forti interazioni», senza spiegazione nel testo (nota del catalogo: vedi [[difetti-noti]]). + +![[immagini/a3ecc2457962649d36b1824710784bec90b0e52d32275fc154743f9bf9f62339.jpg|560]] +*Figura 62 - effetto dell'intensità dello stacking π-π sull'emissione luminosa* · [[fig-062|nota figura]] + +## Caratterizzazione spettroscopica allo stato solido (§4.5, r.1254-1276) + +### Premessa teorica (r.1256-1264) +- Le misure in soluzione diluita indagano la singola catena isolata e solvatata; allo stato solido la vicinanza tra macromolecole genera forti interazioni intermolecolari che alterano i livelli energetici di banda e i processi di assorbimento ed emissione. +- **Assorbimento solido**: limitata mobilità conformazionale e forte impaccamento inducono maggiore **planarizzazione** dello scheletro; delocalizzazione più estesa lungo il backbone → aumento della lunghezza di coniugazione effettiva → spostamento **batocromo** del massimo e, spesso, struttura vibronica più risolta (indice di ordine strutturale locale). +- **Teoria dell'accoppiamento eccitonico di Kasha**: impaccamento in due geometrie principali: **aggregati H** (face-to-face, prevalgono le interazioni π-π laterali) e **aggregati J** (head-to-tail). Nei polimeri coniugati le forti interazioni π-π favoriscono frequentemente gli aggregati H, con transizione otticamente permessa verso lo stato eccitonico a maggiore energia (rif. [[58-kasha-1965|58]]). +- **Emissione**: il fenomeno più comune nei sistemi π-coniugati planari è l'ACQ. Vicinanza degli anelli aromatici e aggregati H favoriscono il rilassamento non radiativo degli eccitoni (formazione di **eccimeri** o trasferimento di energia verso siti di smorzamento: difetti conformazionali, trappole energetiche); le rese quantiche allo stato solido calano drasticamente rispetto alla soluzione (rif. [[59-spano-2014|59]]). +- **Copolimeri D-A**: presenza della banda di trasferimento di carica intramolecolare (**ICT**); l'impaccamento solido riduce le distanze intermolecolari, facilitando anche il trasferimento di carica intermolecolare. Con forti cromofori accettori e unità donatrici (derivati tiofenici) la tendenza a impaccamento e cristallizzazione è notevole. +- **Contromisure**: ingombri sterici mirati (catene alchiliche ramificate, innesti polimerici laterali, **architetture bottle brush**) fanno da spaziatori fisici: mantengono la coniugazione sul backbone, ostacolano l'avvicinamento dei piani π, limitano la formazione di aggregati H non radiativi e preservano in parte l'emissione. + +### Misura sul polimero 3.2b ([[fig-074|Fig. 74]], r.1266-1276) +Analisi combinata UV-Vis ed emissione allo stato solido sul campione rappresentativo [[bottle-brush-3-x]] 3.2b; confronto soluzione liquida (LS) / stato solido (SS). + +| Grandezza | Soluzione (LS) | Stato solido (SS) | +|---|---|---| +| Massimo di assorbimento | circa 550 nm, banda principale | intervallo 570-580 nm; significativo allargamento e marcato batocromico; variazione dell'intensità relativa della spalla vibronica a energie maggiori | +| Massimo di emissione | circa 560-565 nm; banda stretta e strutturata | circa 650-660 nm; banda notevolmente allargata e fortemente red-shiftata | +| Stokes shift | ridotto (rilassamento radiativo da singola catena isolata) | circa 80-90 nm | + +- Il red-shift dell'assorbimento solido è attribuito alla **planarizzazione del backbone** indotta dai vincoli conformazionali, con estensione della lunghezza di coniugazione effettiva. +- L'elevato Stokes shift allo stato solido è «probabilmente legato a un maggiore ingombro delle catene polimeriche, che obbliga gli anelli aromatici ad assumere torsioni maggiori» ed è anche chiara evidenza della forte aggregazione intermolecolare. +- Interpretazione: dopo fotoeccitazione l'energia migra verso siti a minore energia generati dalla vicinanza dei piani coniugati (interazioni π-π); il rilassamento radiativo avviene prevalentemente da **stati aggregati o specie eccimeriche**, non da catene isolate. +- Conclusione del paragrafo: forte riarrangiamento strutturale allo stato solido, che definisce il profilo fotofisico del materiale. + +![[immagini/04f625a8b25744bf2d07d569e55558174b59a5cb564c8bdd0a53c704dfbde545.jpg|560]] +*Figura 74 - confronto tra spettri UV-Vis (in nero) ed emissione (in rosso) del polimero 3.2.b in soluzione (linea continua) e allo stato solido (linea tratteggiata)* · [[fig-074|nota figura]] + +## Esito dichiarato in Abstract e Conclusioni (r.19, r.1287) +Nel solido il PCL agisce da **spaziatore sterico**, limita l'impaccamento e consente un'apprezzabile emissione nel **rosso**, attenuando le vie di disattivazione non radiativa tipiche dell'ACQ. Le Conclusioni precisano: nonostante i riarrangiamenti (assorbimento fino a 570-580 nm, emissione red-shift a ~650-660 nm), l'architettura bottle brush ha mantenuto «un'apprezzabile emissione nel rosso, attenuando i percorsi di disattivazione non radiativa totale tipici dell'ACQ non controllato». Nota: la tesi mostra lo spettro solido solo per 3.2b e non riporta rese quantiche allo stato solido _(osservazione sul testo, non nuova affermazione)_. + +## Collegamenti +- [[bottle-brush]] · [[dpp-struttura-e-proprieta]] · [[fluorescenza]] · [[uv-vis-fluorescenza]] +- [[copolimeri-3a-3b-3c]] · [[bottle-brush-3-x]] +- [[tesi]] · [[bibliografia]] diff --git a/wiki/concepts/bottle-brush.md b/wiki/concepts/bottle-brush.md new file mode 100644 index 0000000..e9d2809 --- /dev/null +++ b/wiki/concepts/bottle-brush.md @@ -0,0 +1,57 @@ +--- +title: Architettura bottle brush - strategia del progetto +type: concept +tags: [bottle-brush, grafting-from, design, strategia] +created: 2026-10-09 +updated: 2026-10-09 +tesi_loc: "Riassunto/Abstract r.15-33; §2 r.545-559; §4.3 r.957-979; §5 r.1281-1291" +refs: [] +figures: ["fig-062", "fig-x-185efd", "fig-x-f6eeb1", "fig-x-cc3f54", "fig-x-136800"] +status: draft +--- + +# Architettura bottle brush - strategia del progetto + +Pagina «hub»: riunisce la logica di progetto. I dati stanno nelle pagine collegate. + +## Obiettivo e ipotesi (§2, r.551-553) +Sviluppare semiconduttori polimerici emissivi che superino i limiti dell'[[acq-e-stato-solido]] con **copolimeri a spazzola (bottle brush)**, promuovendo la separazione fisica dei segmenti planari coniugati: ripristinare ed esaltare le proprietà emissive allo stato solido preservando integrità elettrochimica e stabilità. Il bottle brush è «a spazzola»: scheletro coniugato (backbone) con catene laterali flessibili innestate. + +## Il monomero ortogonale (§2 r.555; §4.1 r.772-774) +Il monomero [[dpp-2]] ha funzioni indipendenti, per questo detto «ortogonale e tetrafunzionale»: +- **anelli tiofenici** → polimerizzazione ossidativa con FeCl3 ([[polimerizzazione-ossidativa-fecl3]]) per lo scheletro coniugato; +- **gruppi -OH** → assimilano la struttura a un'unità monomerica **diolica** (utilizzabile in policondensazioni con opportuni comonomeri) e fungono da **iniziatori** per ROP di monomeri ciclici ([[rop-pcl]]). + +## Sequenza di sintesi (fig. di schema) +| Passo | Reazione | Prodotto | Pagina | +|---|---|---|---| +| 1 | 2-cianotiofene + diisopropil succinato, t-AmONa (pseudo-Stobbe) | DPP **1** | [[dpp-1]] ([[fig-x-185efd\|schema DPP 1]]) | +| 2 | N-alchilazione con 6-bromo-1-esanolo, t-BuOK, DMSO | monomero **2** | [[dpp-2]] ([[fig-x-f6eeb1\|schema DPP 2]]) | +| 3 | polimerizzazione ossidativa di **2** con 3HT, FeCl3/CH3NO2, CHCl3 | copolimeri statistici **3a, 3b, 3c** | [[copolimeri-3a-3b-3c]] ([[fig-x-cc3f54\|schema copolimeri]]) | +| 4 | ROP dell'ε-caprolattone, Sn(Oct)2, toluene, 110 °C | bottle brush **3.1b-3.3c** | [[bottle-brush-3-x]] ([[fig-x-136800\|schema bottle brush]]) | + +Distribuzione statistica dei monomeri lungo la catena (§2, r.555): aumenta l'entropia conformazionale, limita il packing e l'ordine costituzionale → riduce l'aggregazione delle catene principali e rende i gruppi idrossilici più accessibili per la funzionalizzazione. + +## Scelta dei macroiniziatori (§4.3, r.977) +Serie preparate da **3b** e **3c**; il copolimero **3a** non è stato usato per il grafting «a causa della scarsa efficienza della sua via sintetica»: basse rese e difficoltà di work-up per isolare il prodotto puro (perdite di materiale); isolare quantità utili avrebbe richiesto volumi di solventi e costi di reagenti molto elevati → per fattibilità tecnica ed economica solo **3b** e **3c**. + +## Cosa dimostrano i dati (rimandi) +| Aspetto | Esito nella tesi | Dove | +|---|---|---| +| Innesto delle catene | FT-IR: scompare -OH, compare C=O a ~1720 cm⁻¹; ¹H-NMR: segnali PCL | [[ft-ir]], [[nmr-1h]] | +| Dimensione macromolecolare | GPC sottostimata dalla compattezza dell'architettura; Mn da ¹H-NMR (Tab. 12) | [[gpc]], [[bottle-brush-3-x]] | +| Integrità del core in soluzione | λmax abs 544-554 nm, em 557-564 nm, Stokes shift 8-14 nm | [[uv-vis-fluorescenza]] | +| Emissione allo stato solido | spettro SS di 3.2b: abs 570-580 nm, em ~650-660 nm | [[acq-e-stato-solido]] | +| Proprietà termiche | dominate dal PCL: Tm 55-60 °C, Tc 25-35 °C | [[dsc]] | +| Elettroattività | processi redox EC irreversibili; bandgap 0,929-1,521 eV | [[ciclovoltammetria]] | + +## Messaggio conclusivo (§5, r.1291) +«L'approccio ortogonale basato su scheletri semiconduttori DPP-3HT modificati mediante catene laterali di PCL consente di combinare proprietà elettrochimiche modulabili e capacità emissiva allo stato solido.» + +![[immagini/a3ecc2457962649d36b1824710784bec90b0e52d32275fc154743f9bf9f62339.jpg|560]] +*Figura 62 - effetto dell'intensità dello stacking π-π sull'emissione luminosa* · [[fig-062|nota figura]] + +## Collegamenti +- [[acq-e-stato-solido]] · [[rop-pcl]] · [[polimerizzazione-ossidativa-fecl3]] · [[fluorofori-in-polimeri]] +- [[dpp-1]] · [[dpp-2]] · [[copolimeri-3a-3b-3c]] · [[bottle-brush-3-x]] +- [[tesi]] · [[overview]] diff --git a/wiki/concepts/dpp-reattivita.md b/wiki/concepts/dpp-reattivita.md new file mode 100644 index 0000000..0b86234 --- /dev/null +++ b/wiki/concepts/dpp-reattivita.md @@ -0,0 +1,128 @@ +--- +title: DPP - reattività e funzionalizzazione +type: concept +tags: [dpp, reattività, n-alchilazione, cross-coupling, arilazione, litiazione, snar] +created: 2026-10-09 +updated: 2026-10-09 +tesi_loc: "§1.1.2 r.247-373" +refs: [2, 5, 7, 21, 22, 23, 24, 25, 26, 27, 28, 29, 30, 31, 32] +figures: ["fig-017", "fig-018", "fig-019", "fig-020", "fig-021", "fig-022", "fig-023", "fig-024", "fig-025", "fig-026", "fig-027", "fig-028", "fig-029", "fig-030"] +status: draft +--- + +# DPP - reattività e funzionalizzazione + +Seconda parte del §1.1.2. «Nei paragrafi successivi sono riportate le reazioni che più comunemente vengono effettuate su questa famiglia di molecole, alcune delle quali utilizzate nel corso dell'attività sperimentale» (r.257). La reattività è varia per via dei diversi centri reattivi e del grande numero di sostituenti introducibili sull'anello aromatico (rif. [[07-grzybowski-2015|7]], r.247). + +> **Numerazione.** I composti di questa pagina (22-48...) usano la numerazione del cap. 1, diversa da quella dei composti sperimentali 1 e 2 ([[dpp-1]], [[dpp-2]]). Figure con numerazione dubbia: [[fig-026|Fig. 26]], [[fig-027|Fig. 27]], [[fig-029|Fig. 29]] (vedi [[difetti-noti]]). + +## Mappa dei siti reattivi ([[fig-017|Fig. 17]], r.249-255; rif. [[02-shaikh-2022|2]]) +Due macrocategorie. + +| Categoria | Sito (lettera in [[fig-017\|Fig. 17]]) | Reattività citata | +|---|---|---| +| Elettrofili (attacco nucleofilo) | carbonili ammidici (**a**) | - | +| | carbonio 3 e 6 (**b**) | addizione di Michael | +| | anelli aromatici con EWG in certe posizioni (**c**, **d**) | reazioni sugli anelli | +| Nucleofili (attaccano un elettrofilo) | ossigeno del carbonile (**e**) | dopo tautomeria è un ottimo nucleofilo | +| | azoto del lattame (**f**) | dopo deprotonazione attacca un elettrofilo | +| | posizioni 3 e 6 degli anelli aromatici (**g**) | SNAr, grazie all'effetto elettron-attrattore del core DPP | +| | funzionalità nucleofile sugli anelli aromatici (**h**) | reazioni con elettrofili | +| Estensione della coniugazione | alogeni su DPP alogenati (**i**) | oligomeri/polimeri per cross-coupling con reattivi organometallici | + +![[immagini/95db13c0d0b8c409535d4e0501600f0d207c24ed35d9e6dcbd1478b16f470d32.jpg|560]] +*Figura 17 - reattività dei dichetopirrolopirroli2* · [[fig-017|nota figura]] + +## 1. Reazioni sui gruppi ammidici come nucleofili (r.259-281) +- Sostituzione nucleofila favorita da gruppi ammidici facilmente deprotonabili con basi forti. +- **Deprotonazione** ([[fig-018|Fig. 18]]): la carica negativa si distribuisce tra N e O dello stesso gruppo ammidico (**22**, **23**) e può spostarsi sul secondo ossigeno, dando la struttura mesomerica (**24**) con unità pirrolica aromatica; anione fortemente stabilizzato → acidità dei protoni ammidici relativamente elevata. +- La reazione è influenzata dai sostituenti sugli anelli aromatici (effetto sterico e mesomerico sulla carica; modificano anche la solubilità) (rif. [[21-colonna-2007|21]]). La scarsa solubilità del DPP è un ostacolo: servono solventi che lo solubilizzino almeno parzialmente; i **polari aprotici**, in particolare **DMF**, sono i più usati. +- **Scopo più comune**: introdurre catene alchiliche sull'azoto per modificare la solubilità, eliminando i legami a idrogeno ammidici. L'aggiunta di un semplice gruppo metile aumenta la solubilità di **27 volte in DMF** (rif. [[05-iqbal-1988|5]]). +- **Protezione con Boc** (gruppi ter-butossicarbonilici; rif. [[22-zambounis-nd|22]]; [[fig-019|Fig. 19]]): aumenta la solubilità; per decomposizione termica il Boc si rimuove facilmente dando il DPP non protetto in modo quantitativo. +- **Pigmenti «latenti»** (rif. [[23-yue-2014|23]], [[24-zambounis-1997|24]]): i DPP protetti da Boc, ben solubili, si distribuiscono omogeneamente nel polimero; riscaldando la matrice si forma il materiale colorato con il pigmento DPP non protetto. +- **SNAr con l'azoto ammidico nucleofilo**: efficace solo con fluoroareni molto elettron-poveri (es. 1-fluoro-2,4-dinitrobenzene); non funziona con arili meno elettron-poveri (es. 4-nitrofluorobenzene) o con alogeni diversi dal fluoro. Würthner et al.: la SNAr dei DPP può essere eseguita anche con 1-fluoro-2-nitro-4-(trifluorometil)benzene (rif. [[23-yue-2014|23]]). + +![[immagini/ae4331727c45faf9a9b2dcf15ab197430625cbbd896ae767a1558fba1d404205.jpg|560]] +*Figura 18 - deprotonazione stabilizzata per risonanza mesomerica del DPP* · [[fig-018|nota figura]] + +![[immagini/b9a386a9e36a6d42b793aa25702aacb59f0a71bdbccf09d9a281c8ea9b7e6d3e.jpg|560]] +*Figura 19 - reazione di protezione e deprotezione con gruppo Boc* · [[fig-019|nota figura]] + +## 2. Reazioni sugli anelli aromatici (r.283-305) +I sostituenti arilici derivanti dai benzonitrili di partenza sono considerati parte integrante della struttura e danno reazioni aromatiche tipiche, come le sostituzioni elettrofile aromatiche (SeAr). + +- **Solfonazione, bromurazione, clorurazione del DPP 3** ([[fig-020|Fig. 20]]): con acido solforico fumante → DPP **26** con gruppi solfonici in *para*; con bromo → SeAr, DPP **27** *para*-dibromurato; con cloro → addizione ai doppi legami dell'unità centrale (**28**). La bromurazione di **3** ha resa >80%, ma — dice il testo — «il DPP **26** si può ottenere più semplicemente partendo dal 4-bromobenzonitrile» con il metodo di Iqbal ([[dpp-sintesi-letteratura]]). Nel testo il numero è **26** (il solfonato); dal contesto il prodotto bromurato è **27** _(inferenza, possibile refuso: vedi [[difetti-noti]])_. +- **Bromurazione di DPP N,N'-disostituiti con eteroaromatici in 3 e 6** (tiofene, furano, selenofene; [[fig-021|Fig. 21]]): per l'alta densità elettronica reagiscono con NBS dando i derivati bromurati con buone rese; per i DPP **29** e **30** si può usare anche bromo elementare. +- I DPP **32**, **33**, **34** sono difficili da ottenere con il metodo esteri succinici + nitrili: in condizioni fortemente basiche gli atomi di bromo dei nitrili subiscono sostituzione nucleofila (rese più basse, purificazione complicata). +- **Gryko et al.** (rif. [[07-grzybowski-2015|7]]; [[fig-022|Fig. 22]]): DPP con sostituenti aromatici elettron-ricchi alchilati in DMF con K2CO3 come base e tetrabutilammonio bisolfato (TBAHS) come catalizzatore a trasferimento di fase → diacetali (**35**); con un acido forte di Brønsted si trasformano nei derivati carbonilici e danno ciclizzazione elettrofila dell'anello aromatico elettron-ricco adiacente → pigmenti con almeno sei anelli fusi π-coniugati (**36**) con particolari caratteristiche fotofisiche. + +![[immagini/a6d0c2b1e32b84cb966e857c4cb74e90468ba7853ea4180a685a1f3226e2caad.jpg|560]] +*Figura 20 - reazioni di sostituzione elettrofile aromatiche sugli anelli del DPP 3* · [[fig-020|nota figura]] + +![[immagini/b933e7c220a76882cc561e62bcab44a9ed60335dcafa353618f0a3a8eb36ade4.jpg|560]] +*Figura 21 - bromurazione del DPP con sostituenti eteroaromatici in posizione 3 e 6* · [[fig-021|nota figura]] + +![[immagini/1d7d62195b9dfac2fc36ce6c359e0d5ed64e249c8967e57beb30b7fa6135e67c.jpg|560]] +*Figura 22 - reazione di ciclizzazione mediante sostituzione elettrofila aromatica sui DPP studiata da Gryko et al.7* · [[fig-022|nota figura]] + +## 3. Cross-coupling catalizzato da Pd (r.307-331) +- I composti **32**, **33**, **34**, **37** sono usati come in [[fig-023|Fig. 23]]: alte rese, sostituzione degli Br con gruppi arilici, alchilici e amminici. +- Oltre a espandere il sistema π, servono per polimeri π-coniugati a base di DPP; reazioni più usate: **Suzuki** e **Stille**. Composti aromatici bifunzionali polimerizzano con i DPP bromurati **32**-**34** e **37** con catalizzatori al Pd con buone rese ([[fig-024|Fig. 24]]). +- Nella [[fig-024|Fig. 24]] i co-monomeri sono derivati di: tiofene, 2,2'-bitienile, naftalene, 9,9-dialchilfluorene, tienotiofene, benzene, N-alchilcarbazolo. +- Legenda [[fig-024|Fig. 24]]: **X** = S, O, Se, -CH=CH-; **Y** = B(OH)2, B(OAlc)2, SnAlc3; **R1** = alchile, arile, acile; **R2** = H, alchile, OAlchile. +- Per solubilità e processabilità si partono da DPP con sostituenti alifatici a catena lunga o ramificati, polimerizzati con aromatici ricchi di elettroni → polimeri **donatore-accettore** (carattere elettron-accettore del DPP): alta mobilità di carica, banda proibita a bassa energia; applicazioni in **OFET** e fotovoltaico organico (**OPV**) (rif. [[25-tieke-2010|25]], [[26-li-2013|26]]). +- **Limiti di Suzuki/Stille**: richiedono pre-attivazione (Br da un lato; gruppi boronici o trialchilstannici dall'altro). Gli acidi/esteri boronici e organostannici sono più complessi da sintetizzare (condizioni drastiche, reagenti come **BuLi**), purificazione più difficile, composti organostannici altamente tossici. +- Alternative per i legami biarilici (Marder et al.; rif. [[27-mcglacken-2009|27]], [[28-ofial-2011|28]]): **arilazione diretta** e **accoppiamento ossidativo**. + +![[immagini/ab75adde10bed58f011b0e57bb27b271696d79594ff95462ce31eccc969448b1.jpg|560]] +*Figura 23 - reazioni di cross coupling catalizzate da Pd sui DPP* · [[fig-023|nota figura]] + +![[immagini/967a337ba86d6286aa8b01f0989b91a248a31a2a91baafc916325bc124f4bb46.jpg|560]] +*Figura 24 - sintesi generica di polimeri a base di DPP mediante reazioni di cross coupling* · [[fig-024|nota figura]] + +### Arilazione diretta (r.333-341) +- Accoppiamento di alogenuri arilici (spesso bromuri) con areni **senza pre-attivazione**, con catalizzatore al Pd e base: un CH del primo arene si condensa con l'unità C-Br del secondo, formando un legame arilico e HBr (neutralizzato dalla base). La regioselettività dipende da distribuzione di densità elettronica, acidità degli H, eteroatomi o altri gruppi funzionali (rif. [[27-mcglacken-2009|27]]). +- Marder e Chen (rif. [[29-liu-2013|29]]), due studi indipendenti: precursore **29** con diversi bromoareni ([[fig-025|Fig. 25]]). +- **Condizioni**: Pd(OAc)2 + acido pivalico, K2CO3 (neutralizza HBr), solvente **DMA** → prodotti **38 (a-h)**. Arilazione **selettiva in C5 dell'anello tiofenico**, nessun regioisomero identificato. +- Gryko et al.: efficace sia con bromoareni elettron-ricchi sia elettron-poveri, anche quando il bromuro è il DPP stesso (rese minori) ([[fig-026|Fig. 26]]). + +![[immagini/b60b2ed0441c7e89ab38e779618c5eee49a9df36d82e5122da708a9b7c78cbd2.jpg|560]] +*Figura 25 - reazione di arilazione diretta del DPP 29 con diversi bromoarili* · [[fig-025|nota figura]] + +![[immagini/5968c5669dcfd68fd60100a31f5074a12c690f0b4cc45063e8f2b25b4afd949d.jpg|560]] +*Figura 26 - arilazione dei DPP di-brorumati con diversi areni* · [[fig-026|nota figura]] + +### Arilazione ossidativa (r.347-361) +- Procede per attivazione dei legami C-H di entrambi i reagenti, senza pre-attivazione (rif. [[28-ofial-2011|28]]); il legame biarilico si forma per ossidazione di due C-H aromatici attivati dal Pd. Usato da Marder per il DPP **29**. +- Con polifluorurati poveri di elettroni, **Pd(OAc)2** e **Ag2CO3** (ossidante) → derivati coniugati **42 (a-c)** ([[fig-027|Fig. 27]]). +- Resa migliore **79%** per il composto **45a** (tetrafluoropiridina + DPP **29**). Reattività minore con pentafluorobenzene (**23%**) e tetrafluorobenzonitrile (**45%**). +- Criticità: l'uso massiccio di ossidanti come Ag2CO3. Alternativa più economica per polimeri coniugati con DPP affiancato da tiofeni (come **29**): polimerizzazione ossidativa con FeCl3 → [[polimerizzazione-ossidativa-fecl3]]. + +![[immagini/8344868ae6e8de1151d7f70a43a30b2c1557784a0e8b48edd4a99431390092bd.jpg|560]] +*Figura 27 - reazione di arilazione ossidativa* · [[fig-027|nota figura]] + +## 4. Litiazione in C5 (r.363) +I DPP **29**, **30**, **31** ([[fig-021|Fig. 21]]) reagiscono con **LDA** ([[fig-029|Fig. 29]]): +| Elettrofilo | Prodotto | Rif. | +|---|---|---| +| formammidi (N-formilpiperidina o DMF) | dialdeide **43** | [[30-hong-2012\|30]] | +| 2-isopropossi-4,4,5,5-tetrametil-1,3,2-diossaborolano | diestere boronico **44** | [[31-burckstummer-2011\|31]] | +| cloruro di trimetilstagno | stannano **45** | [[32-hu-2012\|32]] | +| I2 (quenching) | di-iodurato **46** (buone rese) | [[31-burckstummer-2011\|31]] | + +**44** e **45** sono utili per successivi cross-coupling. Nell'immagine di [[fig-029|Fig. 29]], **45** è il derivato SnMe3; controllare la numerazione (nota del catalogo). + +![[immagini/eed9eb52dc858b172c4f6739c7b9f352bfa0e7ab10e422129a877a929c4e45bf.jpg|560]] +*Figura 29 - reazione di litiazione e funzionalizzazione con successiva reazione con elettrofili* · [[fig-029|nota figura]] + +## 5. Sostituzione nucleofila aromatica, SNAr (r.369) +- Avviene senza catalizzatori al Pd, su DPP con buoni gruppi uscenti sugli anelli aromatici. Il core di-lattamico è elettron-attrattore. +- Numerosi esempi in letteratura in cui i composti **27** e **47** reagiscono con ammine secondarie, ad alta temperatura in autoclave, dando i sistemi amminici **48 (a-d)** ([[fig-030|Fig. 30]]). + +![[immagini/5efb58f7f7d27a0467d9f14cd5191b3aeb168710c69f6fb0a27ac0cb188b2eac.jpg|560]] +*Figura 30 - sostituzione aromatica classica su derivati di DPP* · [[fig-030|nota figura]] + +## Collegamenti +- [[dpp-struttura-e-proprieta]] · [[dpp-sintesi-letteratura]] · [[polimerizzazione-ossidativa-fecl3]] +- [[dpp-2]] (N-alchilazione applicata in tesi) +- [[tesi]] · [[bibliografia]] diff --git a/wiki/concepts/dpp-sintesi-letteratura.md b/wiki/concepts/dpp-sintesi-letteratura.md new file mode 100644 index 0000000..a8546aa --- /dev/null +++ b/wiki/concepts/dpp-sintesi-letteratura.md @@ -0,0 +1,123 @@ +--- +title: DPP - metodi di sintesi in letteratura +type: concept +tags: [dpp, sintesi, reformatskij, pseudo-stobbe, iqbal] +created: 2026-10-09 +updated: 2026-10-09 +tesi_loc: "§1.1.1 r.84-200; §4.1 r.742-754" +refs: [2, 5, 6, 7, 8, 9, 10, 11, 12, 13, 14, 15] +figures: ["fig-002", "fig-003", "fig-004", "fig-005", "fig-006", "fig-007", "fig-008", "fig-009", "fig-010", "fig-011", "fig-012", "fig-013", "fig-014"] +status: draft +--- + +# DPP - metodi di sintesi in letteratura + +Il §1.1.1 «Storia e sintesi» passa in rassegna le vie sintetiche al nucleo DPP. [[fig-014|Fig. 14]] è lo schema riassuntivo di tutti i metodi del capitolo. La via usata nel lavoro sperimentale (pseudo-Stobbe) è ripresa in [[dpp-1]]. + +> **Numerazione.** I numeri dei composti di questa pagina (1-13, 17, 19-21...) sono quelli del cap. 1 e **non** coincidono con i composti 1 e 2 della parte sperimentale. In questa pagina «DPP 3» è il DPP dal benzonitrile. + +## Indice dei metodi +| Metodo | Autori / anno | Reagenti chiave | Resa riportata | Figura | +|---|---|---|---|---| +| Reformatskij modificato (scoperta) | Farnum et al., 1974 [[02-shaikh-2022\|2]] | bromoacetato + benzonitrile + Zn | pigmento rosso 5-20% (sottoprodotto) | [[fig-002\|Fig. 2]] | +| Studi meccanicistici Reformatskij | Iqbal e Ciba-Geigy, 1988 [[05-iqbal-1988\|5]] | esperimenti di crossover | 25-30% rispetto al bromoacetato; 60% rispetto a nitrile e zinco | [[fig-003\|Fig. 3]], [[fig-004\|Fig. 4]], [[fig-005\|Fig. 5]] | +| Esteri succinici + nitrili aromatici | Iqbal et al. | diestere succinico, nitrile, alcolato | - | [[fig-006\|Fig. 6]], [[fig-007\|Fig. 7]], [[fig-008\|Fig. 8]] | +| Succindiammidi + N,N-dimetilbenzammide dietilacetale | Closs e Gompper, 1987 [[08-closs-1987\|8]] | succindiammide | ~60% globale | [[fig-009\|Fig. 9]] | +| Tetraidro-DPP + deidrogenazione | Iqbal; Sprake [[06-sprake-1976\|6]] | immina + estere succinico, poi DDQ | - | [[fig-010\|Fig. 10]], [[fig-011\|Fig. 11]] | +| Furo[3,4-c]furandioni | Langhals et al., 1996 [[13-langhals-1996\|13]] | intermedio furofurandionico (**17**) | - | [[fig-012\|Fig. 12]], [[fig-013\|Fig. 13]] | + +## Scoperta: Farnum et al., 1974 (r.86-92) +- DPP scoperti da Farnum et al. nel 1974, ottenuti come **sottoprodotti** della sintesi di derivati dell'azetinone con una reazione di Reformatskij modificata. +- Facendo reagire bromoacetato e benzonitrile in presenza di zinco non si ottiene il prodotto desiderato ma un **pigmento rosso con resa del 5-20%**. Schema ipotizzato in [[fig-002|Fig. 2]] (rif. [[02-shaikh-2022|2]]). +- Ipotesi: il benzonitrile reagisce con l'organozinco derivante dall'etilbromoacetato dando il **β-amminocinnamato (1)**; in condizioni ossidative genera il dimero (**2**), che per ciclizzazioni consecutive (attacco nucleofilo delle due ammine sul carbonile estereo, eliminazione di due molecole di alcol etilico) porta al DPP (**3**). + +![[immagini/12c29dc9e968dc2801ea23927ce3ef650e1a3ac5d429a00d260b0ad226cd3d96.jpg|560]] +*Figura 2 - meccanismo di formazione del DPP proposto da Farnum et al2* · [[fig-002|nota figura]] + +## Studi meccanicistici di Iqbal e Ciba-Geigy, 1988 (r.94-128) +- Obiettivo: rendere la produzione di DPP commercialmente sostenibile (rif. [[05-iqbal-1988|5]]). I tentativi basati sull'ipotesi di Farnum non avevano dato i risultati sperati. +- **Esperimento di crossover** ([[fig-003|Fig. 3]]): condizioni della reazione di Reformatskij tra 4-metilbenzonitrile (**A**), etil 2-bromoacetato (**B**) e quantità crescenti di β-amminocinnamato (**1**) sintetizzato a parte, per analizzare la distribuzione dei prodotti. + +![[immagini/0287775d86d0d7a03631bd068b0f3f7ddc40dac6d140a671cb82d95c6427370b.jpg|560]] +*Figura 3 - esperimento crossover in presenza di amminocinnamato* · [[fig-003|nota figura]] + +### Tabella 1 - esperimenti di crossover, risultati in rapporto molare (r.106-112) +| A | B | Zn | 1 | 5 | 4 | 3 | +| --- | --- | --- | --- | --- | --- | --- | +| 1 | 1 | 1 | 0 | 100 | - | - | +| 1 | 1 | 1 | 0,2 | 60 | 35 | ⁓5 | +| 1 | 1 | 1 | 1 | ⁓5 | 85 | 10 | + +L'aggiunta progressiva di amminocinnamato aumenta il prodotto **4**: conferma la formazione e partecipazione dell'intermedio **1** ed evidenzia la selettività verso il prodotto asimmetrico **4** (r.104). + +- **Dimerizzazione ossidativa**: né l'intermedio **1** né il suo sale di zinco dimerizzano per via termica o con acidi di Lewis, basi, aria o ossidanti. Facendo reagire il sale di zinco ([[fig-004|Fig. 4]]) con il bromuro B e il benzonitrile si isola il DPP **3** (r.114). + +![[immagini/72aff80c81e497a042a6b102de0ab896c676af9c8881a5a940fc187c201db4df.jpg|560]] +*Figura 4 - sale di zinco derivato dall'intermedio 3* · [[fig-004|nota figura]] + +- **Nuovo meccanismo** ([[fig-005|Fig. 5]], r.122): condensazione del reagente di Reformatskij con il benzonitrile → sale di Zn (**6**); C-alchilazione con una seconda molecola di bromoacetato → intermedi **7A** e **7B** in equilibrio tautomerico; reazione con il carbonile estereo e chiusura dell'anello lattamico a cinque termini → intermedio **8**; condensazione con un secondo benzonitrile e ciclizzazione dell'intermedio **9** (isolato e citato anche da Farnum) → DPP **3**. Questo penultimo passaggio spiega l'alta selettività per il prodotto asimmetrico **4** del crossover. + +![[immagini/0777b568504fb43b6ef573876dba6f5a272671791d8027d1bcaa42eaf7a9d0fe.jpg|560]] +*Figura 5 - meccanismo di formazione del DPP tramite la reazione di Reformtskij* · [[fig-005|nota figura]] + +- **Limiti** (r.128-130): procedura con rese riproducibili ma insufficienti per la fattibilità commerciale (25-30% rispetto al bromoacetato, 60% rispetto a nitrile e zinco). Criteri di scelta di vie alternative: disponibilità di materie prime, minimizzazione degli stadi, fattibilità tecnologica. +- Analisi del meccanismo ([[fig-005|Fig. 5]]): bassa resa complessiva del DPP **3** in contrasto con l'alta efficienza dei singoli passaggi: formazione del sale di zinco **6** con rese >80%; ciclizzazione di **9** pressoché quantitativa. Dedotto che la **C-alchilazione del sale di zinco 6** sia lo stadio determinante la resa, con probabili reazioni collaterali. Tale reazione forma il legame «**a**», elemento strutturale condiviso da entrambi gli anelli del sistema biciclico. Il gruppo ha quindi cercato un reagente che contenesse già il legame «a»: candidati, **esteri succinici** insieme a **nitrili aromatici**. + +## Esteri succinici + nitrili aromatici (Iqbal et al.) (r.130-158) +- **Retrosintesi** ([[fig-006|Fig. 6]]): tre frammenti (X, Y, X) simmetrici; preserva il legame C-C centrale «a»; reagenti commerciali. +- **Reazione** ([[fig-007|Fig. 7]]): supera la criticità della formazione del legame C-C centrale perché il legame preesiste nell'estere succinico. Non era riportata in letteratura; analogie con la condensazione di Stobbe tra un'aldeide (o base di Schiff) ed esteri succinici, che porta al sistema ottaidropirrolopirrolo (rif. [[06-sprake-1976|6]]). + +![[immagini/817f7a716828f78218ddabd380b9fcad36a14ce9094fed0e9c6db973b0311197.jpg|560]] +*Figura 6 - analisi retrosintetica del DPP proposta da Iqbal et al.* · [[fig-006|nota figura]] + +![[immagini/cf12dd5b5015150d07e4e39c793edc69b197be98844c93bb294624f24b3a24fc.jpg|560]] +*Figura 7 - sintesi del DPP proposta da Iqbal et al.* · [[fig-007|nota figura]] + +- **Base**: serve elevata forza basica con ridotta reattività nucleofila (un alcolato): favorisce la deprotonazione dell'estere succinico e minimizza reazioni indesiderate (attacco nucleofilo al nitrile, condensazione di Claisen). +- **Aggiunta graduale** dell'estere succinico: bassa concentrazione locale, inibisce la ciclizzazione competitiva ([[fig-008|Fig. 8]]). +- **Eccesso di base**: necessario perché il DPP, relativamente acido, sottrae base al sistema (rif. [[05-iqbal-1988|5]], [[07-grzybowski-2015|7]]). +- **Residuo R del diestere**: l'aumento dell'ingombro sterico inibisce la reazione parassita di autocondensazione; resa e selettività migliorano nell'ordine **t-Am > t-Bu > i-Pr > Et > Me**. Gruppi voluminosi (*terz*-amile, *terz*-butile) ottimizzano il prodotto principale rispetto a metile o etile. +- Esito: ottimizzazione dei parametri e selezione dei precursori superano le basse rese precedenti; fattibilità su scala industriale con buon equilibrio tra efficienza sintetica (atom economy) e sostenibilità economica. + +![[immagini/527a3cd0e4d0468cd19b0a75b855eb4903fcb344ef3efab2714fe7265004a236.jpg|560]] +*Figura 8 - reazione competitiva di ciclizzazione dell'estere succinico* · [[fig-008|nota figura]] + +## Closs e Gompper, 1987 (r.160-166) +- Sintesi da **succindiammidi** e **N,N-dimetilbenzammide dietilacetale** ([[fig-009|Fig. 9]], rif. [[08-closs-1987|8]]). +- Ottimizzazione: efficienza globale di circa **60%**. Scaldando i reagenti si ottiene il DPP **3** in quota minoritaria (**30%**); dalla fase liquida residua si recupera l'intermedio **10** (succinilbenzimmidina) con abbondanza del **35%**. Aggiunta di potassio ter-butossido in THF → conversione quantitativa nell'analogo DPP, raddoppiando le rese finali. + +![[immagini/d930a8d7b48446faf3acb4839a5330e3cf9dbf19e1ba59b5cdac9da94addf461.jpg|560]] +*Figura 9 - sintesi del DPP3 proposta da Closs e Gompper* · [[fig-009|nota figura]] + +## Via dei tetraidro-DPP e deidrogenazione con DDQ (r.168-180) +- Variante descritta anche da Iqbal (rif. [[05-iqbal-1988|5]]): passaggio attraverso i **tetraidrodichetopirrolopirroli**, deidrogenati per generare il nucleo DPP. Reagente di solito: **DDQ** (2,3-dicloro-5,6-dicianobenzochinone) ([[fig-010|Fig. 10]]). +- **Sprake** (rif. [[06-sprake-1976|6]]): condensazione di un'immina (**11**) con un estere succinico; l'intermedio **12** viene convertito nel DPP **13** con DDQ ([[fig-011|Fig. 11]]). +- Ottimizzazione dei passaggi finali: contributi di Stas [[09-stas-2010|9]], Avcibasi [[10-avcbasi-2004|10]], Riggs [[11-riggs-2005|11]], Qian [[12-qian-2012|12]]. + +![[immagini/8c6bb2792de10aac72c41042ed82f8d74646772be1a73ef09237e408b5666b0f.jpg|560]] +*Figura 10 - DDQ (2,3-dicloro-5,6-dicianobenzochinone)* · [[fig-010|nota figura]] + +![[immagini/f4ba478941a0c0eb6302ebfee66f43039e2c9e06c55022c8b2e84bbd89d49dda.jpg|560]] +*Figura 11 - esempio di sintesi proposta da Sprake et al.6* · [[fig-011|nota figura]] + +## Langhals et al., 1996 (r.182-194) +- Generazione dei DPP dalla reattività dei composti basati sul nucleo del **furo[3,4-c]furandione** (rif. [[13-langhals-1996|13]]). +- L'intermedio furofurandionico (**17**) si ottiene per via termica in toluene (rif. [[14-de-luca-2001|14]]), oppure da specifici benzoilacetati con accoppiamento radicalico/ossidativo mediato da miscele iodio/sodio e successiva chiusura termica dell'anello (rif. [[15-harris-1998|15]]) ([[fig-012|Fig. 12]]). +- Il metodo ([[fig-013|Fig. 13]]) serve per composti N-arilati simmetrici (**20**), asimmetrici (**19**) e con catene alchiliche (**21**). + +![[immagini/88b885a66e23030d331ef30dc6888e32056f3bf1b70dee168799f897a6e6e66f.jpg|560]] +*Figura 12 - metodi di sintesi per ottenere il nucleo furo[3,4-c]furandione* · [[fig-012|nota figura]] + +![[immagini/92ca1a28a7507b12e73b2e34eb1b92e6ed2b1d241fa8fc2ccfe589b6793c3012.jpg|560]] +*Figura 13 - sintesi dei N-aril-DPP proposta da Langhals et al.* · [[fig-013|nota figura]] + +## Schema riassuntivo +![[immagini/d3804894a7e99bbf5bba8abce2680291b0b6dc0c435b453fa6beb143231ce6f9.jpg|560]] +*Figura 14 - schema riassuntivo dei metodi sintetici analizzati per ottenere un dichetopirrolopirrolo* · [[fig-014|nota figura]] + +## Sintesi del DPP tiofenico usata in tesi +Il DPP della parte sperimentale è ottenuto con la via esteri succinici + nitrili (pseudo-Stobbe) a partire da 2-cianotiofene e diisopropil succinato; il motivo della scelta dell'estere isopropilico (ingombro, r.748) è coerente con la serie t-Am > t-Bu > i-Pr > Et > Me vista sopra _(inferenza)_. Dettagli e meccanismo in [[dpp-1]]. + +## Collegamenti +- [[dpp-struttura-e-proprieta]] · [[dpp-reattivita]] · [[dpp-1]] +- [[tesi]] · [[bibliografia]] diff --git a/wiki/concepts/dpp-struttura-e-proprieta.md b/wiki/concepts/dpp-struttura-e-proprieta.md new file mode 100644 index 0000000..6d54294 --- /dev/null +++ b/wiki/concepts/dpp-struttura-e-proprieta.md @@ -0,0 +1,84 @@ +--- +title: DPP - struttura e proprietà +type: concept +tags: [dpp, struttura, proprietà-ottiche, impaccamento] +created: 2026-10-09 +updated: 2026-10-09 +tesi_loc: "§1.1 r.69-81; §1.1.2 r.203-245; §4.1 r.722-732" +refs: [1, 2, 3, 4, 16, 17, 18, 19, 20] +figures: ["fig-001", "fig-015", "fig-016", "fig-040"] +status: draft +--- + +# DPP - struttura e proprietà + +Sigla DPP = dichetopirrolopirrolo. Per i metodi di sintesi in letteratura vedi [[dpp-sintesi-letteratura]], per le reazioni [[dpp-reattivita]]. I DPP della parte sperimentale sono [[dpp-1]] e [[dpp-2]]. Attenzione: la numerazione dei composti nel cap. 1 è diversa da quella del cap. 3-4 (vedi [[difetti-noti]]). + +## Struttura generale +- Nucleo centrale di **due anelli lattamici a cinque termini condensati**; il sistema biciclico ha due insaturazioni che permettono di introdurre sostituenti aromatici o eteroaromatici periferici (§1.1, r.71, [[fig-001|Fig. 1]]). +- Nel DPP non sostituito il core è a **otto elettroni π, perfettamente planare** (§1.1.2, r.205). + +![[immagini/455dd3d0c7bf0fe6ac581ee70795075c998d4dc7156eaa77a4576774f6fd8050.jpg|560]] +*Figura 1 - struttura generica di un dichetopirrolopirrolo* · [[fig-001|nota figura]] + +## Storia come pigmento +- Caratteristiche fisiche: punto di fusione molto elevato (>350 °C), fortissima insolubilità, colorazione rossa; rimasero inosservate finché i ricercatori della Ciba-Geigy Specialty Chemicals Co. non svilupparono i primi derivati, ispirandosi ad analogie strutturali con altri pigmenti noti (r.77, rif. [[01-bao-2020|1]]). +- Dal 1986, anno in cui il primo DPP fu immesso sul mercato, sono stati sintetizzati altri coloranti della famiglia, usati nella tintura di plastiche, fibre e inchiostri (r.79). +- Da pigmenti industriali sono diventate molecole indagate in svariati settori: unità planare π-coniugata e sostituenti ammidici reattivi permettono di modulare le proprietà ottiche ed elettroniche; impieghi in optoelettronica, fotovoltaico [[02-shaikh-2022|2]] e bio-imaging [[03-auwalu-2021|3]], [[04-zhang-2024|4]] (r.81). Applicazioni: [[optoelettronica-oled-donatore-accettore]]. + +## Interazioni intermolecolari e stabilità (§1.1.2, r.205) +- Fitto network di interazioni intermolecolari. +- **Legami a idrogeno (0,182 nm)** [[16-mizuguchi-1992|16]]: aggregati stabili, solubilità drasticamente limitata nei solventi organici convenzionali. +- **Estesa coniugazione e vicinanza dei piani molecolari (0,334 nm)** [[16-mizuguchi-1992|16]]: ottimale sovrapposizione degli orbitali, intense interazioni di π-π stacking [[17-david-2011|17]]. +- Risultato: grande stabilità termica, punto di fusione superiore a 350 °C, temperatura di degradazione oltre 500 °C. +- Il π-stacking è la causa strutturale dell'[[acq-e-stato-solido]]. + +## Proprietà ottiche e stato di aggregazione (r.207) +- Confronto soluzione/stato solido: nel solido, **allargamento della banda di assorbimento e marcato effetto batocromico, picco spostato di circa 30 nm** ([[fig-015|Fig. 15]], rif. [[18-mizuguchi-1991|18]]). +- [[fig-015|Fig. 15]] riporta lo spettro di assorbimento del DPP non sostituito in film con spessore di 1200 Å (linea tratteggiata) e in DMSO (linea continua). + +![[immagini/0fcb29bca38442ebe113d2d1621fed515e47c21e4535d7737fad11648e42fb62.jpg|560]] +*Figura 15 - spettro di assorbimento del DPP non sostituito in film con spessore di 1200 Å (linea tratteggiata)* · [[fig-015|nota figura]] + +## Modulazione con i sostituenti (r.215-217) +- Gruppi di natura elettronica diversa (presenza simultanea di elettron-donatori ed elettron-attrattori) promuovono un marcato effetto batocromico, aumento dell'intensità di assorbimento e allargamento della differenza tra picchi di assorbimento ed emissione (Stokes shift) (rif. [[19-lunak-2009|19]]). Per lo Stokes shift vedi [[fluorescenza]]. + +### Tabella 2 - proprietà foto-fisiche di DPP con diversi sostituenti, in soluzione e allo stato solido (rif. [[20-lenz-2002|20]]; r.219-231) + +| R | Colorea | λabsmax (nm) Soluzioneb | λabsmax (nm) Solidoc | εmaxd (M-1 cm-1) | +| --- | --- | --- | --- | --- | +| 3-CF3 | Giallo-arancio | 509 | 518 | 21000 | +| 3-Cl | Arancione | 512 | 528 | 27000 | +| H | Giallo-rosso | 504 | 538 | 33000 | +| 4-Br | Blu-rosso | 515 | 555 | 35000 | +| 4-NMe2 | Viola-blu | 554 | 603 | 81500 | + +a soluzione in NMP, b soluzione in DMSO, c ottenuto mediante misure di riflettanza su un film di PVC pigmentato, d in DMSO + +### Lettura dei dati nella tesi (r.233-245) +- **Origine del batocromico solido** (rif. [[20-lenz-2002|20]]): l'idrogeno ammidico interagisce con il doppietto dell'ossigeno carbonilico di una molecola adiacente; la densità elettronica si sposta sull'azoto, formando allo stato solido una parziale carica negativa che influenza la struttura elettronica con variazione delle lunghezze d'onda di assorbimento e dei massimi. +- Le proprietà ottiche dipendono strettamente dai sostituenti aromatici, con generale effetto batocromico dello spettro di emissione in soluzione rispetto al DPP con gruppi aromatici non sostituiti. _(Nel testo la frase che segue - «Rispetto alla molecola di base ... qualsiasi modifica strutturale si traduce, in Il comportamento allo stato solido ...» - è troncata: vedi [[difetti-noti]].)_ +- **Stato solido, effetto sterico**: dipende fortemente dalla *posizione* dei sostituenti, con effetti prettamente sterici. L'ingombro modifica l'angolo di torsione dei gruppi aromatici rispetto al core. Posizione *para*: minimizza l'ingombro e mantiene lo spostamento verso lunghezze d'onda maggiori. Posizione *meta*: aumenta l'angolo di torsione, riduce la coniugazione effettiva e induce uno shift ipsocromico. Il testo precisa che serve distinguere il contributo strutturale da quello elettronico, anche se la posizione sull'anello influenza anche quest'ultimo. +- **Effetti elettronici**: gruppi moderatamente elettron-attrattori danno cambiamenti spettrali limitati (picchi in 504-515 nm); un gruppo fortemente elettron-donatore (4-NMe₂) sposta il massimo di circa 50 nm. Causa: architettura elettronica donatore-accettore-donatore (*push-pull-push*), con core DPP intrinsecamente elettron-povero. +- **Geometria** (Lenz, rif. [[20-lenz-2002|20]]): i gruppi fenilici sono torti di appena **7°** rispetto al piano del nucleo, nonostante la notevole repulsione sterica tra i protoni *orto* dell'anello benzenico e gli eteroatomi (ossigeno e gruppi amminici) dell'anello lattamico. La planarità è conservata da una delocalizzazione π che unisce le unità benzeniche allo scheletro centrale. Prova: il legame di giunzione fenile-nucleo misura **1,46 Å**, più corto di un legame singolo canonico (atteso 1,50-1,54 Å), con carattere di parziale doppio legame. +- Conclusione del paragrafo: la sensibilità dello spettro ai sostituenti deriva dall'elevata coniugazione; ogni variazione elettronica sugli anelli periferici si traduce in una ridistribuzione di carica sull'intero scheletro. + +![[immagini/423e5b40dafcfcf5a959f73e6d8eed74b1f01972cef60482333c2a59f3292753.jpg|560]] +*Figura 16 - struttura cristallina del DPP3 (distanze in Å)16* · [[fig-016|nota figura]] + +## Rigidità e fluorescenza +I DPP rientrano tra le strutture con pochi gradi di libertà (sistemi coniugati e aromatici): lo scheletro planare e il vasto sistema di elettroni delocalizzati limitano il rilassamento vibrazionale (§1.2, r.413, rif. [[34-lakowicz-1999|34]]). Dettagli in [[fluorescenza]]. + +## Lavoro precedente del gruppo di ricerca (§4.1, r.724-732) +- Il gruppo aveva già studiato fluorofori DPP e l'effetto di gruppi elettron-attrattori (EWG) ed elettron-donatori (EDG) in posizione *para* sull'anello benzonitrilico usato nella formazione dei DPP ([[fig-040|Fig. 40]]). +- **EWG in para** → sistemi **altamente emissivi**. +- **EDG** → formazione di un **isomero strutturale (iso-DPP)** con fluorescenza nel visibile inibita, principalmente per attivazione di processi di rilassamento non radiativo. +- Lo studio ha dato le basi per scegliere i fluorofori per le polimerizzazioni, in base a proprietà emissive e reattività. Il lavoro di tesi sostituisce i tradizionali anelli benzenici con anelli tiofenici ([[dpp-1]]) e N-alchila i gruppi ammidici ([[dpp-2]]), con aumento di solubilità, procedura semplice e scalabile (r.734). + +![[immagini/b6398852c7419861eb44da7657cb2af96b59c5953a54007fb0df70f12a4c2cf9.jpg|560]] +*Figura 40 - sostituenti del DPP precedentemente studiati dal gruppo di ricerca* · [[fig-040|nota figura]] + +## Collegamenti +- [[dpp-sintesi-letteratura]] · [[dpp-reattivita]] · [[fluorescenza]] · [[acq-e-stato-solido]] +- [[dpp-1]] · [[dpp-2]] +- [[tesi]] · [[bibliografia]] diff --git a/wiki/concepts/fluorescenza.md b/wiki/concepts/fluorescenza.md new file mode 100644 index 0000000..2fd90b2 --- /dev/null +++ b/wiki/concepts/fluorescenza.md @@ -0,0 +1,102 @@ +--- +title: Fluorescenza - fondamenti +type: concept +tags: [fluorescenza, jablonski, stokes-shift, resa-quantica, tempo-di-vita] +created: 2026-10-09 +updated: 2026-10-09 +tesi_loc: "§1.2 r.376-476" +refs: [33, 34, 35, 36, 37, 38, 39] +figures: ["fig-031", "fig-032", "fig-033", "fig-034"] +status: draft +--- + +# Fluorescenza - fondamenti + +Cap. 1.2 della tesi. La fluorescenza è il fenomeno fisico corrispondente all'emissione di fotoni da parte di una sostanza, in seguito al rilassamento da uno stato elettronico eccitato a uno fondamentale (r.378). Applicazioni ai materiali sintetizzati: [[uv-vis-fluorescenza]]; effetto dell'aggregazione: [[acq-e-stato-solido]]. + +## Fluorescenza e fosforescenza (r.380-386) +- Il termine «fluorescenza» è dovuto a G. G. Stokes (metà XIX secolo). Per molto tempo la distinzione si basò solo sulla durata dell'emissione dopo l'eccitazione (fluorescenza che svanisce con la sorgente; fosforescenza che persiste). Criterio insufficiente: esistono fluorescenze a vita lunga (sali di europio bivalente) e fosforescenze a vita breve (luminescenza violetta del solfuro di zinco) con durate comparabili, dell'ordine delle centinaia di nanosecondi (rif. [[33-valeur-2011|33]]). +- Ciò che distingue i due fenomeni è la **natura dello stato eccitato**: + - **Fluorescenza** (stati eccitati di **singoletto**): l'elettrone promosso mantiene spin opposto (accoppiato) a quello rimasto nell'orbitale fondamentale; il rilassamento radiativo è permesso dalle regole di selezione dello spin, rapido, con emissione di un fotone a energia minore (lunghezze d'onda maggiori) della radiazione incidente. Tempo di vita medio dell'ordine delle decine di nanosecondi (10-9 s). + - **Fosforescenza** (stati di **tripletto**): stesso orientamento di spin; le transizioni radiative verso lo stato fondamentale (di singoletto) sono proibite dalle regole di selezione; tempi di vita da pochi millisecondi a diversi secondi (rif. [[34-lakowicz-1999|34]]). + +## Diagramma di Jablonski ([[fig-031|Fig. 31]], r.388-398) +Punto di partenza per qualunque trattazione teorica su assorbimento e luminescenza molecolare. Frecce continue = fenomeni che coinvolgono l'interazione con radiazione elettromagnetica; linee tratteggiate = rilassamenti molecolari senza interazione con la luce. + +- **Assorbimento**: coinvolge molecole nel livello vibrazionale fondamentale. L'ampio divario tra S0 e S1 impedisce la promozione termica: per indurre fluorescenza serve eccitazione luminosa. +- Dopo l'assorbimento il fluoroforo passa a un livello vibrazionale superiore di S1 o S2. In fase condensata (liquida o solida) segue un rilassamento non radiativo molto rapido fino al livello vibrazionale fondamentale di S1: la **conversione interna**, dell'ordine dei picosecondi (10-12 s), prima del decadimento emissivo. +- Perciò l'emissione parte quasi sempre dal livello vibrazionale a minore energia di S1: **regola di Kasha** (rif. [[35-kasha-1950|35]]). +- **Intersystem crossing (ISC)** ([[fig-032|Fig. 32]]): da S1 a T1 per inversione di spin; T1 non è raggiungibile direttamente; processo non radiativo. Da T1 la molecola torna allo stato fondamentale per conversione interna o per fosforescenza. + +![[immagini/a80b21103343058ce23aafb36ef90f8aa7f49d4ef4055f8e520fdb80d185a8b1.jpg|560]] +*Figura 31 - diagramma di Jablonski* · [[fig-031|nota figura]] + +![[immagini/2eb69c597f77449d9e46674c97478393268b91f0b3d19d8fb04ba6b6e22f2610.jpg|560]] +*Figura 32 - schema rappresentativo del fenomeno di intersystem crossing* · [[fig-032|nota figura]] + +## Rigidità strutturale ([[fig-033|Fig. 33]], r.406-413) +- L'efficienza dell'emissione dipende dalla struttura del fluoroforo: serve elevata **rigidità** per evitare rilassamenti non radiativi. +- Nelle molecole poco flessibili la geometria dello stato fondamentale e di quello eccitato non presentano distorsioni significative: si riduce la probabilità di dissipare energia come calore per moti vibrazionali; l'energia è rilasciata quasi interamente come luce. +- Strutture ideali: pochi gradi di libertà, cioè sistemi coniugati e aromatici. I DPP rientrano in questa categoria: scheletro planare e vasto sistema di elettroni delocalizzati limitano il rilassamento vibrazionale (rif. [[34-lakowicz-1999|34]]) → [[dpp-struttura-e-proprieta]]. + +![[immagini/ba021605d4b365536a686cb2f71f1c58ea2d5f5b9f962692d596f7a5a3d05ac7.jpg|560]] +![[immagini/8047b55e3609435acd325d3602705c73a5308dc9b407322726ea6a1dde74af65.jpg|560]] +*Figura 33 - stati elettronici per molecole rigide e flessibili* · [[fig-033|nota figura]] + +Parametri che caratterizzano la fluorescenza: **shift di Stokes, tempi di vita, resa quantica** (r.415). + +## Shift di Stokes (§1.2.1, r.418-426) +- Differenza tra la lunghezza d'onda della luce assorbita e quella emessa (fluorescenza o fosforescenza) ([[fig-034|Fig. 34]]; rif. [[36-stokes-1852|36]]; figura da [[37-prodi-2011|37]]). +- La minore energia dell'emissione deriva da una dissipazione energetica per decadimenti di natura tipicamente vibrazionale. +- Quantificata come distanza in lunghezza d'onda tra i massimi degli spettri di assorbimento e di fluorescenza; parametro distintivo per ciascun fluoroforo. +- Nella tesi lo Stokes shift misurato è sempre dato in nm, come differenza λmax,em − λmax,abs: tabelle in [[dpp-2]] (Tab. 5), [[copolimeri-3a-3b-3c]] (Tab. 7), [[bottle-brush-3-x]] (Tab. 10). _(inferenza: definizione operativa ricavata dai valori delle tabelle)_ + +![[immagini/0cb83724455d9b75cb980a077787323e0a434fb78192dc220e13069923f37fa6.jpg|560]] +*Figura 34 - shift di Stokes37* · [[fig-034|nota figura]] + +## Resa quantica (§1.2.2, r.429-447) +Efficienza del processo radiativo, ϕ: frazione tra i quanti di luce riemessi e quelli assorbiti. + +$$ +\phi =\frac{n\circ fotoni emessi}{n\circ fotoni assorbiti} +$$ +**Equazione 1** - *resa quantica a livello macroscopico* + +Dal punto di vista cinetico: competizione tra rilassamento emissivo (Kf) e somma delle costanti non radiative (Knr), come intersystem crossing o conversione interna. + +$$ +\phi =\frac{K_{f}}{K_{f}+\sum_{}^{}K_{nr}} +$$ +**Equazione 2** - *resa quantica in cinetica fotofisica* + +- ϕ è legata alla topologia elettronica e all'architettura molecolare. Transizioni ad alta energia come **σ → σ\*** inducono prevalentemente fotodissociazione del legame e spengono l'emissione; **n → π\*** e, in misura maggiore, **π → π\*** garantiscono le migliori efficienze radiative. +- Strutture rigide, ricche di insaturazioni, anelli aromatici e funzionalità carboniliche massimizzano la probabilità di emissione (rif. [[34-lakowicz-1999|34]]). Un'eccessiva flessibilità conformazionale favorisce la dissipazione termica tramite moti vibrazionali (conversione interna) e abbatte la resa (rif. [[38-brouwer-2011|38]], [[39-weber-1957|39]]). + +## Tempi di vita (§1.2.3, r.450-476) +- Tempo medio che la molecola trascorre nello stato eccitato prima di tornare al fondamentale; in generale la fluorescenza avviene in tempi dell'ordine delle decine di nanosecondi. + +$$ +\tau =\frac{1}{K_{f}+\sum_{}^{}K_{nr}} +$$ +**Equazione 3** - *tempo di vita medio* + +- L'emissione è un processo casuale: solo poche molecole emettono esattamente a t = τ; τ è un valore medio. +- Il tempo di vita in assenza di processi non radiativi è il **tempo di vita intrinseco (naturale)**: + +$$ +\tau _{n}=\frac{1}{K_{f}} +$$ +**Equazione 4** - *tempo di vita intrinseco* + +- Si può calcolare dal tempo di vita medio e dalla resa quantica: + +$$ +\tau _{n}=\frac{\tau }{Q} +$$ +**Equazione 5** - *correlazione tra tempo di vita intrinseco e resa quantica* + +- Tempo di vita e resa quantica dipendono dalle costanti di decadimento radiativo (Γ) e non radiativo (Knr). Esempi: gli **scintillatori** hanno rese elevate e tempi di vita brevi (⁓1 ns) per alti valori di Γ; i composti con Knr elevata hanno fluorescenza debole, ad esempio i composti aromatici con gruppi -NO2 (rif. [[34-lakowicz-1999|34]]). + +## Collegamenti +- [[dpp-struttura-e-proprieta]] · [[uv-vis-fluorescenza]] · [[acq-e-stato-solido]] · [[fluorofori-in-polimeri]] +- [[tesi]] · [[bibliografia]] diff --git a/wiki/concepts/fluorofori-in-polimeri.md b/wiki/concepts/fluorofori-in-polimeri.md new file mode 100644 index 0000000..b583878 --- /dev/null +++ b/wiki/concepts/fluorofori-in-polimeri.md @@ -0,0 +1,51 @@ +--- +title: Fluorofori in materiali polimerici +type: concept +tags: [fluorofori, architetture, host-guest, main-chain, side-chain, cross-linked, grafting-from] +created: 2026-10-09 +updated: 2026-10-09 +tesi_loc: "§1.3 r.479-499" +refs: [40, 41, 42, 43] +figures: ["fig-035"] +status: draft +--- + +# Fluorofori in materiali polimerici + +L'inserimento di un fluoroforo in un sistema macromolecolare richiede un accurato design molecolare: l'architettura scelta influenza drasticamente le proprietà finali (r.481). Classificazione dei sistemi polimero-fluoroforo ([[fig-035|Fig. 35]]): **host-guest, main-chain, side-chain, cross-linked**. + +![[immagini/84a75adb472bc4fd46a5f6d27b0f8d6a3f709b8d073d033aeddaba16c2173b7e.png|560]] +*Figura 35 - sistemi polimerici con inserimento di fluorofori, in verde il polimero e in rosso le unità di fluoroforo* · [[fig-035|nota figura]] + +| Tipo | Legame fluoroforo-polimero | Vantaggi | Limiti | Rif. | +|---|---|---|---|---| +| a. host-guest | nessuno (miscela fisica) | versatilità (molti additivi), facilità di preparazione, niente vie sintetiche complesse | scarsa stabilità a lungo termine: migrazione e aggregazione, segregazione di fase, calo della resa quantica | [[40-stoddart-1988\|40]], [[41-valdes-1996\|41]] | +| b. main-chain | parte integrante della catena principale | - | sintesi complessa; controllo di stechiometria e rapporti di reattività | [[42-wang-2015\|42]] | +| c. side-chain | catena laterale | solubilità, tuning del colore e del trasporto di carica | - | [[43-lee-2000\|43]] | +| d. cross-linked | ponti chimici tra macromolecole | cromofori ancorati, niente aggregazione | rigidità: fragile, insolubile, difficile da lavorare | - | + +## a. Host-guest (r.489-493) +- Il fluoroforo (guest) non forma legami covalenti con il polimero (host): è mescolato e disperso fisicamente. Approccio più semplice e immediato; notevole versatilità (diversi additivi) e facilità di preparazione. +- Difetto principale: scarsa stabilità a lungo termine. All'aumentare della concentrazione il guest si comporta come un additivo a basso peso molecolare, migra verso la superficie e si aggrega; segregazione di fase e disomogeneità strutturale portano alla perdita delle proprietà ottiche (diminuzione della resa quantica). +- Stabilizzazione: sinergia fra interazioni secondarie (legami a idrogeno, dipolo-dipolo) con il polimero e uso di host con elevata cristallinità e alta Tg, che immobilizzano il guest riducendo la mobilità macromolecolare (rif. [[40-stoddart-1988|40]], [[41-valdes-1996|41]]). + +## b. Main-chain (r.495) +- Il cromoforo è legato chimicamente come parte integrante della catena principale. Sintesi più complessa: monomeri fluorescenti bifunzionalizzati, controllo rigoroso della stechiometria e dei rapporti di reattività, per evitare un'eccessiva vicinanza dei cromofori (spegnimento della fluorescenza). +- Strategia di successo: **«grafting from»**, esplorata da Wang et al. (rif. [[42-wang-2015|42]]). Un derivato DPP bifunzionalizzato con gruppi idrossilici (**DPP-OH**) come iniziatore fa crescere simmetricamente due catene di policaprolattone (PCL) per ROP, ottenendo un copolimero **PCL-DPP-PCL**. Meccanismo ROP: [[rop-pcl]]. + +## c. Side-chain (r.497) +- Unità luminescenti connesse come catene laterali alla catena principale. Per ridurre l'ingombro sterico e favorire la mobilità locale si inserisce spesso uno **spaziatore flessibile** tra core polimerico e fluoroforo: abbassa la Tg e limita le interazioni tra cromofori adiacenti. +- Sintesi: per polimerizzazione diretta (copolimerizzando un monomero funzionalizzato con altri comonomeri, per «diluire» il fluoroforo e dare processabilità) oppure per post-polimerizzazione (ancorando il colorante a un polimero preformato). +- Esempio: Lee et al. (rif. [[43-lee-2000|43]]), copolimeri radicalici con catena principale di PMMA e cromofori laterali a base di carbazolo e fenilenvinilene. Esito: eccellente solubilità nei comuni solventi organici senza formazione di gel, tuning fine del colore dell'emissione e delle proprietà di trasporto di carica. + +## d. Cross-linked (r.499) +- Rimedio alla mobilità delle catene polimeriche, che nel tempo può avvicinare i cromofori e spegnere la fluorescenza. I fluorofori sono unità multifunzionali che creano ponti chimici tra le macromolecole. +- Pro: ancoraggio permanente dei cromofori nella loro posizione spaziale, che previene l'aggregazione. +- Contro: l'eccessiva rigidità del reticolo → modulo elastico maggiore ma materiali più fragili, insolubili e di difficile lavorabilità. + +## Rapporto con il lavoro di tesi +La tesi segue una strategia diversa da quelle elencate: il fluoroforo DPP è nello scheletro (main-chain, con 3HT) e porta catene laterali di PCL innestate con grafting-from ([[bottle-brush]]). Il passaggio è motivato dal quenching dei film lineari ([[acq-e-stato-solido]]). _(inferenza: collocazione della tesi nella classificazione; la tesi non la dichiara nel §1.3)_ + +## Collegamenti +- [[fluorescenza]] · [[rop-pcl]] · [[bottle-brush]] · [[acq-e-stato-solido]] +- [[tesi]] · [[bibliografia]] diff --git a/wiki/concepts/optoelettronica-oled-donatore-accettore.md b/wiki/concepts/optoelettronica-oled-donatore-accettore.md new file mode 100644 index 0000000..497fdf6 --- /dev/null +++ b/wiki/concepts/optoelettronica-oled-donatore-accettore.md @@ -0,0 +1,62 @@ +--- +title: Optoelettronica organica, OLED e design donatore-accettore +type: concept +tags: [optoelettronica, oled, donatore-accettore, band-gap, 3ht, hopping] +created: 2026-10-09 +updated: 2026-10-09 +tesi_loc: "§1.4 r.502-542; §2 r.547-559" +refs: [44, 45, 46, 47, 48, 49] +figures: ["fig-036", "fig-037", "fig-038"] +status: draft +--- + +# Optoelettronica organica, OLED e design donatore-accettore + +Cap. 1.4 «Applicazioni». Sul perché serve evitare l'ACQ in questi dispositivi: [[acq-e-stato-solido]]. + +## Dai pigmenti ai semiconduttori (r.504-506) +- I derivati del DPP hanno superato l'impiego come pigmenti commerciali: transistor organici a effetto di campo (**OFET**), fotovoltaico, sonde fluorescenti per bioimaging. +- Rilevanza cruciale nell'**optoelettronica organica**: elevata stabilità termica e fotochimica, nucleo fortemente elettron-deficiente → elemento chiave per semiconduttori innovativi e dispositivi a emissione di luce (rif. [[44-bao-2020|44]]). + +## Optoelettronica (r.508-516) +- Studio e sviluppo di dispositivi basati sull'interazione tra radiazione elettromagnetica e semiconduttori: conversione di segnali elettrici in fotoni (**OLED**) o viceversa (celle fotovoltaiche **OSC**, fotorivelatori) ([[fig-036|Fig. 36]]). +- Storicamente dominata da **semiconduttori inorganici rigidi** con reticoli cristallini ordinati, come il silicio (rif. [[45-ostroverkhova-2016|45]]). +- L'optoelettronica organica usa piccole molecole e polimeri con estesi sistemi π-coniugati. Vantaggi: leggerezza, flessibilità meccanica (dispositivi deformabili/pieghevoli, display di nuova generazione, elettronica indossabile; rif. [[46-nowsherwan-2024|46]]); **processabilità**: i polimeri coniugati si depositano da soluzione a basse temperature con tecniche ad alta resa e basso costo (**spin-coating**, stampa su larga scala), con riduzione dei costi rispetto ai processi ad alta temperatura o in alto vuoto dell'inorganico, minore impatto ambientale, elettronica scalabile e sostenibile. + +![[immagini/84f29f22fa09304be18bab32ebed95a16f6ad53a8e0c3082c91550f724deaebc.jpg|560]] +*Figura 36 - rappresentazione schematica dei principi fisici alla base dei materiali optoelettronici: generazione di portatori di carica per assorbimento (sinistra) e ricombinazione radiativa per emissione (destra)* · [[fig-036|nota figura]] + +## Ingegneria del band gap e approccio D-A (r.518) +- Per usare materiali polimerici processabili in dispositivi serve governare le proprietà ottiche ed elettroniche, cioè **ingegnerizzare il band gap** (rif. [[47-li-2014|47]]). +- Strategia d'elezione: approccio **donatore-accettore (D-A)** (rif. [[48-kroon-2008|48]]): copolimerizzazione alternata di unità fortemente elettron-deficienti (accettori) e unità elettron-ricche (donatori) lungo lo scheletro π-coniugato. +- Ibridazione degli orbitali di frontiera: **HOMO** determinato principalmente dalla porzione elettron-donatrice; **LUMO** governato dall'unità elettron-accettrice. Il riposizionamento energetico promuove un marcato **trasferimento di carica intramolecolare**, con drastica riduzione del salto energetico, e permette di centrare lo spettro di assorbimento ed emissione nella regione visibile (rif. [[49-hendriks-2013|49]]). + +## Scelta DPP + 3HT nella tesi (r.520-522) +- Il nucleo elettron-accettore del DPP è combinato con unità di **3-esiltiofene (3HT)**, fortemente elettron-donatrici. +- Il tiofene è partner elettronico ideale per ibridare gli orbitali di frontiera del DPP e, con la catena esilica laterale, garantisce **solubilità** e quindi processabilità (rif. [[49-hendriks-2013|49]]). +- La sinergia D-A DPP/3HT permette di sintonizzare la struttura a bande: requisiti per un impiego come **strato elettro-luminescente in OLED**. Dati reali del band gap: [[ciclovoltammetria]]. Sintesi: [[copolimeri-3a-3b-3c]]. + +## Struttura di un OLED (r.524-528) +- Architettura multistrato (sandwich) per ottimizzare iniezione, trasporto e ricombinazione di carica. I primi dispositivi a singolo strato avevano efficienze ridotte per forte sbilanciamento tra mobilità di elettroni e lacune. +- **EML** (Emissive Layer) tra due elettrodi asimmetrici: anodo trasparente di ossido di indio-stagno (**ITO**), alto lavoro di estrazione, trasparente alla luce visibile; catodo metallico a basso lavoro di estrazione (leghe di alluminio, calcio o bario). +- Strati ausiliari **HTL** (Hole Transport Layer) ed **ETL** (Electron Transport Layer) abbassano le barriere energetiche all'interfaccia elettrodi/polimero ([[fig-037|Fig. 37]]). + +![[immagini/86a414964c7edb97a911082e5b5baced59db545ce7d435e1d67b21d038ceee5a.jpg|560]] +*Figura 37 - rappresentazione schematica dell'architettura OLED* · [[fig-037|nota figura]] + +## Elettroluminescenza (r.534-542) +1. Con una differenza di potenziale il catodo inietta elettroni nel LUMO dell'ETL, verso il materiale emissivo; l'anodo estrae elettroni dall'HOMO dell'HTL iniettando cariche positive («lacune»). +2. Nei semiconduttori organici macromolecolari il trasporto avviene per **hopping**, meccanismo quantistico tra stati energetici localizzati lungo le catene o tra catene adiacenti (a differenza delle bande di conduzione delocalizzate degli inorganici; rif. [[45-ostroverkhova-2016|45]]). +3. Nel copolimero DPP-3HT, la tendenza del nucleo planare del DPP a interazioni intermolecolari a corto raggio promuove domini microstrutturali ordinati nel film solido (rif. [[44-bao-2020|44]]); una morfologia ordinata e omogenea aumenta la sovrapposizione degli orbitali π tra molecole vicine, facilita l'hopping e fa convergere elettroni e lacune nel bulk dello strato emissivo. +4. Un elettrone (sull'unità accettrice DPP) e una lacuna (sull'unità donatrice tiofene) formano un **eccitone**, stato transitorio termodinamicamente instabile: l'elettrone rilassa dal LUMO e si ricombina con la lacuna nell'HOMO, rilasciando l'energia come fotone ([[fig-038|Fig. 38]]; rif. [[45-ostroverkhova-2016|45]]). +5. L'entità del band gap corrisponde approssimativamente all'energia del fotone emesso ($E=h\nu$): il controllo chimico della struttura governa lunghezza d'onda, intensità e colore della luce; il copolimero DPP-3HT è proposto come candidato per display flessibili e illuminazione a stato solido. + +![[immagini/af427dca9415944332b7e4022b98a9f345a78495915bbadf60d254143c3d545e.jpg|560]] +*Figura 38 - profilo energetico dell'elettroluminescenza in un polimero coniugato* · [[fig-038|nota figura]] + +## Contesto di progetto (§2, r.547-549) +La tesi è svolta in un gruppo dell'Università di Bologna specializzato in materiali polimerici ingegnerizzati, con attenzione alla **soft optoelectronics**: ramo interdisciplinare che combina emissione e rilevamento della luce con dispositivi flessibili e adattabili (interfacce interattive, robotica biomimetica, sensori indossabili per la salute). Il problema dei materiali π-coniugati è la perdita di proprietà ottiche allo stato solido → [[acq-e-stato-solido]]. + +## Collegamenti +- [[dpp-struttura-e-proprieta]] · [[acq-e-stato-solido]] · [[ciclovoltammetria]] · [[bottle-brush]] +- [[tesi]] · [[bibliografia]] diff --git a/wiki/concepts/polimerizzazione-ossidativa-fecl3.md b/wiki/concepts/polimerizzazione-ossidativa-fecl3.md new file mode 100644 index 0000000..21fb976 --- /dev/null +++ b/wiki/concepts/polimerizzazione-ossidativa-fecl3.md @@ -0,0 +1,61 @@ +--- +title: Polimerizzazione ossidativa con FeCl3 +type: concept +tags: [polimerizzazione-ossidativa, fecl3, nitrometano, cloroformio, work-up, set] +created: 2026-10-09 +updated: 2026-10-09 +tesi_loc: "§1.1.2 r.355-361; §4.2 r.828-858" +refs: [53, 52] +figures: ["fig-028", "fig-052", "fig-053"] +status: draft +--- + +# Polimerizzazione ossidativa con FeCl3 + +Metodo usato per costruire lo scheletro coniugato DPP-3HT ([[copolimeri-3a-3b-3c]]). Procedura sperimentale con quantità: [[copolimeri-3a-3b-3c]] (§3.2, r.642-644). + +## Introduzione dal cap. 1 (r.355-361) +- Alternativa più economica all'arilazione ossidativa (che richiede ossidanti massicci come Ag2CO3, vedi [[dpp-reattivita]]) per polimeri coniugati, in particolare per DPP affiancati da anelli tiofenici (come il precursore **29**). +- A differenza dei cross-coupling al Pd **non richiede pre-attivazione** dei monomeri (alogenazione, borilazione, stannilazione) né metalli di transizione pregiati. +- Procede in solventi poco polari; FeCl3 agisce sia da **acido di Lewis** sia da **ossidante**, innescando la formazione di radical cationi sugli anelli tiofenici che portano alla formazione del legame C-C e alla crescita della catena ([[fig-028|Fig. 28]]). +- Limite: l'ossidazione chimica offre minore controllo su polidispersione e regioregolarità rispetto a Suzuki o Stille, ma è un approccio «estremamente diretto e scalabile» per materiali semiconduttori con eccellenti proprietà optoelettroniche. + +![[immagini/043876b8b6cbe0ab2f02e61ee15320a65446a515e24ab474e51cb7ee2a53fe17.jpg|560]] +*Figura 28 - meccanismo di polimerizzazione ossidativa mediante FeCl3* · [[fig-028|nota figura]] + +## Perché questo metodo (§4.2, r.830-832) +- La scelta del 3HT come comonomero deriva dalla collaborazione con il gruppo del Prof. Lanzi, la cui esperienza pregressa ha convalidato efficacia e versatilità della polimerizzazione ossidativa su questa classe di derivati tiofenici. +- **Vantaggi operativi**: nessuna pre-funzionalizzazione dei monomeri (meno step sintetici); condizioni blande (temperatura ambiente e pressione atmosferica); semplicità esecutiva e basso costo energetico; grande potenziale di **scale-up**. +- **Perché 3HT**: i politiofeni sono tra i più efficienti polimeri semiconduttori organici (rif. [[52-abdel-aziz-2025|52]]). Doppio obiettivo: la catena esilica aumenta la solubilità nei comuni solventi organici (processabilità); l'anello tiofenico estende il sistema π-coniugato e modula il band gap e il trasporto di carica. + +![[immagini/0cc72ddb7b8a730785dfaeb2abb381f6ef486e86e068d50b5d0b0ac0e8bc220d.jpg|560]] +*Figura 52 - schema di reazione dei copolimeri coniugati* · [[fig-052|nota figura]] + +## Meccanismo (r.840 e [[fig-053|Fig. 53]]) +1. FeCl3 è l'ossidante, in **eccesso stechiometrico** rispetto ai reagenti. +2. Fe3+ attiva i monomeri per **trasferimento mono-elettronico (SET)** (rif. [[53-paganin-nd|53]]): estrae un elettrone dagli anelli tiofenici (elettron-ricchi) e si riduce a Fe2+. +3. Si generano **cationi radicalici** fortemente delocalizzati sul sistema π-coniugato di DPP e tiofeni: sono i centri attivi, che si legano formando i nuovi legami C-C e la crescita di catena. + +![[immagini/34cdcf9d6836a55ee2dd35ac99f5e80cd9dffb87cbfaf818b5257c5ccfed2b51.jpg|560]] +*Figura 53 - meccanismo di polimerizzazione ossidativa mediante tricloruro ferrico* · [[fig-053|nota figura]] + +## Ruolo del nitrometano (CH3NO2) (r.846) +- In stato solido e in solventi non coordinanti come il cloroformio, FeCl3 forma dimeri o aggregati, con siti attivi limitati alla superficie o ai difetti dei cluster. +- Il nitrometano, come **legante**, rompe i ponti alogeno intermolecolari, spezza i dimeri e solvata il cloruro ferrico → soluzione omogenea di centri metallici discreti e stericamente accessibili per il trasferimento elettronico. +- La coordinazione con il nitrometano **modera** acidità di Lewis e potenziale ossidante: controllando la forza dell'ossidante si prevengono iper-ossidazione della catena e difetti di reticolazione (cross-linking); migliora la regioselettività, massimizzando regolarità strutturale ed estensione della π-coniugazione nel copolimero **3**. + +## Ruolo del cloroformio anidro (r.848) +Necessario per prevenire reazioni indotte dall'umidità. L'acqua (nucleofilo e base di Lewis) potrebbe: (1) coordinarsi a FeCl3 formando specie idrate stabili, saturando la sfera di coordinazione, riducendo il potenziale ossidativo e inibendo l'innesco; (2) causare il **quenching degli intermedi cationico-radicalici** in propagazione per attacco nucleofilo, con terminazione prematura e difetti che interrompono la coniugazione e compromettono le proprietà semiconduttrici. + +## Work-up e purificazione (r.850-858; procedura r.644) +| Passaggio | Funzione | +|---|---| +| Lavaggi con **HCl** (0,6 M) | mantengono i sali di ferro in fase acquosa evitando la precipitazione come idrossidi insolubili all'interfaccia. La rimozione completa dell'ossidante è un requisito: tracce di metalli di transizione nel backbone abbatterebbero la mobilità dei portatori e spegnerebbero la fluorescenza | +| **Saggio del tiocianato** sulle acque di lavaggio | SCN- + Fe3+ → complesso rosso intenso. Lavaggi ripetuti fino a saggio negativo (soluzione incolore; test dal terzo lavaggio) | +| Ultimo lavaggio con soluzione acquosa (mezza) satura di **NaCl** | salting-out: estrae l'acqua parzialmente disciolta nel solvente organico (pre-anidrificazione) e trascina le ultime impurità idrosolubili (HCl residuo) | +| Anidrificazione ed evaporazione | fase organica pura | +| **Precipitazione solvente/non-solvente**: solido solubilizzato nel minimo THF, gocciolato in un ampio eccesso di **metanolo freddo** (150 mL) | allontana i sottoprodotti, primo fra tutti l'omopolimero del 3HT (poli-3HT), che è insolubile nel non-solvente e precipita; il copolimero resta in soluzione e si isola portando a secco la fase liquida | + +## Collegamenti +- [[copolimeri-3a-3b-3c]] · [[dpp-reattivita]] · [[optoelettronica-oled-donatore-accettore]] · [[reagenti-e-materiali]] +- [[tesi]] · [[bibliografia]] diff --git a/wiki/concepts/rop-pcl.md b/wiki/concepts/rop-pcl.md new file mode 100644 index 0000000..47601eb --- /dev/null +++ b/wiki/concepts/rop-pcl.md @@ -0,0 +1,54 @@ +--- +title: ROP dell'ε-caprolattone e catene di PCL +type: concept +tags: [rop, pcl, caprolattone, snoct2, grafting-from, macroiniziatore] +created: 2026-10-09 +updated: 2026-10-09 +tesi_loc: "§4.3 r.959-979" +refs: [55, 56] +figures: ["fig-063", "fig-x-136800"] +status: draft +--- + +# ROP dell'ε-caprolattone e catene di PCL + +ROP = Ring Opening Polymerization. PCL = poli(ε-caprolattone). Applicazione ai campioni: [[bottle-brush-3-x]]; architettura complessiva: [[bottle-brush]]. + +## Perché grafting-from con ROP (r.965) +- L'architettura bottle brush con approccio **«grafting from»** richiede che la catena principale sia predisposta come **macroiniziatore**: l'unità DPP è stata progettata con una funzionalità **ossidrilica terminale** ([[dpp-2]]). +- Il gruppo **-OH** è il sito nucleofilo iniziatore della ROP, che permette di **regolare il peso molecolare** e **mantenere bassa la dispersità** delle catene laterali in crescita: parametri rilevanti per bottle brush regolari e riproducibili. +- Precedente di letteratura (main-chain, DPP-OH + CL → PCL-DPP-PCL): [[fluorofori-in-polimeri]]. + +## Perché PCL (r.967) +- Scelta basata su studi precedenti del gruppo di ricerca. +- La ROP del caprolattone è un processo **lineare ed efficiente**. +- Proprietà del PCL: bassa temperatura di transizione vetrosa (Tg) e buona solubilità nei comuni solventi organici (rif. [[55-woodruff-2010|55]]) → semplicità di lavorazione e di integrazione del sistema bottle brush in una matrice polimerica per i materiali finali. + +## Meccanismo con Sn(Oct)2 (r.969, [[fig-063|Fig. 63]]) +- Esistono diversi meccanismi di ROP (rif. [[56-labet-2009|56]]); uno dei più sfruttati è quello di **coordinazione-inserzione** del monomero sul centro attivo dell'iniziatore. +- La ROP catalizzata da **stagno ottanoato (Sn(Oct)2)** richiede in genere l'aggiunta di co-iniziatori nucleofili come alcoli. +- Sequenza: (1) scambio di leganti tra l'alcol e l'ottanoato del catalizzatore → specie attiva; (2) il centro metallico si coordina al carbonile del caprolattone, rendendo il carbonio più elettrofilo; (3) attacco nucleofilo del gruppo alcolico con apertura dell'anello; (4) la crescita del PCL prosegue per attacchi successivi del terminale ossidrilico, che mantiene la reattività durante la propagazione. + +![[immagini/86add528de15d390b0a228d524bbd008d318d4ae0e85530a063f2df5ddf904ee.jpg|560]] +*Figura 63 - meccanismo di reazione della ROP con gruppo alcolico come iniziatore* · [[fig-063|nota figura]] + +## Controllo della lunghezza delle catene (r.979, Tab. 9) +La lunghezza delle catene laterali si modula variando il **rapporto molare monomero (ε-caprolattone) / siti iniziatori (-OH)** sul backbone. Target di Mn delle catene di PCL: **1500, 5000, 10000 Da**. Formula per il volume di caprolattone ($V_{CL}$) e tabella dei campioni in [[bottle-brush-3-x]]. + +## Condizioni sperimentali (§3.2, r.663) +Toluene, **110 °C**, catalizzatore Sn(Oct)2 in quantità catalitica, reflusso per **24 h** (nota: lo schema [[fig-x-136800|schema bottle brush]] riporta 4 h; vedi [[difetti-noti]]). Dettaglio in [[bottle-brush-3-x]]. + +![[immagini/136800375cf0b441570672093e255d90a47c45a009bd254929fb74b1f17b382d.jpg|560]] +*schema bottle brush (didascalia generata dal catalogo): Polimerizzazione ad apertura di anello di epsilon-caprolattone sui gruppi OH dei copolimeri DPP-3HT per ottenere i polimeri bottle brush con catene di PCL.* · [[fig-x-136800|nota figura]] + +## Purificazione (r.975) +Precipitazione in non-solvente: miscela di reazione gocciolata in largo eccesso di **metanolo freddo**. L'ε-caprolattone residuo e le specie a basso peso molecolare hanno elevata affinità per il metanolo; il copolimero ad alto peso molecolare vi è insolubile. La bassa temperatura riduce ulteriormente la solubilità del polimero, ne favorisce la rapida coagulazione e massimizza la resa. Il precipitato è recuperato per filtrazione. + +## Verifica dell'innesto +- ¹H-NMR: tripletto a ~4,0 ppm (-CH2-O- adiacente all'ossigeno estereo) e segnale a 2,3 ppm (protoni in α al carbonile) → [[nmr-1h]]. +- FT-IR: scomparsa della banda O-H (3600-3200 cm⁻¹) e comparsa del C=O estereo a ~1720 cm⁻¹ → [[ft-ir]]. +- GPC: [[gpc]] (valori sottostimati per effetto dell'architettura). + +## Collegamenti +- [[bottle-brush]] · [[bottle-brush-3-x]] · [[dpp-2]] · [[copolimeri-3a-3b-3c]] · [[fluorofori-in-polimeri]] +- [[tesi]] · [[bibliografia]] diff --git a/wiki/figures/fig-009.md b/wiki/figures/fig-009.md index 0c9e481..414bda7 100644 --- a/wiki/figures/fig-009.md +++ b/wiki/figures/fig-009.md @@ -21,6 +21,8 @@ derivata: true _Posizione: tesi.md §1.1.1 r.164 (sezione 1.1.1 Storia e sintesi), didascalia r.166_ +> ⚠ Flag `caption_mismatch`: la didascalia stampata qui sopra è quella attribuita dal catalogo e potrebbe non descrivere l'immagine (vedi «Didascalia generata» e «Da verificare»). + > Sotto: contenuto generato guardando l'immagine, non verificato una per una. **Didascalia generata:** Sintesi del DPP3 secondo Closs e Gompper: succindiammide e N,N-dimetilbenzammide dietilacetale danno il bis-amidino intermedio, che con t-BuOK cicla a DPP3. diff --git a/wiki/figures/fig-026.md b/wiki/figures/fig-026.md index 0cd70d1..bf4c5e0 100644 --- a/wiki/figures/fig-026.md +++ b/wiki/figures/fig-026.md @@ -21,6 +21,8 @@ derivata: true _Posizione: tesi.md §1.1.2 r.343 (sezione 1.1.2 Struttura e reattività), didascalia r.345_ +> ⚠ Flag `caption_mismatch`: la didascalia stampata qui sopra è quella attribuita dal catalogo e potrebbe non descrivere l'immagine (vedi «Didascalia generata» e «Da verificare»). + > Sotto: contenuto generato guardando l'immagine, non verificato una per una. **Didascalia generata:** Arilazione diretta dei DPP dibromurati 32 e 37 con tiofeni sostituiti (Y-tiofene) a dare i prodotti 39, 40 e 41. diff --git a/wiki/figures/fig-027.md b/wiki/figures/fig-027.md index 72a6c4c..fc30a87 100644 --- a/wiki/figures/fig-027.md +++ b/wiki/figures/fig-027.md @@ -21,6 +21,8 @@ derivata: true _Posizione: tesi.md §1.1.2 r.349 (sezione 1.1.2 Struttura e reattività), didascalia r.351_ +> ⚠ Flag `caption_mismatch`: la didascalia stampata qui sopra è quella attribuita dal catalogo e potrebbe non descrivere l'immagine (vedi «Didascalia generata» e «Da verificare»). + > Sotto: contenuto generato guardando l'immagine, non verificato una per una. **Didascalia generata:** Arilazione ossidativa (attivazione C-H) del DPP 29 con fluoroareni polifluorurati (X = N, C-CN, C-F) per dare i prodotti 42a-c. diff --git a/wiki/figures/fig-029.md b/wiki/figures/fig-029.md index bab3c7f..f766a56 100644 --- a/wiki/figures/fig-029.md +++ b/wiki/figures/fig-029.md @@ -21,6 +21,8 @@ derivata: true _Posizione: tesi.md §1.1.2 r.365 (sezione 1.1.2 Struttura e reattività), didascalia r.367_ +> ⚠ Flag `caption_mismatch`: la didascalia stampata qui sopra è quella attribuita dal catalogo e potrebbe non descrivere l'immagine (vedi «Didascalia generata» e «Da verificare»). + > Sotto: contenuto generato guardando l'immagine, non verificato una per una. **Didascalia generata:** Litiazione del DPP 29 con LDA a -78 °C e successiva reazione con elettrofili per dare i derivati 43-46 funzionalizzati in C5 dei tiofeni. diff --git a/wiki/figures/fig-057.md b/wiki/figures/fig-057.md index 1c3ca89..4e82ab5 100644 --- a/wiki/figures/fig-057.md +++ b/wiki/figures/fig-057.md @@ -21,6 +21,8 @@ derivata: true _Posizione: tesi.md §4.2 r.900 (sezione 4.2 Copolimeri coniugati), didascalia r.902_ +> ⚠ Flag `caption_mismatch`: la didascalia stampata qui sopra è quella attribuita dal catalogo e potrebbe non descrivere l'immagine (vedi «Didascalia generata» e «Da verificare»). + > Sotto: contenuto generato guardando l'immagine, non verificato una per una. **Didascalia generata:** Spettri FT-IR sovrapposti dei copolimeri 3a, 3b e 3c. diff --git a/wiki/figures/fig-062.md b/wiki/figures/fig-062.md index 2fa7757..705c864 100644 --- a/wiki/figures/fig-062.md +++ b/wiki/figures/fig-062.md @@ -21,6 +21,8 @@ derivata: true _Posizione: tesi.md §4.3 r.961 (sezione 4.3 Polimeri bottle brush), didascalia r.963_ +> ⚠ Flag `caption_mismatch`: la didascalia stampata qui sopra è quella attribuita dal catalogo e potrebbe non descrivere l'immagine (vedi «Didascalia generata» e «Da verificare»). + > Sotto: contenuto generato guardando l'immagine, non verificato una per una. **Didascalia generata:** Schema dell'effetto dell'intensità dello stacking π-π sull'emissione luminosa. diff --git a/wiki/figures/fig-065.md b/wiki/figures/fig-065.md index 9921ef4..8457d20 100644 --- a/wiki/figures/fig-065.md +++ b/wiki/figures/fig-065.md @@ -21,6 +21,8 @@ derivata: true _Posizione: tesi.md §4.3 r.1012 (sezione 4.3 Polimeri bottle brush), didascalia r.1014_ +> ⚠ Flag `caption_mismatch`: la didascalia stampata qui sopra è quella attribuita dal catalogo e potrebbe non descrivere l'immagine (vedi «Didascalia generata» e «Da verificare»). + > Sotto: contenuto generato guardando l'immagine, non verificato una per una. **Didascalia generata:** Spettri FT-IR sovrapposti dei polimeri bottle brush derivati dal copolimero 3b (precursore, verde) e dei polimeri 3.1b (arancione), 3.2b (rosa), 3.3b (azzurro). diff --git a/wiki/figures/fig-066.md b/wiki/figures/fig-066.md index 1315a1d..7d47c5e 100644 --- a/wiki/figures/fig-066.md +++ b/wiki/figures/fig-066.md @@ -21,6 +21,8 @@ derivata: true _Posizione: tesi.md §4.3 r.1018 (sezione 4.3 Polimeri bottle brush), didascalia r.1020_ +> ⚠ Flag `caption_mismatch`: la didascalia stampata qui sopra è quella attribuita dal catalogo e potrebbe non descrivere l'immagine (vedi «Didascalia generata» e «Da verificare»). + > Sotto: contenuto generato guardando l'immagine, non verificato una per una. **Didascalia generata:** Spettri FT-IR sovrapposti dei polimeri bottle brush derivati dal copolimero 3c (precursore, verde) e dei polimeri 3.1c (arancione), 3.2c (rosa), 3.3c (azzurro). diff --git a/wiki/figures/fig-x-136800.md b/wiki/figures/fig-x-136800.md index 7976267..52459c6 100644 --- a/wiki/figures/fig-x-136800.md +++ b/wiki/figures/fig-x-136800.md @@ -21,6 +21,8 @@ derivata: true _Posizione: tesi.md §3.2 r.648 (sezione 3.2 Sintesi e procedure), didascalia r.661_ +> ⚠ Flag `caption_mismatch`: la didascalia stampata qui sopra è quella attribuita dal catalogo e potrebbe non descrivere l'immagine (vedi «Didascalia generata» e «Da verificare»). + > Sotto: contenuto generato guardando l'immagine, non verificato una per una. **Didascalia generata:** Polimerizzazione ad apertura di anello di epsilon-caprolattone sui gruppi OH dei copolimeri DPP-3HT per ottenere i polimeri bottle brush con catene di PCL. diff --git a/wiki/figures/fig-x-cc3f54.md b/wiki/figures/fig-x-cc3f54.md index 80f7908..2afbd32 100644 --- a/wiki/figures/fig-x-cc3f54.md +++ b/wiki/figures/fig-x-cc3f54.md @@ -21,6 +21,8 @@ derivata: true _Posizione: tesi.md §3.2 r.630 (sezione 3.2 Sintesi e procedure), didascalia r.640_ +> ⚠ Flag `caption_mismatch`: la didascalia stampata qui sopra è quella attribuita dal catalogo e potrebbe non descrivere l'immagine (vedi «Didascalia generata» e «Da verificare»). + > Sotto: contenuto generato guardando l'immagine, non verificato una per una. **Didascalia generata:** Copolimerizzazione ossidativa del DPP 2 con 3-esiltiofene (3HT) con FeCl3 per dare i copolimeri 3a/3b/3c. Il file è uno schema, non la Tabella 3. diff --git a/wiki/overview.md b/wiki/overview.md index 6ba7626..b17998f 100644 --- a/wiki/overview.md +++ b/wiki/overview.md @@ -1,19 +1,48 @@ --- title: Overview type: overview -tags: [overview] +tags: [overview, sintesi] created: 2026-10-09 updated: 2026-10-09 -sources: +tesi_loc: "Riassunto r.13-23; Abstract r.25-33; §2 r.545-559; §5 r.1279-1291" +refs: [] status: draft --- # Overview -Tema e research question: _da definire alla prima ingest._ +Sintesi della tesi (unica fonte ingerita finora): dichiarazioni del Riassunto/Abstract, dello Scopo e delle Conclusioni, con rimando alle pagine di dettaglio. Mappa completa: [[tesi]]. Incoerenze da tener presenti: [[difetti-noti]]. -## Stato della sintesi -Nessuna fonte ancora ingerita. +## Problema e research question +I semiconduttori π-coniugati usati nella soft optoelectronics perdono emissione allo stato solido per **ACQ** (Aggregation-Caused Quenching): la planarità induce forte π-stacking e dissipazione non radiativa (Abstract r.27; §2 r.549). **Domanda**: una architettura **bottle brush** può separare fisicamente i segmenti coniugati, ripristinando l'emissione allo stato solido e preservando integrità elettrochimica e stabilità (§2 r.553)? → [[acq-e-stato-solido]], [[bottle-brush]]. + +## Strategia in quattro passi (Abstract r.29; §4; §5 r.1283-1285) +1. **Monomero ortogonale** DPP-tiofene con due -OH: ciclizzazione pseudo-Stobbe di 2-cianotiofene e diisopropil succinato → [[dpp-1]]; N-alchilazione con 6-bromo-1-esanolo → [[dpp-2]]. +2. **Scheletro coniugato** per polimerizzazione ossidativa diretta con 3HT (FeCl3/nitrometano) → copolimeri statistici **3a, 3b, 3c** ([[copolimeri-3a-3b-3c]], [[polimerizzazione-ossidativa-fecl3]]). +3. **Catene laterali** di PCL per ROP dell'ε-caprolattone (Sn(Oct)2) dai -OH di **3b** e **3c**: Mn target 1500, 5000, 10000 Da → 6 bottle brush ([[bottle-brush-3-x]], [[rop-pcl]]). +4. **Caratterizzazione**: [[nmr-1h]], [[ft-ir]], [[gpc]], [[uv-vis-fluorescenza]], [[dsc]], [[ciclovoltammetria]]. + +## Risultati dichiarati (con riferimento ai dati) +| Tema | Risultato | Dati / pagina | +|---|---|---| +| Struttura | analisi spettroscopiche (¹H-NMR, FT-IR) e GPC confermano la sintesi e macromolecole ramificate ad alta densità strutturale (Riassunto r.19) | [[nmr-1h]], [[ft-ir]], [[gpc]] | +| Copolimeri lineari | Mn 1400-2150 Da; Tg ≈ −10 °C; DPP incorporato al massimo 35% (25,2 / 32,6 / 35,3%) | [[copolimeri-3a-3b-3c]] | +| Innesto del PCL | scompare l'O-H, compare il C=O a ~1720 cm⁻¹; PD 1,23-1,52 (GPC); volume idrodinamico contratto rispetto al lineare | [[bottle-brush-3-x]], [[gpc]] | +| Termico | dominato dal PCL: Tm 55-60 °C, Tc 25-35 °C | [[dsc]] | +| Ottico in soluzione | core DPP intatto: λabs 544-554 nm, λem 557-564 nm, Stokes shift 8-14 nm | [[uv-vis-fluorescenza]] | +| Ottico allo stato solido | film lineari non emissivi; bottle brush 3.2b: assorbimento 570-580 nm, emissione ~650-660 nm; emissione nel rosso apprezzabile | [[acq-e-stato-solido]] | +| Elettrochimico | processi EC irreversibili; bandgap 0,970-1,371 eV (lineari, crescente con la % di DPP) e 0,929-1,521 eV (bottle brush) | [[ciclovoltammetria]] | + +## Conclusione della tesi (§5, r.1291) +L'approccio ortogonale basato su scheletri semiconduttori DPP-3HT modificati con catene laterali di PCL combina **proprietà elettrochimiche modulabili** e **capacità emissiva allo stato solido**, con potenziale per dispositivi optoelettronici. + +## Limiti e dubbi evidenziati dalla tesi o dall'ingest +- Il DPP incorporato non supera il **35%** (reattività dei comonomeri, ingombro sterico del DPP) (r.862). +- **3a** non usato per il grafting (basse rese, work-up) (r.977). +- GPC dei bottle brush sottostima (r.1058); outlier **3.3c** (r.1062); Mn da NMR non sempre vicino al teorico ([[difetti-noti]], punto 7). +- Emissione allo stato solido mostrata solo per **3.2b**; la tesi non riporta rese quantiche allo stato solido (verificato su `raw/tesi.md`). +- Le Conclusioni riportano valori di bandgap e R² non coerenti con la Tabella 13, e una fusione dei lineari non coerente con la DSC (punti 5-6 di [[difetti-noti]]). ## Collegamenti -- [[index]] +- [[tesi]] · [[bibliografia]] · [[difetti-noti]] · [[index]] +- Concetti: [[bottle-brush]] · [[acq-e-stato-solido]] · [[dpp-struttura-e-proprieta]] · [[optoelettronica-oled-donatore-accettore]] diff --git a/wiki/techniques/ciclovoltammetria.md b/wiki/techniques/ciclovoltammetria.md new file mode 100644 index 0000000..336ff3b --- /dev/null +++ b/wiki/techniques/ciclovoltammetria.md @@ -0,0 +1,167 @@ +--- +title: Ciclovoltammetria (CV) +type: technique +tags: [cv, elettrochimica, bandgap, homo-lumo, onset, ferrocene, drogaggio] +created: 2026-10-09 +updated: 2026-10-09 +tesi_loc: "§3.3 r.666-699; §3.4 r.702-714; §4.4 r.1100-1251; §5 r.1289" +refs: [50] +figures: ["fig-039", "fig-069", "fig-070", "fig-071", "fig-072", "fig-073"] +status: draft +--- + +# Ciclovoltammetria (CV) + +La CV è una tecnica elettrochimica dinamica della famiglia delle voltammetriche, usata per studiare i processi redox; per materiali macromolecolari e coniugati serve a indagare trasferimento elettronico, stabilità elettrochimica e **gap energetico elettrochimico** (§4.4, r.1102-1104). Risultati per composto: [[copolimeri-3a-3b-3c]], [[bottle-brush-3-x]]. + +## 1. Principi teorici (§3.3, r.668-699) +- A differenza delle tecniche in stato stazionario il potenziale varia in modo continuo nel tempo (strumento utile per i meccanismi di trasferimento elettronico). +- **Cella a tre elettrodi** con potenziostato: + - **WE** (Working Electrode): superficie dove avviene l'ossidazione o riduzione del campione. + - **RE** (Reference Electrode): potenziale noto e stabile (es. Ag/AgCl o filo d'argento come pseudo-riferimento). Il potenziostato ha impedenza d'ingresso molto elevata: nel RE non passa corrente, non si polarizza, il riferimento resta costante. + - **CE** (Counter Electrode): materiale inerte ad ampia area (es. filo di platino); chiude il circuito e permette il passaggio della corrente che bilancia la reazione faradica sul WE. +- Il WE riceve un potenziale che varia linearmente nel tempo con **onda triangolare**: da Ei a Eλ (inversione) a velocità costante (scan rate, V/s), poi inversione del verso. +- La corrente misurata = **corrente capacitiva** (carica/scarica del doppio strato elettrico all'interfaccia) + **corrente faradica** (trasferimento di elettroni reale, legge di Faraday). +- **Elettrolita di supporto**: minimizza la caduta ohmica e sopprime la migrazione delle specie cariche; il moto delle specie elettroattive è governato quasi solo da **diffusione** (gradiente di concentrazione). +- In un processo redox reversibile, avvicinandosi al potenziale standard di riduzione E0 la corrente faradica sale secondo Nernst: + +$$ +E=E^{0}+\frac{RT}{nF}ln\left(\frac{C_{ox}}{C_{red}}\right) +$$ +**Equazione 6** - *equazione di Nernst* + +- La corrente cresce fino al picco **Ip**: lo strato di soluzione vicino all'elettrodo si impoverisce, il processo è limitato dalla diffusione dal bulk. Dopo il picco lo strato di diffusione si espande e la corrente decresce come t-1/2 (**Cottrell**): + +$$ +I\left(t\right)=\frac{nFAD^{1/2}C^{*}}{\pi ^{1/2}t^{1/2}} +$$ +**Equazione 7** - *equazione di Cottrell* + +con I(t) corrente al tempo t, n numero di elettroni scambiati, F costante di Faraday, A area attiva dell'elettrodo, D coefficiente di diffusione, C\* concentrazione nel bulk, t tempo. +- Invertendo il potenziale, le specie generate subiscono il processo inverso e danno un picco di corrente di segno opposto. +- Per un sistema diffusivo ideale e reversibile (**Randles-Sevcik**): + +$$ +I_{p}=\left(2{,}69\times 10^{5}\right)\cdot n^{3/2}\cdot A\cdot D^{1/2}\cdot C\cdot v^{1/2} +$$ +**Equazione 8** - *equazione di Randles-Sevcik* + +n = elettroni scambiati; A = area attiva (cm²); D = coefficiente di diffusione (cm²/s); C = concentrazione nel bulk (mol/cm³); v = velocità di scansione (V/s, 25 °C). La proporzionalità lineare fra Ip e v1/2 è il criterio per confermare che il processo è controllato dal trasporto di materia per diffusione. + +## 2. Procedura sperimentale (§3.4, r.704-714) +![[immagini/7454f0793d62db92121d98aa27815bc85d5aae9f16807d3f188d7feb1ee83463.jpg|560]] +*Figura 39 - schema della cella elettrochimica impiegata nelle misure voltammetriche* · [[fig-039|nota figura]] + +- Temperatura ambiente; potenziostato **CHI660C (CH Instruments)**; cella standard a tre elettrodi ([[fig-039|Fig. 39]]): WE in **glassy carbon**, RE **Ag/AgCl**, CE **filo di platino**. +- Misure in fase omogenea, solvente **THF**; elettrolita di supporto **TBAPF6 0,1 M**. +- CV del **bianco** sulla sola soluzione elettrolitica (verifica pulizia e assenza di specie elettroattive interferenti nella finestra di potenziale). Poi soluzioni polimeriche a concentrazione fissa **10 mg/mL**. +- **Degasaggio** con gorgogliamento di azoto per rimuovere l'ossigeno disciolto (si ridurrebbe al catodo); poi il flusso viene rimosso dalla soluzione (evita perturbazioni meccaniche) e mantenuto solo come battente. +- Scansioni di base per l'identificazione dei processi redox a **0,05 V/s**; poi variazione delle velocità (**0.05, 0.1, 0.5 e 1.0 V/s**) per l'influenza della cinetica di trasferimento. +- A fine misura di ogni campione si aggiunge **ferrocene** direttamente nella cella come **standard redox interno** (i potenziali misurati sono relativi e dipendono dal riferimento): la coppia reversibile Fc/Fc+ di potenziale noto calibra l'asse e riferisce gli onset alla scala assoluta delle energie nel vuoto, necessario per calcolare HOMO e LUMO (rif. [[50-cardona-2011|50]]). + +## 3. Scopo nel progetto (§4.4.1, r.1109-1115) +- Verificare l'**elettroattività** derivante dall'estesa coniugazione π e stimare un **band gap elettrochimico** compatibile con i semiconduttori. +- Identificare i processi redox dello scheletro e i **potenziali di onset** per il gap. +- Indagare la cinetica dei processi e il **grado di reversibilità**; profilo voltammetrico e andamento delle correnti in scansioni multiple consecutive distinguono un sistema che tollera il trasferimento ciclico di carica da eventuali degradazioni elettrochimiche. +- Funge da ponte tra validazione dell'architettura elettronica dei bottle brush e stabilità operazionale. + +## 4. Metodologia di analisi (§4.4.2, r.1120-1172) +**Parte qualitativa** — forma delle curve. I materiali coniugati subiscono due processi: estrazione di elettroni (**ossidazione, p-doping**) e iniezione di elettroni (**riduzione, n-doping**). La forma dei picchi e la presenza dei picchi di ritorno indicano reversibilità e stabilità sotto stress elettrochimico. + +**Parte quantitativa** — **potenziali di onset**, punto di partenza per il gap. + +Esempio di elaborazione: voltammogramma di **3.2c** a 0,05 V/s in THF con TBAPF6 0,1 M ([[fig-069|Fig. 69]]), ripetuto sistematicamente su tutti i voltammogrammi. + +![[immagini/6afc0d601841f25b1c02e27bc6b1616abc101c5f1ceaa0ba9d30ed0f965ebed2.jpg|560]] +*Figura 69 - voltammogramma ciclico del polimero 3.2.c registrato a una velocità di scansione di 0,05 V/s in soluzione di THF con TBAPF6 0,1 M* · [[fig-069|nota figura]] + +### Reversibilità +- In un sistema reversibile: picco diretto e picco di ritorno con rapporto Ipa/Ipc prossimo all'unità. +- Nei polimeri della tesi si osserva **sistematicamente** un marcato discostamento: ampie onde faradiche in andata **senza picco di ritorno simmetrico** → irreversibilità. +- A velocità crescenti ([[fig-070|Fig. 70]], 3.2c): totale assenza di onde di scarica simmetriche al ritorno e **progressiva diminuzione dell'intensità delle onde faradiche** → la specie generata è intrinsecamente **instabile** (degradazione e perdita di materiale elettroattivo all'interfaccia). + +![[immagini/5491a0651d00b47f168b335586b4f144e1b25834ff74113ff26b1d3a2c8cc991.jpg|560]] +*Figura 70 - voltammogramma ciclico del polimero 3.2.c registrato a diverse velocità di scansione* · [[fig-070|nota figura]] + +- Interpretazione: il trasferimento elettronico è accoppiato a fenomeni secondari che consumano/alterano irreversibilmente la specie generata. Scansione anodica = p-doping: formazione di specie positive (**polaroni**, radicali cationi); catodica = n-doping: specie **radical-anioniche**. La mancanza delle onde di ritorno indica che queste macromolecole cariche sono altamente instabili nelle condizioni usate. +- Un meccanismo ideale **E** (puro trasferimento di elettroni) darebbe processo inverso simmetrico; nei materiali è invece un meccanismo **EC** (elettrochimico-chimico): il trasferimento iniziale (fase E) genera un intermedio reattivo consumato da una reazione chimica secondaria (fase C) prima di poter restituire/accettare l'elettrone. Tipiche degradazioni irreversibili: accoppiamento tra catene radicaliche, sovraossidazione, reazioni parassite. Il materiale non ripristina lo stato neutro iniziale (asimmetria dei cicli). + +### Potenziale di onset (metodo grafico delle tangenti, [[fig-069|Fig. 69]]) +- A causa dell'irreversibilità, i **potenziali di picco** (Ep) sono fortemente alterati dalla degradazione delle specie cariche e **non sono affidabili** per i livelli energetici. Il potenziale di **onset** approssima meglio la minima energia per innescare i primi trasferimenti elettronici, correlandosi ai limiti di banda. +- Costruzione: (1) **baseline** — retta della sola corrente capacitiva (doppio strato) in un intervallo in cui il polimero è inerte, prima dell'avvio dei processi redox; (2) **tangente al punto di massima pendenza** del fronte di salita dell'onda (processo faradico di drogaggio); (3) l'**intersezione** delle due rette, proiettata sull'asse dei potenziali, dà il valore in Volt: onda anodica → Eonsetox; onda catodica → Eonsetred. +- Il metodo esclude l'interferenza della corrente di fondo ed è riproducibile. + +### Calibrazione con il ferrocene +- I valori sono relativi all'elettrodo Ag/AgCl e alle fluttuazioni solvente/elettrolita: serve calibrare l'asse. Il ferrocene (coppia Fc/Fc+ reversibile, stabile, potenziale ben noto) è il riferimento classico in solventi organici. +- L'energia associata all'ossidazione del ferrocene è convenzionalmente posta a **−4,8 eV** rispetto al livello del vuoto. +- Voltammogramma del ferrocene a fine analisi → potenziale di semionda sperimentale → sottratto a tutti i potenziali (scala Fc/Fc+). + +### Livelli energetici e bandgap +$$ +E_{HOMO}=-\left(E_{onset}^{ox}+4{,}8\right) eV E_{LUMO}=-\left(E_{onset}^{red}+4{,}8\right) eV +$$ +**Equazione 11** - *calcolo dei livelli energetici HOMO e LUMO* + +$$ +E_{g}=E_{LUMO}-E_{HOMO} +$$ +**Equazione 12** - *bandgap elettrochimico* + +## 5. Risultati sui copolimeri lineari (§4.4.3, r.1177-1227) +Scopo: capire come la **frazione reale di DPP** modula l'architettura energetica dello scheletro coniugato puro, senza gli effetti sterici/conformazionali dell'innesto. + +**Tabella 13** - *dati voltammetrici dei copolimeri sintetizzati* +| Polimero | % reale DPP | Eonsetox (V) | Eonsetred (V) | HOMO (eV) | LUMO (eV) | Bandgap (eV) | +| --- | --- | --- | --- | --- | --- | --- | +| 3a | 25 | 0,238 | -0,732 | -5,038 | -4,068 | 0,970 | +| 3b | 32 | 0,054 | -1,262 | -4,854 | -3,538 | 1,316 | +| 3c | 35 | 0,0006 | -1,372 | -4,799 | -3,428 | 1,371 | + +### Bandgap vs % DPP ([[fig-071|Fig. 71]]) +- All'aumentare del DPP si osserva un **allargamento progressivo del bandgap**: la variazione è governata dalla composizione stechiometrica effettiva. +- La netta pendenza positiva della retta di interpolazione indica forte sensibilità alla composizione: incrementi modesti di DPP aumentano molto l'energia per le transizioni elettroniche. Lettura della tesi: l'unità DPP **riduce la lunghezza di coniugazione effettiva**, limitando la delocalizzazione π e aumentando la separazione HOMO-LUMO. +- Dimostra la fattibilità di un controllo mirato del band gap calibrando il rapporto fra i due monomeri. + +![[immagini/6c7bd8393eb8c1a329f65b7fc74e5f338a866e514455c0122a43d13ca340ded5.jpg|560]] +*Figura 71 - correlazione tra bandgap elettrochimico e frazione reale di DPP nei copolimeri sintetizzati* · [[fig-071|nota figura]] + +### Potenziali di picco vs % DPP ([[fig-072|Fig. 72]]) +- **Riduzione (n-doping)**: variazione più marcata. Da 25% DPP (Epc ≈ −1 V) a 32-35% il picco si sposta tra **−1,6 V e −1,8 V**: l'inserzione di elettroni diventa termodinamicamente più sfavorita, con sovratensioni maggiori per formare i radical-anioni. +- **Ossidazione (p-doping)**: impatto minore; Epa passa da ≈ **0,4 V** (minor DPP) a ≈ **0,2/0,25 V** per frazioni maggiori. +- Effetto combinato: aumento della separazione tra i picchi con la % di DPP, coerente con l'aumento del bandgap. + +![[immagini/d7a3694f2d97dcaa84465aeed07d8d26adca6a8f8ed64f7ea2bf86943b918b66.jpg|560]] +*Figura 72 - correlazione tra Epicco e frazione reale di DPP nei copolimeri sintetizzati* · [[fig-072|nota figura]] + +### Potenziali di onset vs % DPP ([[fig-073|Fig. 73]]) +- Eonsetred (LUMO): da ≈ **−0,75 V** (basso DPP) a ≈ **−1,4 V** (frazioni maggiori). +- Eonsetox (HOMO): da ≈ **0,25 V** a quasi **0 V** (lieve traslazione). +- La progressiva separazione fra i due onset conferma l'allargamento del bandgap: la composizione agisce sistematicamente sui livelli di frontiera. + +![[immagini/b2931ebedd31df7df3b344c25fcbb4a64aceb7b356181adecf39363e49dcb0fe.jpg|560]] +*Figura 73 - correlazione tra Eonset e frazione reale di DPP nei copolimeri sintetizzati* · [[fig-073|nota figura]] + +### Confronto con P3HT (r.1223-1227) +- Il P3HT omopolimero è molto elettron-ricco: ossidazione (p-doping) a potenziali accessibili, **nessun contributo faradico significativo** per la riduzione (n-doping) nella consueta finestra dei solventi organici. +- Nei copolimeri il DPP, forte porzione elettron-attrattrice in un'architettura D-A, **stabilizza il LUMO**: rende favorevole l'iniezione di elettroni e giustifica le onde catodiche assenti nel P3HT. L'abbassamento del LUMO, con la modulazione dell'HOMO ad opera dei segmenti di 3HT, determina il **restringimento del bandgap** rispetto all'omopolimero. +- Conclusione della tesi: la sistematicità con cui la composizione influenza la risposta termodinamica convalida l'approccio come strumento di ingegnerizzazione del materiale. + +## 6. Effetto del design bottle brush (§4.4.4, r.1232-1251) +**Tabella 14** - *dati voltammetrici dei polimeri sintetizzati* +| Polimero | Eonsetox (V) | Eonsetred (V) | HOMO (eV) | LUMO (eV) | Bandgap (eV) | +| --- | --- | --- | --- | --- | --- | +| 3.1.b | -0,183 | -1,22 | -4,617 | -3,580 | 1,037 | +| 3.2.b | -0,175 | -1,273 | -4,625 | -3,527 | 1,098 | +| 3.3.b | -0,17 | -1,202 | -4,630 | -3,598 | 1,032 | +| 3.1.c | -0,0259 | -1,547 | -4,774 | -3,253 | 1,521 | +| 3.2.c | -0,112 | -1,531 | -4,688 | -3,269 | 1,419 | +| 3.3.c | -0,321 | -1,25 | -4,479 | -3,550 | 0,929 | + +- I bottle brush **mantengono l'elettroattività** dello scheletro: i processi redox avvengono a carico del core DPP-3HT, mentre i rami alifatici fungono da **matrice dielettrica** circostante. +- Le ingombranti catene laterali modificano HOMO e LUMO rispetto ai lineari, quindi l'ampiezza del bandgap. Attribuzione: effetti di ingombro sterico dei rami di PCL sul **grado di coplanarità locale** dello scheletro → estensione effettiva della delocalizzazione. +- Bandgap dei bottle brush in 0,929-1,521 eV: l'ingegnerizzazione con PCL «non compromette le spiccate potenzialità optoelettroniche». +- Il confronto con i lineari nel testo rimanda a «paragrafo XX (XX)», segnaposto non risolto ([[difetti-noti]]). + +## Collegamenti +- [[copolimeri-3a-3b-3c]] · [[bottle-brush-3-x]] · [[optoelettronica-oled-donatore-accettore]] · [[bottle-brush]] +- [[tesi]] · [[bibliografia]] diff --git a/wiki/techniques/dsc.md b/wiki/techniques/dsc.md new file mode 100644 index 0000000..591e803 --- /dev/null +++ b/wiki/techniques/dsc.md @@ -0,0 +1,31 @@ +--- +title: DSC - calorimetria differenziale a scansione +type: technique +tags: [dsc, tg, tm, tc, pcl] +created: 2026-10-09 +updated: 2026-10-09 +tesi_loc: "§3.1 r.583; §4.2 r.954; §4.3 r.1091-1097" +refs: [] +figures: ["fig-068"] +status: draft +--- + +# DSC - calorimetria differenziale a scansione + +## Strumento e programma (§3.1, r.583) +**TA Q2000**, atmosfera inerte di **azoto**. Due cicli di riscaldamento da **−50 °C a 250 °C** a **20 °C/min**, intervallati da un ciclo di raffreddamento da 250 °C a −50 °C a **−10 °C/min**. + +## Risultati +| Campioni | Risultato | Interpretazione della tesi | +|---|---|---| +| Copolimeri lineari [[copolimeri-3a-3b-3c]] (r.954) | Tg intorno a **−10 °C** per tutti; **nessuna transizione di fusione** (a differenza del 3HT) | copolimero **random**; elevato disordine impedisce la cristallizzazione nonostante i bassi pesi molecolari | +| Bottle brush [[bottle-brush-3-x]] (r.1091-1093) | **Tm 55-60 °C**, **Tc 25-35 °C**, pressoché costanti per tutti | transizioni dominate dai segmenti di caprolattone delle catene laterali; alta densità di grafting e PCL frazione preponderante → mobilità e propensione a cristallizzare dettano le proprietà termiche dell'intero materiale; influenza del backbone minimizzata, profili essenzialmente indipendenti dalle lievi variazioni strutturali | + +![[immagini/d2ed44d32060aa9ee04e73304940b111e53bf65cf115a93ace696933048e308b.jpg|560]] +*Figura 68 - esempio di termogramma dei polimeri bottle brush realizzati (in figura l'analisi del campione 3.1c)* · [[fig-068|nota figura]] + +Nota del catalogo su [[fig-068|Fig. 68]] (campione 3.1c): l'assegnazione dei picchi (~64 °C fusione, ~24 °C cristallizzazione) è dedotta da «Exo Down» e dal contesto, non da diciture in immagine. Le Conclusioni (r.1283) citano per i copolimeri lineari «temperature di fusione superiori a 110 °C», non coerenti con r.954 ([[difetti-noti]]); per i bottle brush le Conclusioni dicono «fase semicristallina dominante delle catene laterali di PCL» (r.1285). + +## Collegamenti +- [[copolimeri-3a-3b-3c]] · [[bottle-brush-3-x]] · [[rop-pcl]] +- [[tesi]] diff --git a/wiki/techniques/ft-ir.md b/wiki/techniques/ft-ir.md new file mode 100644 index 0000000..20a0b43 --- /dev/null +++ b/wiki/techniques/ft-ir.md @@ -0,0 +1,41 @@ +--- +title: FT-IR (ATR) +type: technique +tags: [ir, atr, caratterizzazione] +created: 2026-10-09 +updated: 2026-10-09 +tesi_loc: "§3.1 r.575; §4.1 r.800-802; §4.2 r.900-904; §4.3 r.1006-1010" +refs: [] +figures: ["fig-049", "fig-057", "fig-065", "fig-066"] +status: draft +--- + +# FT-IR (ATR) + +## Strumento (§3.1, r.575) +Spettroscopia infrarossa a **riflettanza totale attenuata** (ATR) con spettrofotometro **ATR-IR Bruker alpha I**. + +## Bande diagnostiche usate nella tesi +| Banda | Assegnazione | Campione | Pagina | +|---|---|---|---| +| 3400 / 3300-3400 cm⁻¹ (larga) | O-H terminale | [[dpp-2]], **3a-c** (più debole in 3a) | [[dpp-2]], [[copolimeri-3a-3b-3c]] | +| 3600-3200 cm⁻¹ | O-H del precursore; **assente** nei bottle brush | macroiniziatori vs bottle brush | [[bottle-brush-3-x]] | +| ~3100 cm⁻¹ | C-H aromatici tiofenici | [[dpp-2]] | [[dpp-2]] | +| 2930 e 2850 cm⁻¹ (~2920/~2850; 2950-2860) | stretching asimmetrico/simmetrico C-H alifatici | tutti | - | +| ~1650 cm⁻¹ | C=O dei lattami in sistemi coniugati, DPP | [[dpp-2]], **3a-c** | - | +| ~1720 cm⁻¹ | C=O estereo del PCL (stretto, intenso) | bottle brush | [[bottle-brush-3-x]] | +| 1500-1400 cm⁻¹ | C=C aromatici e del core | [[dpp-2]] | - | +| ~1050 cm⁻¹ | stretching C-O | **3a-c** | - | +| 1240-1160 cm⁻¹ | stretching C-O-C | bottle brush | - | +| ~820 cm⁻¹ | anello del 3-esiltiofene | **3a-c** | - | + +Dati IR della procedura per [[dpp-2]] (§3.2): 3350, 3070, 2920, 2850, 1645, 1555, 1495, 1440, 1390, 820, 730 cm⁻¹. + +## Figure +- [[fig-049|Fig. 49]]: spettro di [[dpp-2]]. +- [[fig-057|Fig. 57]]: copolimeri 3a, 3b, 3c (discordanza colori didascalia/testo). +- [[fig-065|Fig. 65]], [[fig-066|Fig. 66]]: serie bottle brush da 3b e da 3c, con il macroiniziatore in traccia di base. + +## Collegamenti +- [[nmr-1h]] · [[dpp-2]] · [[copolimeri-3a-3b-3c]] · [[bottle-brush-3-x]] +- [[tesi]] diff --git a/wiki/techniques/gpc.md b/wiki/techniques/gpc.md new file mode 100644 index 0000000..045518c --- /dev/null +++ b/wiki/techniques/gpc.md @@ -0,0 +1,40 @@ +--- +title: GPC - cromatografia a permeazione di gel +type: technique +tags: [gpc, peso-molecolare, polidispersità] +created: 2026-10-09 +updated: 2026-10-09 +tesi_loc: "§3.1 r.577; §4.2 r.938-952; §4.3 r.1045-1062" +refs: [54, 57] +figures: [] +status: draft +--- + +# GPC - cromatografia a permeazione di gel + +## Strumento e condizioni (§3.1, r.577) +- Colonna **5MXL da 300 mm**, range di Mw analizzabile **800-30000 Da**. +- Detector a **indice di rifrazione**. +- Campioni in **THF**; flusso **1 mL/min**; temperatura **20 °C**. +- Calibrazione con standard monodispersi di **polistirene**. + +## Copolimeri lineari (§4.2, r.938-952) +Dati: Tabella 8 in [[copolimeri-3a-3b-3c]]. Mn ≈ 1400-2150 Da; PD 1,979-4,592. PD ≈ 2 o superiori sono attesi in una polimerizzazione non controllata (distribuzione più probabile di Flory, rif. [[54-odian-2004|54]]). Il campione **3b** (Mn 1402; Mw 6439; PD 4,592) indica oligomeri a catena corta accanto a una frazione di peso più alto. + +## Bottle brush (§4.3, r.1045-1062) +Dati: Tabella 11 in [[bottle-brush-3-x]]. Scopo: valutare l'accrescimento delle catene e le dimensioni, e verificare a posteriori il grado di controllo della ROP rispetto ai target 1500, 5000, 10000 Da. + +**Interpretazione della tesi — sottostima dei pesi molecolari:** +- I valori GPC sono «significativamente sottostimati» rispetto ai teorici. +- La GPC separa per **volume idrodinamico** e dà valori relativi agli standard di calibrazione (qui polistirene lineare). +- A parità di peso molecolare un polimero **altamente ramificato** assume in soluzione una conformazione più compatta di un lineare, con volume idrodinamico nettamente inferiore: penetra di più nei pori della colonna ed eluisce agli stessi tempi di polimeri lineari molto più corti. +- La sottostima è **proporzionale all'ingombro delle catene laterali**: con innesti di PCL a basso peso (~1500 Da) l'approssimazione lineare è più attendibile e la GPC dà valori attorno a **12000 Da**. +- Con segmenti più lunghi (ad esempio stimando tre catene per lato, peso teorico atteso ~**62000 Da**) la compattazione porta a una sottostima del peso reale attorno al **70%** (rif. [[57-floyd-2021|57]]). +- Quindi i dati GPC non indicano il peso assoluto né una bassa resa, ma confermano indirettamente una **struttura ramificata altamente impaccata** e permettono un confronto diretto fra i polimeri. +- **Outlier 3.3c**: valore fuori andamento. Ipotesi della tesi: essendo il materiale di partenza random, possibili elevate concentrazioni locali di DPP e relativi ossidrili avrebbero ridotto la crescita delle catene laterali per ingombro sterico delle catene in crescita. Da indagare con ulteriori analisi. + +Per un confronto con la stima via ¹H-NMR: [[nmr-1h]] (Eq. 10) e Tabella 12 in [[bottle-brush-3-x]]. + +## Collegamenti +- [[copolimeri-3a-3b-3c]] · [[bottle-brush-3-x]] · [[nmr-1h]] +- [[tesi]] · [[bibliografia]] diff --git a/wiki/techniques/nmr-1h.md b/wiki/techniques/nmr-1h.md new file mode 100644 index 0000000..1767903 --- /dev/null +++ b/wiki/techniques/nmr-1h.md @@ -0,0 +1,61 @@ +--- +title: ¹H-NMR +type: technique +tags: [nmr, caratterizzazione, composizione, peso-molecolare] +created: 2026-10-09 +updated: 2026-10-09 +tesi_loc: "§3.1 r.573; §4.1 r.762-764, 796; §4.2 r.872-896; §4.3 r.1000-1004, 1064-1089" +refs: [] +figures: ["fig-044", "fig-048", "fig-054", "fig-055", "fig-056", "fig-064"] +status: draft +--- + +# ¹H-NMR + +## Strumento e condizioni (§3.1, r.573) +Spettri ¹H-NMR in soluzione con spettrometro **Varian Mercury 400 (400 MHz)**, **TMS** come standard interno. Solventi dei dati: d6-DMSO per [[dpp-1]]; CDCl3 per [[dpp-2]], copolimeri e bottle brush. + +## Dove sono i dati +| Campione | Spettro | Contenuto | Pagina | +|---|---|---|---| +| DPP **1** | [[fig-044\|Fig. 44]] (DMSO) | NH ~11 ppm; tiofene: dd, d, dd | [[dpp-1]] | +| DPP **2** | [[fig-048\|Fig. 48]] (CDCl3) | tiofene 8,9 / 7,6 / 7,3 ppm; NCH2 4,1; CH2OH 3,6; CH2 1-2 | [[dpp-2]] | +| Copolimeri **3a, 3b, 3c** | [[fig-054\|Fig. 54]], [[fig-055\|Fig. 55]], [[fig-056\|Fig. 56]] (CDCl3) | % DPP reale | [[copolimeri-3a-3b-3c]] | +| Bottle brush | [[fig-064\|Fig. 64]] (**3.1b**, rappresentativo) | segnali PCL; Mn via NMR | [[bottle-brush-3-x]] | + +## Composizione dei copolimeri: %DPP (§4.2, r.872-884) +Analisi quantitativa sull'integrazione di due segnali: +- protoni del **CH3** del 3-esiltiofene; +- protoni dei **CH2 adiacenti alle funzioni idrossiliche** del DPP. + +Le aree sono normalizzate per il numero di protoni magneticamente equivalenti. + +$$ +\%DPP=\frac{\frac{A_{DPP}}{n_{DPP}}}{\frac{A_{DPP}}{n_{DPP}}+\frac{A_{3HT}}{n_{3HT}}}\times 100 +$$ +**Equazione 9** - *calcolo della percentuale di DPP nei copolimeri dagli spettri ¹H-NMR* + +$A_{DPP}$, $A_{3HT}$ = aree integrate dei rispettivi segnali; $n_{DPP}$, $n_{3HT}$ = numero di protoni equivalenti che generano il segnale. Risultati: Tabella 6 in [[copolimeri-3a-3b-3c]] (25,2 / 32,6 / 35,3 %). + +## Verifica dell'innesto di PCL (§4.3, r.1000) +Segnali del PCL: tripletto a ~**4,0 ppm** (-CH2-O-) e segnale a **2,3 ppm** (protoni in α al carbonile). Spettri analoghi per tutti i campioni (cambia solo l'integrazione). + +## Peso molecolare dei bottle brush via ¹H-NMR (§4.3, r.1064-1089) +Usato per superare i limiti della GPC ([[gpc]]). Si basa sul grado di polimerizzazione delle singole catene laterali di PCL. + +$$ +MW_{tot}=MW_{backbone}+\left[\left(\frac{I_{4{,}05}}{I_{3{,}65}}\times MW_{CL}\right)\times \left(DP_{backbone}\times \chi _{DPP}\times 2\right)\right] +$$ +**Equazione 10** - *calcolo del peso molecolare dei polimeri bottle brush mediante ¹H-NMR* + +- $I_{4{,}05}$: area dei metileni interni alla catena (-CH2O-CO-, ~**4,05 ppm**). +- $I_{3{,}65}$: area dei metileni terminali adiacenti all'ossidrile (-CH2-OH, ~**3,65 ppm**), posta convenzionalmente pari a **1**. +- Il rapporto dà il numero di unità ripetenti per catena; $\times MW_{CL}$ (peso molecolare dell'unità ripetente del caprolattone) dà il peso molecolare della singola catena di PCL. +- Moltiplicato per il numero medio di siti di polimerizzazione per macromolecola, stimato da $DP_{backbone}$ (dalla GPC) e $\chi_{DPP}$ (rapporto molare 3HT/DPP via NMR), con **2 gruppi -OH di innesco per unità di DPP**. +- Si somma il $MW_{backbone}$ del copolimero lineare. + +Risultati (Tabella 12): in [[bottle-brush-3-x]]. + +## Collegamenti +- [[copolimeri-3a-3b-3c]] · [[bottle-brush-3-x]] · [[dpp-1]] · [[dpp-2]] · [[gpc]] · [[ft-ir]] +- [[tesi]] diff --git a/wiki/techniques/uv-vis-fluorescenza.md b/wiki/techniques/uv-vis-fluorescenza.md new file mode 100644 index 0000000..d122e2d --- /dev/null +++ b/wiki/techniques/uv-vis-fluorescenza.md @@ -0,0 +1,48 @@ +--- +title: UV-Vis e fluorescenza +type: technique +tags: [uv-vis, fluorescenza, emissione, stokes-shift, coefficiente-di-estinzione] +created: 2026-10-09 +updated: 2026-10-09 +tesi_loc: "§3.1 r.579-581; §4.1 r.768-823; §4.2 r.906-928; §4.3 r.1024-1043; §4.5 r.1266-1276" +refs: [51] +figures: ["fig-045", "fig-050", "fig-051", "fig-058", "fig-059", "fig-060", "fig-067", "fig-074"] +status: draft +--- + +# UV-Vis e fluorescenza + +## Strumenti (§3.1, r.579-581) +- **UV-Vis**: spettrofotometro a doppio raggio **Agilent Cary 3500 UV-Vis**; spettro da **800 a 200 nm**; cuvette di quarzo con cammino ottico di **1 cm**. +- **Fluorescenza**: spettrometro **Agilent Cary Eclipse**; sorgente lampada allo **xenon (80 Hz)**; detector fotomoltiplicatore **PMT 900**. +- Solvente delle misure di soluzione: **THF** (per ε di **2**: CHCl3). + +## Riepilogo dei dati in soluzione (da tabelle della tesi) +| Campione | λmax,abs (nm) | λmax,em/ex (nm) | Stokes shift (nm) | Fonte | +|---|---|---|---|---| +| [[dpp-1]] | 531 | 542 | 11 | Tab. 5 | +| [[dpp-2]] | 541 | 555 | 14 | Tab. 5 | +| 3a | 540 | 547 | 7 | Tab. 7 | +| 3b | 544 | 550 | 6 | Tab. 7 | +| 3c | 542 | 552 | 10 | Tab. 7 | +| 3.1b | 554 | 562 | 8 | Tab. 10 | +| 3.2b | 550 | 564 | 14 | Tab. 10 | +| 3.3b | 553 | 563 | 10 | Tab. 10 | +| 3.1c | 547 | 561 | 14 | Tab. 10 | +| 3.2c | 544 | 557 | 13 | Tab. 10 | +| 3.3c | 553 | 564 | 11 | Tab. 10 | + +Questi valori derivano da tabelle diverse della tesi; nel testo delle procedure (§3.2) i valori per 1 e 2 differiscono ([[difetti-noti]]). Commenti e figure: nelle pagine dei composti ([[dpp-1]], [[dpp-2]], [[copolimeri-3a-3b-3c]], [[bottle-brush-3-x]]). + +Valori delle procedure §3.2 (verbatim): **1**: UV-Vis (THF) 532 nm, 498 nm; fluorescenza (THF) 490 nm. **2**: UV-Vis (THF) 541 nm; fluorescenza (THF) 540 nm. + +## Coefficienti di estinzione molare ε +- **1**: 28000 M⁻¹ cm⁻¹ (dal rif. [[51-wang-2022|51]]). +- **2**: 13218 M⁻¹ cm⁻¹ da retta di calibrazione (assorbanza vs concentrazione, CHCl3), pendenza = ε per Lambert-Beer ([[fig-051|Fig. 51]]). + +## Stato solido +Spettri di assorbimento ed emissione di 3.2b in soluzione e in film ([[fig-074|Fig. 74]]): [[acq-e-stato-solido]]. + +## Collegamenti +- [[fluorescenza]] · [[acq-e-stato-solido]] · [[dpp-1]] · [[dpp-2]] · [[copolimeri-3a-3b-3c]] · [[bottle-brush-3-x]] +- [[tesi]] diff --git a/wiki/tesi.md b/wiki/tesi.md index 122b5d3..9803a95 100644 --- a/wiki/tesi.md +++ b/wiki/tesi.md @@ -10,16 +10,49 @@ status: draft # Tesi - mappa -Sintesi e caratterizzazione di copolimeri bottle brush foto-elettro attivi (Aurora Luzi, rel. Stefano Scurti, a.a. 2025-2026). Sorgente: `raw/tesi.md`. +Sintesi e caratterizzazione di copolimeri bottle brush foto-elettro attivi. Candidata: Aurora Luzi. Relatore: Dr. Stefano Scurti. Correlatori: Prof. Massimiliano Lanzi, Dr. Simone Gabellini, Dr. Riccardo Medri. Dipartimento di Chimica Industriale "Toso Montanari", Corso di Laurea Magistrale in Chimica Industriale (Classe LM-71), a.a. 2025-2026 (r.1-11). Sorgente: `raw/tesi.md` (1411 righe): Riassunto (r.13), Abstract (r.25), Sommario (r.35), cap. 1 (r.66), 2 (r.545), 3 (r.562), 4 (r.717), 5 (r.1279), Bibliografia (r.1293). -| Capitolo | Riga | Sezioni | Pagine wiki | -|---|---|---|---| -| 1 Introduzione | 66 | 1.1 Dichetopirrolopirroli (69), 1.2 Fluorescenza (376), 1.3 Fluorofori in materiali polimerici (479), 1.4 Applicazioni (502) | da fare | -| 2 Scopo | 545 | - | da fare | -| 3 Procedure sperimentali | 562 | 3.1 Materiali e metodi (565), 3.2 Sintesi e procedure (586), 3.3 Principi teorici della ciclovoltammetria (666), 3.4 Procedure voltammetriche (702) | da fare | -| 4 Discussione dei risultati | 717 | 4.1 DPP (722), 4.2 Copolimeri coniugati (826), 4.3 Bottle brush (957), 4.4 Ciclovoltammetrie (1100), 4.5 Caratterizzazione spettroscopica allo stato solido (1254) | da fare | -| 5 Conclusioni | 1279 | - | da fare | +## Come è organizzata la wiki +Il contenuto della tesi è riorganizzato per argomento, non per capitolo. Ogni dato sta in una sola pagina (la pagina dove la tesi lo discute), le altre rimandano. +- **Concetti**: [[bottle-brush]] (hub), [[acq-e-stato-solido]], [[dpp-struttura-e-proprieta]], [[dpp-sintesi-letteratura]], [[dpp-reattivita]], [[fluorescenza]], [[fluorofori-in-polimeri]], [[optoelettronica-oled-donatore-accettore]], [[polimerizzazione-ossidativa-fecl3]], [[rop-pcl]] +- **Composti**: [[dpp-1]], [[dpp-2]], [[copolimeri-3a-3b-3c]], [[bottle-brush-3-x]], [[reagenti-e-materiali]] +- **Tecniche**: [[nmr-1h]], [[ft-ir]], [[gpc]], [[uv-vis-fluorescenza]], [[dsc]], [[ciclovoltammetria]] +- **Altro**: [[overview]], [[bibliografia]], [[difetti-noti]], le note delle 78 figure in `wiki/figures/` (generate da `raw/immagini.json`) + +## Mappa sezioni → pagine → figure +Figure: numero della tesi con link alla nota (`fig-NNN`); «schema» = i 4 file senza numero stampato (schemi di reazione del cap. 3). + +| § | Titolo | Riga | Pagine wiki | Figure | +| --- | --- | --- | --- | --- | +| 1 | Introduzione | r.66 | - | - | +| 1.1 | Dichetopirrolopirroli | r.69 | [[dpp-struttura-e-proprieta]] | [[fig-001|1]] | +| 1.1.1 | Storia e sintesi | r.84 | [[dpp-sintesi-letteratura]] | [[fig-002|2]], [[fig-003|3]], [[fig-004|4]], [[fig-005|5]], [[fig-006|6]], [[fig-007|7]], [[fig-008|8]], [[fig-009|9]], [[fig-010|10]], [[fig-011|11]], [[fig-012|12]], [[fig-013|13]], [[fig-014|14]] | +| 1.1.2 | Struttura e reattività | r.203 | [[dpp-struttura-e-proprieta]] (struttura), [[dpp-reattivita]] (reattività), [[polimerizzazione-ossidativa-fecl3]] | [[fig-015|15]], [[fig-016|16]], [[fig-017|17]], [[fig-018|18]], [[fig-019|19]], [[fig-020|20]], [[fig-021|21]], [[fig-022|22]], [[fig-023|23]], [[fig-024|24]], [[fig-025|25]], [[fig-026|26]], [[fig-027|27]], [[fig-028|28]], [[fig-029|29]], [[fig-030|30]] | +| 1.2 | Fluorescenza | r.376 | [[fluorescenza]] | [[fig-031|31]], [[fig-032|32]], [[fig-033|33]] | +| 1.2.1 | Shift di Stokes | r.418 | [[fluorescenza]] | [[fig-034|34]] | +| 1.2.2 | Resa quantica | r.429 | [[fluorescenza]] | - | +| 1.2.3 | Tempi di vita | r.450 | [[fluorescenza]] | - | +| 1.3 | Utilizzo di fluorofori in materiali polimerici | r.479 | [[fluorofori-in-polimeri]] | [[fig-035|35]] | +| 1.4 | Applicazioni | r.502 | [[optoelettronica-oled-donatore-accettore]] | [[fig-036|36]], [[fig-037|37]], [[fig-038|38]] | +| 2 | Scopo | r.545 | [[bottle-brush]], [[acq-e-stato-solido]], [[optoelettronica-oled-donatore-accettore]] | - | +| 3 | Procedure sperimentali | r.562 | - | - | +| 3.1 | Materiali e metodi | r.565 | [[reagenti-e-materiali]], [[nmr-1h]], [[ft-ir]], [[gpc]], [[uv-vis-fluorescenza]], [[dsc]] | - | +| 3.2 | Sintesi e procedure | r.586 | [[dpp-1]], [[dpp-2]], [[copolimeri-3a-3b-3c]], [[bottle-brush-3-x]] | [[fig-x-185efd|schema]], [[fig-x-f6eeb1|schema]], [[fig-x-cc3f54|schema]], [[fig-x-136800|schema]] | +| 3.3 | Principi teorici della ciclovoltammetria | r.666 | [[ciclovoltammetria]] | - | +| 3.4 | Procedure sperimentali delle analisi voltammetriche | r.702 | [[ciclovoltammetria]] | [[fig-039|39]] | +| 4 | Discussione dei risultati | r.717 | - | - | +| 4.1 | Dichetopirrolopirroli | r.722 | [[dpp-1]], [[dpp-2]], [[dpp-struttura-e-proprieta]] | [[fig-040|40]], [[fig-041|41]], [[fig-042|42]], [[fig-043|43]], [[fig-044|44]], [[fig-045|45]], [[fig-046|46]], [[fig-047|47]], [[fig-048|48]], [[fig-049|49]], [[fig-050|50]], [[fig-051|51]] | +| 4.2 | Copolimeri coniugati | r.826 | [[copolimeri-3a-3b-3c]], [[polimerizzazione-ossidativa-fecl3]], [[gpc]], [[dsc]] | [[fig-052|52]], [[fig-053|53]], [[fig-054|54]], [[fig-055|55]], [[fig-056|56]], [[fig-057|57]], [[fig-058|58]], [[fig-059|59]], [[fig-060|60]], [[fig-061|61]] | +| 4.3 | Polimeri bottle brush | r.957 | [[bottle-brush-3-x]], [[rop-pcl]], [[bottle-brush]] | [[fig-062|62]], [[fig-063|63]], [[fig-064|64]], [[fig-065|65]], [[fig-066|66]], [[fig-067|67]], [[fig-068|68]] | +| 4.4 | Ciclovoltammetrie | r.1100 | [[ciclovoltammetria]] | - | +| 4.4.1 | Ciclovoltammetrie su polimeri elettroattivi | r.1107 | [[ciclovoltammetria]] | - | +| 4.4.2 | Metodologie di analisi voltammetrica | r.1118 | [[ciclovoltammetria]] | [[fig-069|69]], [[fig-070|70]] | +| 4.4.3 | Proprietà elettrochimiche dei copolimeri lienari | r.1175 | [[ciclovoltammetria]] | [[fig-071|71]], [[fig-072|72]], [[fig-073|73]] | +| 4.4.4 | Effetto del design bottle brush | r.1230 | [[ciclovoltammetria]] | - | +| 4.5 | Caratterizzazione spettroscopica allo stato solido | r.1254 | [[acq-e-stato-solido]] | [[fig-074|74]] | +| 5 | Conclusioni | r.1279 | [[overview]], [[bottle-brush]] | - | + +Riassunto, Abstract (r.13-33) e Conclusioni (§5, r.1279-1291) sono sintetizzati in [[overview]]; la bibliografia è in [[bibliografia]]. ## Collegamenti -- [[overview]] -- [[index]] +- [[overview]] · [[index]] From 57ea4d74fef1bfa1835ad287c877e30254a59d0e Mon Sep 17 00:00:00 2001 From: Davide Grilli Date: Fri, 9 Oct 2026 19:30:30 +0200 Subject: [PATCH 3/5] Spezza la pagina CV, aggiunge indice dati e lint, applica correzioni meccaniche - Divide ciclovoltammetria in metodo + cv-risultati-copolimeri + cv-risultati-bottle-brush e ripunta i link - Aggiunge wiki/dati.md (grandezza -> pagina) e scripts/lint.py - Corregge spaziatura delle tabelle e coerenza figures/refs nel frontmatter; link alle schede in difetti-noti - Aggiorna CLAUDE.md, index.md e log.md Co-Authored-By: Claude Sonnet 5.5 --- .obsidian/graph.json | 2 +- CLAUDE.md | 5 +- index.md | 7 +- log.md | 10 +++ scripts/lint.py | 89 +++++++++++++++++++ wiki/analyses/difetti-noti.md | 14 +-- wiki/compounds/bottle-brush-3-x.md | 12 ++- wiki/compounds/copolimeri-3a-3b-3c.md | 12 ++- wiki/compounds/dpp-1.md | 1 + wiki/compounds/dpp-2.md | 2 + wiki/compounds/reagenti-e-materiali.md | 1 + wiki/concepts/bottle-brush.md | 4 +- wiki/concepts/dpp-reattivita.md | 3 +- wiki/concepts/dpp-sintesi-letteratura.md | 2 + wiki/concepts/dpp-struttura-e-proprieta.md | 2 +- ...optoelettronica-oled-donatore-accettore.md | 2 +- .../polimerizzazione-ossidativa-fecl3.md | 1 + wiki/dati.md | 81 +++++++++++++++++ wiki/overview.md | 3 +- wiki/techniques/ciclovoltammetria.md | 63 +------------ wiki/techniques/cv-risultati-bottle-brush.md | 35 ++++++++ wiki/techniques/cv-risultati-copolimeri.md | 58 ++++++++++++ wiki/techniques/dsc.md | 1 + wiki/techniques/ft-ir.md | 1 + wiki/techniques/nmr-1h.md | 1 + wiki/techniques/uv-vis-fluorescenza.md | 3 +- wiki/tesi.md | 6 +- 27 files changed, 335 insertions(+), 86 deletions(-) create mode 100644 scripts/lint.py create mode 100644 wiki/dati.md create mode 100644 wiki/techniques/cv-risultati-bottle-brush.md create mode 100644 wiki/techniques/cv-risultati-copolimeri.md diff --git a/.obsidian/graph.json b/.obsidian/graph.json index be925e9..83ecb44 100644 --- a/.obsidian/graph.json +++ b/.obsidian/graph.json @@ -17,6 +17,6 @@ "repelStrength": 10, "linkStrength": 1, "linkDistance": 250, - "scale": 0.25883865621816243, + "scale": 0.2588386562181621, "close": true } \ No newline at end of file diff --git a/CLAUDE.md b/CLAUDE.md index 7803cc9..d75b358 100644 --- a/CLAUDE.md +++ b/CLAUDE.md @@ -33,9 +33,11 @@ CLAUDE.md index.md log.md raw/ immutabile (vedi sopra) scripts/gen_figures.py genera wiki/figures/ da raw/immagini.json scripts/gen_bibliografia.py genera wiki/bibliografia.md da raw/bibliografia.json +scripts/lint.py controlli meccanici (link, orfane, frontmatter, numeri non in tesi.md) wiki/ overview.md sintesi evolutiva, research question, risultati tesi.md mappa capitolo/sezione → pagine wiki (unica pagina "source" della tesi) + dati.md indice «grandezza → pagina» con intervalli di valori (aggiornarlo a ogni nuova tabella) bibliografia.md i 59 riferimenti (GENERATA dallo script), con link alle schede raw/fonti/ concepts/ meccanismi, ROP, ACQ, bottle brush, π-stacking, ciclovoltammetria… compounds/ un file per composto numerato (composto-32.md) o polimero/campione @@ -79,6 +81,7 @@ status: draft | stable - `compounds` nel catalogo sono numeri della tesi; `concepts` sono slug candidati, non nomi definitivi: crea la pagina solo se la regola dei ≥2 usi è soddisfatta. ## Regole di organizzazione dei dati +- Pagine sopra ~1.500 parole vanno spezzate per argomento (es. `ciclovoltammetria` = metodo; i risultati in `cv-risultati-*`). - Una tabella o un dato sta in **una sola pagina**: quella dove la tesi lo discute (per es. Tab. 5 in `dpp-2`, Tab. 13-14 in `ciclovoltammetria`). Le altre pagine rimandano con wikilink; fanno eccezione i riepiloghi comparativi (es. in `uv-vis-fluorescenza`), che citano la tabella di origine. - Le pagine riorganizzano per argomento, non per capitolo, senza eliminare informazioni: procedure con quantità in tabella, condizioni, assegnazioni e ragionamenti della tesi restano, con `tesi_loc` e righe. - Composti sperimentali: `dpp-1`, `dpp-2`, `copolimeri-3a-3b-3c`, `bottle-brush-3-x`. La numerazione dei composti del cap. 1 (1-48) è un'altra: non confonderle. @@ -101,7 +104,7 @@ Ordine: Abstract/Introduzione/Scopo (concepts, research question) → Procedure Leggi `index.md` e le pagine rilevanti (non rileggere `raw/` se la wiki basta); rispondi in italiano con citazioni `[[...]]` e `tesi_loc`; proponi di salvare in `analyses/` le risposte durevoli; log `query`. ### Lint (su richiesta o ogni ~10 ingest) -Contraddizioni, pagine orfane, concetti citati senza pagina, link rotti, frontmatter mancante, valori che non tornano con `raw/tesi.md`. Riporta, correggi dopo conferma. Log `lint`. +Esegui `python scripts/lint.py` (link rotti, pagine orfane, frontmatter, coerenza `figures`/`refs` con il corpo, numeri non presenti in `raw/tesi.md`, slug concetto candidati). Poi controlli semantici a mano: contraddizioni, valori che non tornano con `raw/tesi.md`, pagine oltre ~1.500 parole da spezzare. Riporta; le correzioni meccaniche (spaziatura, frontmatter) si applicano subito, il resto dopo conferma. Log `lint`. ## index.md e log.md - `index.md`: catalogo per categoria (Overview, Tesi e bibliografia, Concetti, Composti, Tecniche, Figure, Analisi), voci `- [[pagina]] — riga di sintesi`, ordine alfabetico, conteggi aggiornati. Le 78 figure non si elencano una per una: una riga con link alla cartella e il conteggio per tipo. diff --git a/index.md b/index.md index e3707b4..c72ac41 100644 --- a/index.md +++ b/index.md @@ -1,11 +1,12 @@ # Indice della wiki -_Catalogo di tutte le pagine. Aggiornato a ogni ingest/query. Pagine curate: 25 · Figure generate: 78 · Fonti ingerite: 1 (la tesi)_ +_Catalogo di tutte le pagine. Aggiornato a ogni ingest/query. Pagine curate: 28 · Figure generate: 78 · Fonti ingerite: 1 (la tesi)_ ## Overview - [[overview]] — problema, strategia, risultati dichiarati e limiti della tesi ## Tesi e bibliografia +- [[dati]] — indice «grandezza → pagina» con intervalli di valori - [[bibliografia]] — i 59 riferimenti con link alle schede in `raw/fonti/` (generata) - [[tesi]] — mappa sezione → pagine wiki → figure @@ -29,7 +30,9 @@ _Catalogo di tutte le pagine. Aggiornato a ogni ingest/query. Pagine curate: 25 - [[reagenti-e-materiali]] — reagenti per passaggio e trattamento dei solventi ## Tecniche -- [[ciclovoltammetria]] — teoria (Eq. 6-8), procedura, metodo (Eq. 11-12), Tab. 13-14 +- [[ciclovoltammetria]] — teoria (Eq. 6-8), procedura, metodo di analisi (Eq. 11-12) +- [[cv-risultati-bottle-brush]] — Tab. 14, bandgap 0,929-1,521 eV +- [[cv-risultati-copolimeri]] — Tab. 13, correlazione bandgap/% DPP, confronto con P3HT - [[dsc]] — programma termico e risultati - [[ft-ir]] — bande diagnostiche - [[gpc]] — condizioni e interpretazione della sottostima diff --git a/log.md b/log.md index e3a904a..2d6c897 100644 --- a/log.md +++ b/log.md @@ -29,3 +29,13 @@ _Append-only. Formato: `## [YYYY-MM-DD] tipo | titolo`_ ## [2026-10-09] schema | Regole di organizzazione dati e script bibliografia - CLAUDE.md: una tabella in una sola pagina; script `gen_bibliografia.py`; `bibliografia.md` derivata +## [2026-10-09] lint | Primo lint dopo l'ingest della tesi +- Esito `scripts/lint.py`: 0 link/embed rotti, 0 pagine orfane; numeri nelle pagine tutti presenti in `raw/tesi.md` (eccetto valori calcolati o in LaTeX in `difetti-noti`: 4,8006; 1,373; 0,9719 è in `raw/tesi.md` come `0{,}9719`) +- Corretto (meccanico): 33 tabelle senza riga vuota prima; incoerenze `figures`/`refs` nel frontmatter in 8 pagine; link alle schede nelle voci della tabella bibliografia di `difetti-noti` +- Nessuna pagina concetto nuova: gli slug del catalogo usati da >=2 figure sono già coperti dalle pagine esistenti (reformatskij, n-alchilazione, cross-coupling, ecc.) +- Controlli semantici: righe `tesi_loc` a campione coerenti; riepilogo ottico e `dati.md` verificati contro le tabelle + +## [2026-10-09] schema | Spezzata ciclovoltammetria, aggiunto dati.md e scripts/lint.py +- `ciclovoltammetria` (2.065 parole) -> `ciclovoltammetria` (teoria, procedura, metodo) + `cv-risultati-copolimeri` (Tab. 13) + `cv-risultati-bottle-brush` (Tab. 14) +- `wiki/dati.md`: indice grandezza -> pagina; regola: pagine > ~1.500 parole si spezzano; lint con `scripts/lint.py` + diff --git a/scripts/lint.py b/scripts/lint.py new file mode 100644 index 0000000..3d79af5 --- /dev/null +++ b/scripts/lint.py @@ -0,0 +1,89 @@ +"""Controlli meccanici della wiki (vedi CLAUDE.md, sezione Lint). Uso: python scripts/lint.py +Stampa solo segnalazioni; non modifica nulla. Le verifiche semantiche (contraddizioni, valori) restano all'LLM.""" +import json +import re +from collections import Counter +from pathlib import Path + +root = Path(__file__).resolve().parent.parent +BS = "\\" +pages = [p for p in root.glob("wiki/**/*.md") if "figures" not in p.parts and p.name != "bibliografia.md"] +allp = list(root.glob("wiki/**/*.md")) + [root / "index.md"] +stems = {p.stem for p in root.glob("wiki/**/*.md")} | {p.stem for p in root.glob("raw/fonti/*.md")} | {"index", "log", "CLAUDE"} +imgs = {p.name for p in root.glob("raw/immagini/*")} +tesi = (root / "raw/tesi.md").read_text(encoding="utf8") +n_lines = len(tesi.split("\n")) +LINK = re.compile(r"(!?)\[\[([^\]]+)\]\]") +FIG = re.compile(r"\[\[(fig-[\w-]+)(?:\||\]|\\)") +REF = re.compile(r"\[\[(\d\d)-[\w-]+(?:\||\\)") + +# 1 link rotti, embed mancanti, pagine orfane +bad, inbound = [], Counter() +for p in allp: + for m in LINK.finditer(p.read_text(encoding="utf8")): + tg = m.group(2).split("|")[0].split("#")[0].replace(BS, "") + if m.group(1): + if Path(tg).name not in imgs: + bad.append((p.name, tg)) + elif tg not in stems: + bad.append((p.name, tg)) + else: + inbound[tg] += 1 +print("1 link/embed rotti:", bad or "nessuno") +print("1 pagine orfane:", [s for s in stems if not inbound[s] and s not in ("CLAUDE", "log") and not s[:2].isdigit()] or "nessuna") + +for p in pages: + t = p.read_text(encoding="utf8") + m = re.match(r"---\n(.*?)\n---\n(.*)", t, re.S) + if not m: + print("2 frontmatter assente:", p.name) + continue + fm, body = m.groups() + # 2 chiavi obbligatorie + miss = [k for k in ("title", "type", "tags", "created", "updated", "tesi_loc", "status") if not re.search(rf"^{k}:", fm, re.M)] + if miss: + print("2 chiavi mancanti:", p.name, miss) + # 3 figure e riferimenti del frontmatter coerenti con il corpo + fmf, bf = set(re.findall(r'"(fig-[\w-]+)"', fm)), set(FIG.findall(body)) + if re.search(r"^figures:", fm, re.M) and fmf != bf: + print("3 figure fm/corpo:", p.name, "solo fm", sorted(fmf - bf), "solo corpo", sorted(bf - fmf)) + r = re.search(r"^refs: \[(.*?)\]", fm, re.M) + fr = {int(x) for x in re.findall(r"\d+", r.group(1))} if r else set() + br = {int(x) for x in REF.findall(body)} + if r and fr != br: + print("3 refs fm/corpo:", p.name, "solo fm", sorted(fr - br), "solo corpo", sorted(br - fr)) + # 4 tesi_loc entro il file + loc = re.search(r'tesi_loc: "(.*?)"', fm) + for a, b in re.findall(r"r\.(\d+)(?:-(\d+))?", loc.group(1) if loc else ""): + if max(int(a), int(b or 0)) > n_lines: + print("4 riga oltre la fine di tesi.md:", p.name, a, b) + +# 5 numero del riferimento coerente con il nome della scheda +for p in allp: + for m in re.finditer(r"\[\[(\d\d)-[\w-]+\\?\|(\d+)\]\]", p.read_text(encoding="utf8")): + if int(m.group(1)) != int(m.group(2)): + print("5 riferimento incoerente:", p.name, m.group(0)) + +# 6 tabelle senza riga vuota prima +for p in allp: + L = p.read_text(encoding="utf8").split("\n") + for i, l in enumerate(L): + if l.startswith("|") and i and L[i - 1].strip() and not L[i - 1].startswith("|"): + print("6 tabella senza riga vuota prima:", p.name, i + 1) + +# 7 numeri nelle pagine che non compaiono in tesi.md (da rivedere a mano: molti sono legittimi, es. conversioni) +tn = set(re.findall(r"\d+(?:[.,]\d+)?", tesi)) +for p in pages: + body = re.sub(r"^---\n.*?\n---\n", "", p.read_text(encoding="utf8"), flags=re.S) + for pat in (r"!?\[\[[^\]]*\]\]", r"\br\.\d+(?:-\d+)?(?:, ?\d+)*", r"§[\d.]+", + r"[Ff]ig(?:ura|\.)? ?\d+|Tab(?:ella|\.)? ?\d+|Eq(?:uazione|\.)? ?\d+|rif\. [\d,]+", r".*?"): + body = re.sub(pat, "", body) + nums = set(re.findall(r"(?=2 figure (candidati a pagina concetto) +cat = json.loads((root / "raw/immagini.json").read_text(encoding="utf8")) +c = Counter(x for f in cat["figures"] for x in f.get("concepts", [])) +print("8 slug in >=2 figure:", [(k, v) for k, v in c.most_common() if v >= 2]) diff --git a/wiki/analyses/difetti-noti.md b/wiki/analyses/difetti-noti.md index 7454b57..e2152f7 100644 --- a/wiki/analyses/difetti-noti.md +++ b/wiki/analyses/difetti-noti.md @@ -6,7 +6,7 @@ created: 2026-10-09 updated: 2026-10-09 tesi_loc: "varie (indicate per voce)" refs: [1, 20, 22, 36, 44, 47, 48, 49, 53] -figures: ["fig-004", "fig-009", "fig-010", "fig-026", "fig-027", "fig-029", "fig-033", "fig-034", "fig-049", "fig-057", "fig-061", "fig-062", "fig-065", "fig-066", "fig-068", "fig-x-cc3f54", "fig-x-136800"] +figures: ["fig-004", "fig-005", "fig-009", "fig-010", "fig-026", "fig-027", "fig-029", "fig-033", "fig-034", "fig-044", "fig-049", "fig-057", "fig-061", "fig-062", "fig-065", "fig-066", "fig-068", "fig-x-cc3f54", "fig-x-136800"] status: draft --- @@ -15,12 +15,13 @@ status: draft Pagina unica: le altre pagine rimandano qui. Regola: **segnalare, non correggere**. Sezioni A-D = difetti già noti (CLAUDE.md, catalogo immagini); sezione E = incoerenze rilevate durante questo ingest, confrontando testo, tabelle e conclusioni di `raw/tesi.md` (le righe sono di quel file). Dove indicato, è stato fatto un controllo aritmetico o sul PDF originale. ## A. Bibliografia (da `raw/bibliografia.json`, `raw/fonti/`) + | Voce | Problema | Stato | |---|---|---| -| 44 | duplica la voce 1 (Bao 2020, Front. Chem.) | `duplicate_entry` | -| 20 (Lenz), 22 (Zambounis & Iqbal), 36 (Stokes), 53 (Paganin, Bizzarri, Lanzi) | incomplete già nel testo originale (`incomplete_in_source`) | 20 e 36 identificate; 22 candidata; 53 non risolta | -| 47 (Li, 2014), 49 (Hendriks, 2013) | DOI errati/non registrati; voci non identificabili | `non_risolta` | -| 48 (Kroon, 2008) | DOI errato; il DOI corretto è **10.1080/15583720802231833** | `verificata_con_correzioni` | +| [[44-bao-2020\|44]] | duplica la voce [[01-bao-2020\|1]] (Bao 2020, Front. Chem.) | `duplicate_entry` | +| [[20-lenz-2002\|20]] (Lenz), [[22-zambounis-nd\|22]] (Zambounis & Iqbal), [[36-stokes-1852\|36]] (Stokes), [[53-paganin-nd\|53]] (Paganin, Bizzarri, Lanzi) | incomplete già nel testo originale (`incomplete_in_source`) | 20 e 36 identificate; 22 candidata; 53 non risolta | +| [[47-li-2014\|47]] (Li, 2014), [[49-hendriks-2013\|49]] (Hendriks, 2013) | DOI errati/non registrati; voci non identificabili | `non_risolta` | +| [[48-kroon-2008\|48]] (Kroon, 2008) | DOI errato; il DOI corretto è **10.1080/15583720802231833** | `verificata_con_correzioni` | Schede in `raw/fonti/`. La voce 53 è citata a r.840 per il meccanismo di trasferimento mono-elettronico (SET) nella polimerizzazione ossidativa ([[53-paganin-nd|53]]); la sua scheda la dà come non risolta (senza anno, rivista o DOI). @@ -31,6 +32,7 @@ Schede in `raw/fonti/`. La voce 53 è citata a r.840 per il meccanismo di trasfe - §1.1.2, r.235: «...qualsiasi modifica strutturale si traduce, in Il comportamento allo stato solido appare, invece, ...». La frase è interrotta anche nel testo di `tesi.pdf` (controllato nella versione in cronologia git): non è un errore di estrazione. [[dpp-struttura-e-proprieta]]. ## D. Discrepanze figura/testo (dal catalogo `raw/immagini.json`) + | Figura | Nota | |---|---| | [[fig-026\|Fig. 26]] | Didascalia («DPP di-bromurati con diversi areni») non coincide col testo, che cita i prodotti 38(a-h) della Figura 25; l'immagine mostra l'arilazione di 32 e 37 con tiofeni sostituiti | @@ -55,7 +57,7 @@ Anche: la didascalia di [[fig-004|Fig. 4]] dice «sale di zinco derivato dall'in 3. **Dati ottici di [[dpp-2]].** §3.2 (r.624-626): UV-Vis 541 nm, fluorescenza **540 nm**. Tabella 5: λabs 541, λex **555**, Stokes 14. Inoltre il testo (r.810) dice «Stokes shift ... simile per entrambi i fluorofori e vale circa 14 nm», mentre la tabella dà 11 nm per 1 e 14 nm per 2. 4. **Integrazioni ¹H-NMR in §3.2.** Per **1** (r.602): 4H + 4H + 4H = 12H, mentre il DPP 1 ha 6 H tiofenici (più 2 NH, non riportati nella lista). Per **2** (r.620): aromatici 1H + 1H + 2H = 4H, mentre i tiofeni sono 6 H. _(verifica sulla struttura; i dati originali non sono disponibili in `raw/`)_ 5. **Fusione dei copolimeri lineari.** §4.2 (r.954): DSC senza transizioni di fusione, Tg ≈ −10 °C. Conclusioni (r.1283): «transizioni vetrose intorno a −10 °C e temperature di fusione superiori a 110 °C». Vedi [[dsc]]. -6. **Bandgap nelle Conclusioni.** r.1289: correlazione lineare con R² = 0,9719 «tra la percentuale reale di DPP ... e l'allargamento del bandgap (da 3,42 eV a oltre 4,30 eV)». Tabella 13 ([[ciclovoltammetria]]): 0,970 / 1,316 / 1,371 eV. R² non compare altrove nel testo. +6. **Bandgap nelle Conclusioni.** r.1289: correlazione lineare con R² = 0,9719 «tra la percentuale reale di DPP ... e l'allargamento del bandgap (da 3,42 eV a oltre 4,30 eV)». Tabella 13 ([[cv-risultati-copolimeri]]): 0,970 / 1,316 / 1,371 eV. R² non compare altrove nel testo. 7. **Pesi molecolari via ¹H-NMR (Tab. 12).** Il testo (r.1078) li definisce «molto più vicini ai valori teorici» rispetto alla GPC, ma 3.3b = 88000 Da vs 34500 teorico (≈2,5×), 3.1c = 18200 vs 10000, 3.3c = 41300 vs 55000 (inferiore al teorico). Vedi [[bottle-brush-3-x]]. 8. **Aritmetica CV.** Le Tabelle 13 e 14 sono state ricalcolate con le Eq. 11-12 (HOMO = −(Eonsetox + 4,8), LUMO = −(Eonsetred + 4,8), Eg = LUMO − HOMO): tutte le righe tornano entro l'arrotondamento, **tranne 3c** (Tab. 13), dove Eonsetox = 0,0006 V darebbe HOMO ≈ −4,8006 eV (tabella: −4,799) e Eg ≈ 1,373 eV (tabella: 1,371). Differenza di pochi millielettronvolt. _(controllo eseguito in questo ingest)_ 9. **Tabelle UV.** Gli Stokes shift delle Tabelle 7 e 10 coincidono con la differenza λex − λabs (controllato). diff --git a/wiki/compounds/bottle-brush-3-x.md b/wiki/compounds/bottle-brush-3-x.md index 28d10a6..036a377 100644 --- a/wiki/compounds/bottle-brush-3-x.md +++ b/wiki/compounds/bottle-brush-3-x.md @@ -6,8 +6,8 @@ tags: [bottle-brush, pcl, rop, serie-b, serie-c] created: 2026-10-09 updated: 2026-10-09 tesi_loc: "§3.2 r.646-663; §4.3 r.957-1097; §4.4.4 r.1230-1251; §4.5 r.1254-1276" -refs: [55, 56, 57] -figures: ["fig-x-136800", "fig-062", "fig-063", "fig-064", "fig-065", "fig-066", "fig-067", "fig-068"] +refs: [] +figures: ["fig-x-136800", "fig-064", "fig-065", "fig-066", "fig-067", "fig-068"] status: draft --- @@ -24,6 +24,7 @@ Sei polimeri in due serie, ottenuti per [[rop-pcl]] dai macroiniziatori **3b** e La quantità di ε-caprolattone è fissata in base agli equivalenti di gruppi -OH del derivato DPP, considerati iniziatori attivi per la ROP. **Tabella 4** - *composizione dei polimeri bottle brush* + | Copolimero | Mn teorico | Caprolattone V (ml) | Caprolattone mol | | --- | --- | --- | --- | | 3b | 1500 Da (**3.1b**) | 1,06 | 0,01 | @@ -83,6 +84,7 @@ Spettri sovrapposti per le due serie con la traccia del macroiniziatore alla bas - Stokes shift **8-14 nm**, conferma del design: i domini flessibili di PCL allontanano le catene principali (meno impaccamento, più mobilità) senza introdurre distorsioni alla geometria del backbone; il basso Stokes shift indica che il core conserva la conformazione planare senza rilassamenti nel passaggio allo stato eccitato. **Tabella 10** - *dati spettroscopici dei polimeri sintetizzati* + | Polimero | λmax, abs (nm) | λmax, ex (nm) | Stokes shift (nm) | | --- | --- | --- | --- | | 3.1b | 554 | 562 | 8 | @@ -99,6 +101,7 @@ Stato solido (solo 3.2b): [[acq-e-stato-solido]]. ## GPC (r.1045-1062) → [[gpc]] **Tabella 11** - *pesi molecolari e polidispersità dei polimeri bottle brush determinati mediante GPC* + | Polimero | Massa molecolare media numerale (Da) | Massa molecolare media ponderale (Da) | Polidispersità (PD) | | --- | --- | --- | --- | | 3.1b | 12188 | 18536 | 1,521 | @@ -112,6 +115,7 @@ Interpretazione della tesi (sottostima per volume idrodinamico, outlier 3.3c): [ ## Peso molecolare da ¹H-NMR (r.1064-1089) → [[nmr-1h]] **Tabella 12** - *pesi molecolari dei polimeri bottle brush determinati via ¹H-NMR* + | Polimero | Peso Molecolare teorico (Da) | Peso Molecolare da ¹H-NMR (Da) | | --- | --- | --- | | 3.1b | 6500 | 8900 | @@ -129,9 +133,9 @@ Transizioni principali pressoché costanti per tutti i polimeri, dominate dal PC ![[immagini/d2ed44d32060aa9ee04e73304940b111e53bf65cf115a93ace696933048e308b.jpg|560]] *Figura 68 - esempio di termogramma dei polimeri bottle brush realizzati (in figura l'analisi del campione 3.1c)* · [[fig-068|nota figura]] -## Ciclovoltammetria (§4.4.4) → [[ciclovoltammetria]] +## Ciclovoltammetria (§4.4.4) → [[cv-risultati-bottle-brush]] Tabella 14: bandgap 0,929-1,521 eV. ## Collegamenti -- [[copolimeri-3a-3b-3c]] · [[rop-pcl]] · [[bottle-brush]] · [[acq-e-stato-solido]] · [[nmr-1h]] · [[ft-ir]] · [[uv-vis-fluorescenza]] · [[gpc]] · [[dsc]] · [[ciclovoltammetria]] · [[reagenti-e-materiali]] +- [[copolimeri-3a-3b-3c]] · [[rop-pcl]] · [[bottle-brush]] · [[acq-e-stato-solido]] · [[nmr-1h]] · [[ft-ir]] · [[uv-vis-fluorescenza]] · [[gpc]] · [[dsc]] · [[ciclovoltammetria]] · [[cv-risultati-bottle-brush]] · [[reagenti-e-materiali]] - [[tesi]] · [[bibliografia]] diff --git a/wiki/compounds/copolimeri-3a-3b-3c.md b/wiki/compounds/copolimeri-3a-3b-3c.md index 2477505..f5d95be 100644 --- a/wiki/compounds/copolimeri-3a-3b-3c.md +++ b/wiki/compounds/copolimeri-3a-3b-3c.md @@ -6,8 +6,8 @@ tags: [copolimeri, dpp-3ht, polimerizzazione-ossidativa, macroiniziatore] created: 2026-10-09 updated: 2026-10-09 tesi_loc: "§3.2 r.628-644; §4.2 r.826-954" -refs: [52, 53, 54] -figures: ["fig-x-cc3f54", "fig-052", "fig-053", "fig-054", "fig-055", "fig-056", "fig-057", "fig-058", "fig-059", "fig-060", "fig-061"] +refs: [54] +figures: ["fig-x-cc3f54", "fig-054", "fig-055", "fig-056", "fig-057", "fig-058", "fig-059", "fig-060", "fig-061"] status: draft --- @@ -22,6 +22,7 @@ Copolimeri **statistici (random)** del monomero [[dpp-2]] con **3-esiltiofene (3 ## Composizione di reazione (§3.2) **Tabella 3** - *composizione dei copolimeri* (r.634-640) + | Copolimero | DPP (mmol) | DPP (eq) | 3HT (mmol) | 3HT (eq) | | --- | --- | --- | --- | --- | | 3a | 0,2 | 0,2 | 0,8 | 0,8 | @@ -44,6 +45,7 @@ Motivazioni dei singoli passaggi: [[polimerizzazione-ossidativa-fecl3]]. - Libreria: **3a** (minime quantità di DPP) → **3b** → **3c** (più arricchito), sempre con rapporto molare a favore del 3HT. **Tabella 6** - *composizione dei copolimeri coniugati* + | Copolimero | moli DPP **2** | moli 3HT | % DPP teorica (mol/mol) | % DPP reale (mol/mol) | | --- | --- | --- | --- | --- | | 3a | 0,2 | 0,8 | 20 | 25,2 | @@ -74,6 +76,7 @@ La % reale è determinata da ¹H-NMR ([[nmr-1h]], Equazione 9) sul rapporto fra Profili pressoché identici tra i tre copolimeri e simili a quello del monomero DPP: ampia banda di assorbimento (transizione π→π\*, λmax ≈ **540-545 nm**) ed emissione con λmax ≈ **550 nm**. Stokes shift estremamente ridotto → forte sovrapposizione assorbimento/emissione → notevole rigidità dello scheletro, minima riorganizzazione conformazionale. **Tabella 7** - *dati spettroscopici dei copolimeri sintetizzati* + | copolimero | λmax, abs (nm) | λmax, ecc (nm) | Stokes shift (nm) | | --- | --- | --- | --- | | 3a | 540 | 547 | 7 | @@ -99,6 +102,7 @@ I film su vetrino sotto lampada UV non mostrano emissione apprezzabile ([[fig-06 Mn 1400-2150 Da. Dati: **Tabella 8** - *pesi molecolari e polidispersità determinati mediante GPC* + | Copolimero | Massa molecolare media numerica (Da) | Massa molecolare media ponderale (Da) | Polidispersità (PD) | | --- | --- | --- | --- | | 3a | 2149 | 5526 | 2,571 | @@ -112,9 +116,9 @@ Mn 1400-2150 Da. Dati: ## DSC (r.954) → [[dsc]] Per tutti i campioni **Tg intorno a −10 °C**; a differenza del 3HT **nessuna transizione di fusione**: conferma il copolimero **random**; l'elevato disordine impedisce la cristallizzazione nonostante i bassi pesi molecolari. (Le Conclusioni parlano invece di «temperature di fusione superiori a 110 °C»: [[difetti-noti]].) -## Ciclovoltammetria → [[ciclovoltammetria]] +## Ciclovoltammetria → [[cv-risultati-copolimeri]] Tabella 13 (bandgap 0,970 / 1,316 / 1,371 eV per 3a/3b/3c). ## Collegamenti -- [[dpp-2]] · [[polimerizzazione-ossidativa-fecl3]] · [[bottle-brush-3-x]] · [[bottle-brush]] · [[nmr-1h]] · [[ft-ir]] · [[uv-vis-fluorescenza]] · [[gpc]] · [[dsc]] · [[ciclovoltammetria]] · [[reagenti-e-materiali]] +- [[dpp-2]] · [[polimerizzazione-ossidativa-fecl3]] · [[bottle-brush-3-x]] · [[bottle-brush]] · [[nmr-1h]] · [[ft-ir]] · [[uv-vis-fluorescenza]] · [[gpc]] · [[dsc]] · [[ciclovoltammetria]] · [[cv-risultati-copolimeri]] · [[reagenti-e-materiali]] - [[tesi]] · [[bibliografia]] diff --git a/wiki/compounds/dpp-1.md b/wiki/compounds/dpp-1.md index 4845657..2747f5a 100644 --- a/wiki/compounds/dpp-1.md +++ b/wiki/compounds/dpp-1.md @@ -36,6 +36,7 @@ Pallone a tre colli da 25 mL con ancoretta magnetica e refrigerante, sotto fluss 5. Filtrazione su Büchner; lavaggi ripetuti con acqua distillata e metanolo; essiccamento in stufa a **85 °C**. ## Caratterizzazione (§3.2, r.600-606) + | Tecnica | Dato (verbatim) | |---|---| | 1H NMR (400 MHz, d6-DMSO) | δ = 8.24 – 8.18 (dd, *J* = 3.8, 1.2 Hz, 4H), 8.00 – 7.93 (dd, *J* = 5.0, 1.1 Hz, 4H), 7.38 – 7.25 (m, 4H) | diff --git a/wiki/compounds/dpp-2.md b/wiki/compounds/dpp-2.md index 7cf565e..c17ac79 100644 --- a/wiki/compounds/dpp-2.md +++ b/wiki/compounds/dpp-2.md @@ -34,6 +34,7 @@ Pallone a 3 colli da 50 mL con ancoretta e refrigerante. 4. Purificazione per **cristallizzazione in etanolo**: solido sciolto a caldo nella minima quantità di solvente; **freezer a −20 °C per 24 h**; precipitato scuro = DPP bis-alchilato **2**; stufa a **85 °C** fino a eliminazione del solvente. ## Caratterizzazione (§3.2, r.618-626) + | Tecnica | Dato (verbatim) | |---|---| | 1H NMR (400 MHz, CDCl3) | δ 8.96 – 8.84 (m, 1H), 7.67 – 7.58 (m, 1H), 7.33 – 7.19 (m, 2H), 4.17 – 4.04 (m, 2H), 3.73 – 3.59 (t, *J* = 6.4 Hz, 2H), 1.82 – 1.20 (m, 9H) | @@ -65,6 +66,7 @@ Per la coerenza dei valori fra §3.2 e Tabella 5 vedi [[difetti-noti]]. *Figura 48 - spettro 1H-NMR in CDCl3 del prodotto 2* · [[fig-048|nota figura]] ## FT-IR ([[fig-049|Fig. 49]], r.802) + | Numero d'onda | Assegnazione | |---|---| | ~3400 cm⁻¹ (banda larga) | stretching O-H dei gruppi alcolici terminali | diff --git a/wiki/compounds/reagenti-e-materiali.md b/wiki/compounds/reagenti-e-materiali.md index 382303e..7f3758b 100644 --- a/wiki/compounds/reagenti-e-materiali.md +++ b/wiki/compounds/reagenti-e-materiali.md @@ -20,6 +20,7 @@ Reagenti e solventi commerciali ad elevato grado di purezza, **usati senza ulter - **THF**: purificato a pressione ridotta con evaporatore rotante per rimuovere lo stabilizzante («THF sbiancato»). ## Reagenti per passaggio + | Passaggio | Reagente | Ruolo | Pagina | |---|---|---|---| | DPP **1** | Na, t-AmOH, FeCl3 (cat.) | formazione di t-AmONa (base) | [[dpp-1]] | diff --git a/wiki/concepts/bottle-brush.md b/wiki/concepts/bottle-brush.md index e9d2809..8c19e90 100644 --- a/wiki/concepts/bottle-brush.md +++ b/wiki/concepts/bottle-brush.md @@ -23,6 +23,7 @@ Il monomero [[dpp-2]] ha funzioni indipendenti, per questo detto «ortogonale e - **gruppi -OH** → assimilano la struttura a un'unità monomerica **diolica** (utilizzabile in policondensazioni con opportuni comonomeri) e fungono da **iniziatori** per ROP di monomeri ciclici ([[rop-pcl]]). ## Sequenza di sintesi (fig. di schema) + | Passo | Reazione | Prodotto | Pagina | |---|---|---|---| | 1 | 2-cianotiofene + diisopropil succinato, t-AmONa (pseudo-Stobbe) | DPP **1** | [[dpp-1]] ([[fig-x-185efd\|schema DPP 1]]) | @@ -36,6 +37,7 @@ Distribuzione statistica dei monomeri lungo la catena (§2, r.555): aumenta l'en Serie preparate da **3b** e **3c**; il copolimero **3a** non è stato usato per il grafting «a causa della scarsa efficienza della sua via sintetica»: basse rese e difficoltà di work-up per isolare il prodotto puro (perdite di materiale); isolare quantità utili avrebbe richiesto volumi di solventi e costi di reagenti molto elevati → per fattibilità tecnica ed economica solo **3b** e **3c**. ## Cosa dimostrano i dati (rimandi) + | Aspetto | Esito nella tesi | Dove | |---|---|---| | Innesto delle catene | FT-IR: scompare -OH, compare C=O a ~1720 cm⁻¹; ¹H-NMR: segnali PCL | [[ft-ir]], [[nmr-1h]] | @@ -43,7 +45,7 @@ Serie preparate da **3b** e **3c**; il copolimero **3a** non è stato usato per | Integrità del core in soluzione | λmax abs 544-554 nm, em 557-564 nm, Stokes shift 8-14 nm | [[uv-vis-fluorescenza]] | | Emissione allo stato solido | spettro SS di 3.2b: abs 570-580 nm, em ~650-660 nm | [[acq-e-stato-solido]] | | Proprietà termiche | dominate dal PCL: Tm 55-60 °C, Tc 25-35 °C | [[dsc]] | -| Elettroattività | processi redox EC irreversibili; bandgap 0,929-1,521 eV | [[ciclovoltammetria]] | +| Elettroattività | processi redox EC irreversibili; bandgap 0,929-1,521 eV | [[ciclovoltammetria]], [[cv-risultati-bottle-brush]] | ## Messaggio conclusivo (§5, r.1291) «L'approccio ortogonale basato su scheletri semiconduttori DPP-3HT modificati mediante catene laterali di PCL consente di combinare proprietà elettrochimiche modulabili e capacità emissiva allo stato solido.» diff --git a/wiki/concepts/dpp-reattivita.md b/wiki/concepts/dpp-reattivita.md index 0b86234..7b4795b 100644 --- a/wiki/concepts/dpp-reattivita.md +++ b/wiki/concepts/dpp-reattivita.md @@ -6,7 +6,7 @@ created: 2026-10-09 updated: 2026-10-09 tesi_loc: "§1.1.2 r.247-373" refs: [2, 5, 7, 21, 22, 23, 24, 25, 26, 27, 28, 29, 30, 31, 32] -figures: ["fig-017", "fig-018", "fig-019", "fig-020", "fig-021", "fig-022", "fig-023", "fig-024", "fig-025", "fig-026", "fig-027", "fig-028", "fig-029", "fig-030"] +figures: ["fig-017", "fig-018", "fig-019", "fig-020", "fig-021", "fig-022", "fig-023", "fig-024", "fig-025", "fig-026", "fig-027", "fig-029", "fig-030"] status: draft --- @@ -103,6 +103,7 @@ I sostituenti arilici derivanti dai benzonitrili di partenza sono considerati pa ## 4. Litiazione in C5 (r.363) I DPP **29**, **30**, **31** ([[fig-021|Fig. 21]]) reagiscono con **LDA** ([[fig-029|Fig. 29]]): + | Elettrofilo | Prodotto | Rif. | |---|---|---| | formammidi (N-formilpiperidina o DMF) | dialdeide **43** | [[30-hong-2012\|30]] | diff --git a/wiki/concepts/dpp-sintesi-letteratura.md b/wiki/concepts/dpp-sintesi-letteratura.md index a8546aa..e1a16c7 100644 --- a/wiki/concepts/dpp-sintesi-letteratura.md +++ b/wiki/concepts/dpp-sintesi-letteratura.md @@ -17,6 +17,7 @@ Il §1.1.1 «Storia e sintesi» passa in rassegna le vie sintetiche al nucleo DP > **Numerazione.** I numeri dei composti di questa pagina (1-13, 17, 19-21...) sono quelli del cap. 1 e **non** coincidono con i composti 1 e 2 della parte sperimentale. In questa pagina «DPP 3» è il DPP dal benzonitrile. ## Indice dei metodi + | Metodo | Autori / anno | Reagenti chiave | Resa riportata | Figura | |---|---|---|---|---| | Reformatskij modificato (scoperta) | Farnum et al., 1974 [[02-shaikh-2022\|2]] | bromoacetato + benzonitrile + Zn | pigmento rosso 5-20% (sottoprodotto) | [[fig-002\|Fig. 2]] | @@ -42,6 +43,7 @@ Il §1.1.1 «Storia e sintesi» passa in rassegna le vie sintetiche al nucleo DP *Figura 3 - esperimento crossover in presenza di amminocinnamato* · [[fig-003|nota figura]] ### Tabella 1 - esperimenti di crossover, risultati in rapporto molare (r.106-112) + | A | B | Zn | 1 | 5 | 4 | 3 | | --- | --- | --- | --- | --- | --- | --- | | 1 | 1 | 1 | 0 | 100 | - | - | diff --git a/wiki/concepts/dpp-struttura-e-proprieta.md b/wiki/concepts/dpp-struttura-e-proprieta.md index 6d54294..53a6773 100644 --- a/wiki/concepts/dpp-struttura-e-proprieta.md +++ b/wiki/concepts/dpp-struttura-e-proprieta.md @@ -5,7 +5,7 @@ tags: [dpp, struttura, proprietà-ottiche, impaccamento] created: 2026-10-09 updated: 2026-10-09 tesi_loc: "§1.1 r.69-81; §1.1.2 r.203-245; §4.1 r.722-732" -refs: [1, 2, 3, 4, 16, 17, 18, 19, 20] +refs: [1, 2, 3, 4, 16, 17, 18, 19, 20, 34] figures: ["fig-001", "fig-015", "fig-016", "fig-040"] status: draft --- diff --git a/wiki/concepts/optoelettronica-oled-donatore-accettore.md b/wiki/concepts/optoelettronica-oled-donatore-accettore.md index 497fdf6..b5073ef 100644 --- a/wiki/concepts/optoelettronica-oled-donatore-accettore.md +++ b/wiki/concepts/optoelettronica-oled-donatore-accettore.md @@ -34,7 +34,7 @@ Cap. 1.4 «Applicazioni». Sul perché serve evitare l'ACQ in questi dispositivi ## Scelta DPP + 3HT nella tesi (r.520-522) - Il nucleo elettron-accettore del DPP è combinato con unità di **3-esiltiofene (3HT)**, fortemente elettron-donatrici. - Il tiofene è partner elettronico ideale per ibridare gli orbitali di frontiera del DPP e, con la catena esilica laterale, garantisce **solubilità** e quindi processabilità (rif. [[49-hendriks-2013|49]]). -- La sinergia D-A DPP/3HT permette di sintonizzare la struttura a bande: requisiti per un impiego come **strato elettro-luminescente in OLED**. Dati reali del band gap: [[ciclovoltammetria]]. Sintesi: [[copolimeri-3a-3b-3c]]. +- La sinergia D-A DPP/3HT permette di sintonizzare la struttura a bande: requisiti per un impiego come **strato elettro-luminescente in OLED**. Dati reali del band gap: [[cv-risultati-copolimeri]], [[cv-risultati-bottle-brush]]. Sintesi: [[copolimeri-3a-3b-3c]]. ## Struttura di un OLED (r.524-528) - Architettura multistrato (sandwich) per ottimizzare iniezione, trasporto e ricombinazione di carica. I primi dispositivi a singolo strato avevano efficienze ridotte per forte sbilanciamento tra mobilità di elettroni e lacune. diff --git a/wiki/concepts/polimerizzazione-ossidativa-fecl3.md b/wiki/concepts/polimerizzazione-ossidativa-fecl3.md index 21fb976..aa5166a 100644 --- a/wiki/concepts/polimerizzazione-ossidativa-fecl3.md +++ b/wiki/concepts/polimerizzazione-ossidativa-fecl3.md @@ -48,6 +48,7 @@ Metodo usato per costruire lo scheletro coniugato DPP-3HT ([[copolimeri-3a-3b-3c Necessario per prevenire reazioni indotte dall'umidità. L'acqua (nucleofilo e base di Lewis) potrebbe: (1) coordinarsi a FeCl3 formando specie idrate stabili, saturando la sfera di coordinazione, riducendo il potenziale ossidativo e inibendo l'innesco; (2) causare il **quenching degli intermedi cationico-radicalici** in propagazione per attacco nucleofilo, con terminazione prematura e difetti che interrompono la coniugazione e compromettono le proprietà semiconduttrici. ## Work-up e purificazione (r.850-858; procedura r.644) + | Passaggio | Funzione | |---|---| | Lavaggi con **HCl** (0,6 M) | mantengono i sali di ferro in fase acquosa evitando la precipitazione come idrossidi insolubili all'interfaccia. La rimozione completa dell'ossidante è un requisito: tracce di metalli di transizione nel backbone abbatterebbero la mobilità dei portatori e spegnerebbero la fluorescenza | diff --git a/wiki/dati.md b/wiki/dati.md new file mode 100644 index 0000000..9858742 --- /dev/null +++ b/wiki/dati.md @@ -0,0 +1,81 @@ +--- +title: Indice dei dati +type: overview +tags: [dati, indice, lookup] +created: 2026-10-09 +updated: 2026-10-09 +tesi_loc: "r.588-1291" +status: draft +--- + +# Indice dei dati + +Mappa «grandezza → dove sta». I valori restano nelle pagine indicate (una tabella in una sola pagina); qui solo campo di variazione e rimando. Campioni: **1**, **2** = [[dpp-1]], [[dpp-2]]; **3a-c** = [[copolimeri-3a-3b-3c]]; **3.1b-3.3c** = [[bottle-brush-3-x]]. + +## Quantità e condizioni di sintesi + +| Dato | Campioni | Dove | +|---|---|---| +| Reagenti, mmol, eq, T, tempi | 1 | [[dpp-1]] (procedura) | +| Reagenti, mmol, eq, T, tempi | 2 | [[dpp-2]] (procedura) | +| Composizione di reazione (Tab. 3) e procedura FeCl₃ | 3a, 3b, 3c | [[copolimeri-3a-3b-3c]] | +| Volumi di caprolattone (Tab. 4, 9) e formula $V_{CL}$ | 3.1b-3.3c | [[bottle-brush-3-x]] | +| Tutti i reagenti per passaggio, trattamento dei solventi | tutti | [[reagenti-e-materiali]] | + +## Composizione e pesi molecolari + +| Dato | Campioni | Intervallo | Dove | +|---|---|---|---| +| % DPP teorica/reale (Tab. 6) | 3a-c | reale 25,2-35,3% (max 35%) | [[copolimeri-3a-3b-3c]], metodo in [[nmr-1h]] (Eq. 9) | +| Mn, Mw, PD GPC (Tab. 8) | 3a-c | Mn 1402-2149 Da; PD 1,979-4,592 | [[copolimeri-3a-3b-3c]], interpretazione in [[gpc]] | +| Mn, Mw, PD GPC (Tab. 11) | 3.1b-3.3c | Mn 12188-21269 Da; PD 1,238-1,521 | [[bottle-brush-3-x]], interpretazione in [[gpc]] | +| Peso molecolare teorico vs ¹H-NMR (Tab. 12, Eq. 10) | 3.1b-3.3c | NMR 8900-88000 Da | [[bottle-brush-3-x]], metodo in [[nmr-1h]] | + +## Proprietà ottiche + +| Dato | Campioni | Intervallo | Dove | +|---|---|---|---| +| λabs, λem, Stokes shift (Tab. 5) | 1, 2 | abs 531-541 nm; Stokes 11-14 nm | [[dpp-2]] | +| Idem (Tab. 7) | 3a-c | abs 540-544 nm; Stokes 6-10 nm | [[copolimeri-3a-3b-3c]] | +| Idem (Tab. 10) | 3.1b-3.3c | abs 544-554 nm; em 557-564 nm; Stokes 8-14 nm | [[bottle-brush-3-x]] | +| Riepilogo di tutti i valori in soluzione | tutti | - | [[uv-vis-fluorescenza]] | +| ε | 1; 2 | 28000; 13218 M⁻¹ cm⁻¹ | [[dpp-2]], [[uv-vis-fluorescenza]] | +| Stato solido (assorbimento, emissione, Stokes) | 3.2b | abs 570-580 nm; em ~650-660 nm | [[acq-e-stato-solido]] | +| Tab. 2 (DPP letteratura, sostituenti) | - | - | [[dpp-struttura-e-proprieta]] | + +## Proprietà termiche ed elettrochimiche + +| Dato | Campioni | Intervallo | Dove | +|---|---|---|---| +| Tg | 3a-c | ≈ −10 °C | [[dsc]] | +| Tm, Tc | 3.1b-3.3c | 55-60 °C; 25-35 °C | [[dsc]] | +| Eonset, HOMO, LUMO, bandgap (Tab. 13) | 3a-c | bandgap 0,970-1,371 eV | [[cv-risultati-copolimeri]] | +| Idem (Tab. 14) | 3.1b-3.3c | bandgap 0,929-1,521 eV | [[cv-risultati-bottle-brush]] | +| Condizioni CV (elettrodi, solvente, elettrolita, scan rate) | tutti | - | [[ciclovoltammetria]] | + +## Spettroscopia di struttura + +| Dato | Dove | +|---|---| +| δ ¹H-NMR verbatim (procedure) | [[dpp-1]], [[dpp-2]] | +| Assegnazioni ¹H-NMR | [[dpp-1]], [[dpp-2]], [[nmr-1h]] | +| Bande IR | [[ft-ir]], [[dpp-2]] | + +## Equazioni + +| Eq. | Contenuto | Dove | +|---|---|---| +| 1-5 | resa quantica, tempo di vita | [[fluorescenza]] | +| 6-8 | Nernst, Cottrell, Randles-Sevcik | [[ciclovoltammetria]] | +| 9 | % DPP da ¹H-NMR | [[nmr-1h]] | +| 10 | peso molecolare bottle brush da ¹H-NMR | [[nmr-1h]] | +| 11-12 | HOMO, LUMO, bandgap | [[ciclovoltammetria]] | +| $V_{CL}$ | volume di caprolattone | [[bottle-brush-3-x]] | + +Tab. 1 (crossover Reformatskij): [[dpp-sintesi-letteratura]]. + +## Dati da usare con cautela +Valori discordanti fra procedure, tabelle e Conclusioni: [[difetti-noti]]. + +## Collegamenti +- [[tesi]] · [[overview]] · [[index]] diff --git a/wiki/overview.md b/wiki/overview.md index b17998f..8cf0237 100644 --- a/wiki/overview.md +++ b/wiki/overview.md @@ -23,6 +23,7 @@ I semiconduttori π-coniugati usati nella soft optoelectronics perdono emissione 4. **Caratterizzazione**: [[nmr-1h]], [[ft-ir]], [[gpc]], [[uv-vis-fluorescenza]], [[dsc]], [[ciclovoltammetria]]. ## Risultati dichiarati (con riferimento ai dati) + | Tema | Risultato | Dati / pagina | |---|---|---| | Struttura | analisi spettroscopiche (¹H-NMR, FT-IR) e GPC confermano la sintesi e macromolecole ramificate ad alta densità strutturale (Riassunto r.19) | [[nmr-1h]], [[ft-ir]], [[gpc]] | @@ -31,7 +32,7 @@ I semiconduttori π-coniugati usati nella soft optoelectronics perdono emissione | Termico | dominato dal PCL: Tm 55-60 °C, Tc 25-35 °C | [[dsc]] | | Ottico in soluzione | core DPP intatto: λabs 544-554 nm, λem 557-564 nm, Stokes shift 8-14 nm | [[uv-vis-fluorescenza]] | | Ottico allo stato solido | film lineari non emissivi; bottle brush 3.2b: assorbimento 570-580 nm, emissione ~650-660 nm; emissione nel rosso apprezzabile | [[acq-e-stato-solido]] | -| Elettrochimico | processi EC irreversibili; bandgap 0,970-1,371 eV (lineari, crescente con la % di DPP) e 0,929-1,521 eV (bottle brush) | [[ciclovoltammetria]] | +| Elettrochimico | processi EC irreversibili; bandgap 0,970-1,371 eV (lineari, crescente con la % di DPP) e 0,929-1,521 eV (bottle brush) | [[ciclovoltammetria]], [[cv-risultati-copolimeri]], [[cv-risultati-bottle-brush]] | ## Conclusione della tesi (§5, r.1291) L'approccio ortogonale basato su scheletri semiconduttori DPP-3HT modificati con catene laterali di PCL combina **proprietà elettrochimiche modulabili** e **capacità emissiva allo stato solido**, con potenziale per dispositivi optoelettronici. diff --git a/wiki/techniques/ciclovoltammetria.md b/wiki/techniques/ciclovoltammetria.md index 336ff3b..72c6c9a 100644 --- a/wiki/techniques/ciclovoltammetria.md +++ b/wiki/techniques/ciclovoltammetria.md @@ -4,15 +4,15 @@ type: technique tags: [cv, elettrochimica, bandgap, homo-lumo, onset, ferrocene, drogaggio] created: 2026-10-09 updated: 2026-10-09 -tesi_loc: "§3.3 r.666-699; §3.4 r.702-714; §4.4 r.1100-1251; §5 r.1289" +tesi_loc: "§3.3 r.666-699; §3.4 r.702-714; §4.4.1-4.4.2 r.1100-1172" refs: [50] -figures: ["fig-039", "fig-069", "fig-070", "fig-071", "fig-072", "fig-073"] +figures: ["fig-039", "fig-069", "fig-070"] status: draft --- # Ciclovoltammetria (CV) -La CV è una tecnica elettrochimica dinamica della famiglia delle voltammetriche, usata per studiare i processi redox; per materiali macromolecolari e coniugati serve a indagare trasferimento elettronico, stabilità elettrochimica e **gap energetico elettrochimico** (§4.4, r.1102-1104). Risultati per composto: [[copolimeri-3a-3b-3c]], [[bottle-brush-3-x]]. +La CV è una tecnica elettrochimica dinamica della famiglia delle voltammetriche, usata per studiare i processi redox; per materiali macromolecolari e coniugati serve a indagare trasferimento elettronico, stabilità elettrochimica e **gap energetico elettrochimico** (§4.4, r.1102-1104). Questa pagina contiene teoria, procedura e metodo di analisi. Risultati: [[cv-risultati-copolimeri]] (Tab. 13) e [[cv-risultati-bottle-brush]] (Tab. 14). ## 1. Principi teorici (§3.3, r.668-699) - A differenza delle tecniche in stato stazionario il potenziale varia in modo continuo nel tempo (strumento utile per i meccanismi di trasferimento elettronico). @@ -107,61 +107,6 @@ E_{g}=E_{LUMO}-E_{HOMO} $$ **Equazione 12** - *bandgap elettrochimico* -## 5. Risultati sui copolimeri lineari (§4.4.3, r.1177-1227) -Scopo: capire come la **frazione reale di DPP** modula l'architettura energetica dello scheletro coniugato puro, senza gli effetti sterici/conformazionali dell'innesto. - -**Tabella 13** - *dati voltammetrici dei copolimeri sintetizzati* -| Polimero | % reale DPP | Eonsetox (V) | Eonsetred (V) | HOMO (eV) | LUMO (eV) | Bandgap (eV) | -| --- | --- | --- | --- | --- | --- | --- | -| 3a | 25 | 0,238 | -0,732 | -5,038 | -4,068 | 0,970 | -| 3b | 32 | 0,054 | -1,262 | -4,854 | -3,538 | 1,316 | -| 3c | 35 | 0,0006 | -1,372 | -4,799 | -3,428 | 1,371 | - -### Bandgap vs % DPP ([[fig-071|Fig. 71]]) -- All'aumentare del DPP si osserva un **allargamento progressivo del bandgap**: la variazione è governata dalla composizione stechiometrica effettiva. -- La netta pendenza positiva della retta di interpolazione indica forte sensibilità alla composizione: incrementi modesti di DPP aumentano molto l'energia per le transizioni elettroniche. Lettura della tesi: l'unità DPP **riduce la lunghezza di coniugazione effettiva**, limitando la delocalizzazione π e aumentando la separazione HOMO-LUMO. -- Dimostra la fattibilità di un controllo mirato del band gap calibrando il rapporto fra i due monomeri. - -![[immagini/6c7bd8393eb8c1a329f65b7fc74e5f338a866e514455c0122a43d13ca340ded5.jpg|560]] -*Figura 71 - correlazione tra bandgap elettrochimico e frazione reale di DPP nei copolimeri sintetizzati* · [[fig-071|nota figura]] - -### Potenziali di picco vs % DPP ([[fig-072|Fig. 72]]) -- **Riduzione (n-doping)**: variazione più marcata. Da 25% DPP (Epc ≈ −1 V) a 32-35% il picco si sposta tra **−1,6 V e −1,8 V**: l'inserzione di elettroni diventa termodinamicamente più sfavorita, con sovratensioni maggiori per formare i radical-anioni. -- **Ossidazione (p-doping)**: impatto minore; Epa passa da ≈ **0,4 V** (minor DPP) a ≈ **0,2/0,25 V** per frazioni maggiori. -- Effetto combinato: aumento della separazione tra i picchi con la % di DPP, coerente con l'aumento del bandgap. - -![[immagini/d7a3694f2d97dcaa84465aeed07d8d26adca6a8f8ed64f7ea2bf86943b918b66.jpg|560]] -*Figura 72 - correlazione tra Epicco e frazione reale di DPP nei copolimeri sintetizzati* · [[fig-072|nota figura]] - -### Potenziali di onset vs % DPP ([[fig-073|Fig. 73]]) -- Eonsetred (LUMO): da ≈ **−0,75 V** (basso DPP) a ≈ **−1,4 V** (frazioni maggiori). -- Eonsetox (HOMO): da ≈ **0,25 V** a quasi **0 V** (lieve traslazione). -- La progressiva separazione fra i due onset conferma l'allargamento del bandgap: la composizione agisce sistematicamente sui livelli di frontiera. - -![[immagini/b2931ebedd31df7df3b344c25fcbb4a64aceb7b356181adecf39363e49dcb0fe.jpg|560]] -*Figura 73 - correlazione tra Eonset e frazione reale di DPP nei copolimeri sintetizzati* · [[fig-073|nota figura]] - -### Confronto con P3HT (r.1223-1227) -- Il P3HT omopolimero è molto elettron-ricco: ossidazione (p-doping) a potenziali accessibili, **nessun contributo faradico significativo** per la riduzione (n-doping) nella consueta finestra dei solventi organici. -- Nei copolimeri il DPP, forte porzione elettron-attrattrice in un'architettura D-A, **stabilizza il LUMO**: rende favorevole l'iniezione di elettroni e giustifica le onde catodiche assenti nel P3HT. L'abbassamento del LUMO, con la modulazione dell'HOMO ad opera dei segmenti di 3HT, determina il **restringimento del bandgap** rispetto all'omopolimero. -- Conclusione della tesi: la sistematicità con cui la composizione influenza la risposta termodinamica convalida l'approccio come strumento di ingegnerizzazione del materiale. - -## 6. Effetto del design bottle brush (§4.4.4, r.1232-1251) -**Tabella 14** - *dati voltammetrici dei polimeri sintetizzati* -| Polimero | Eonsetox (V) | Eonsetred (V) | HOMO (eV) | LUMO (eV) | Bandgap (eV) | -| --- | --- | --- | --- | --- | --- | -| 3.1.b | -0,183 | -1,22 | -4,617 | -3,580 | 1,037 | -| 3.2.b | -0,175 | -1,273 | -4,625 | -3,527 | 1,098 | -| 3.3.b | -0,17 | -1,202 | -4,630 | -3,598 | 1,032 | -| 3.1.c | -0,0259 | -1,547 | -4,774 | -3,253 | 1,521 | -| 3.2.c | -0,112 | -1,531 | -4,688 | -3,269 | 1,419 | -| 3.3.c | -0,321 | -1,25 | -4,479 | -3,550 | 0,929 | - -- I bottle brush **mantengono l'elettroattività** dello scheletro: i processi redox avvengono a carico del core DPP-3HT, mentre i rami alifatici fungono da **matrice dielettrica** circostante. -- Le ingombranti catene laterali modificano HOMO e LUMO rispetto ai lineari, quindi l'ampiezza del bandgap. Attribuzione: effetti di ingombro sterico dei rami di PCL sul **grado di coplanarità locale** dello scheletro → estensione effettiva della delocalizzazione. -- Bandgap dei bottle brush in 0,929-1,521 eV: l'ingegnerizzazione con PCL «non compromette le spiccate potenzialità optoelettroniche». -- Il confronto con i lineari nel testo rimanda a «paragrafo XX (XX)», segnaposto non risolto ([[difetti-noti]]). - ## Collegamenti -- [[copolimeri-3a-3b-3c]] · [[bottle-brush-3-x]] · [[optoelettronica-oled-donatore-accettore]] · [[bottle-brush]] +- [[cv-risultati-copolimeri]] · [[cv-risultati-bottle-brush]] · [[copolimeri-3a-3b-3c]] · [[bottle-brush-3-x]] · [[optoelettronica-oled-donatore-accettore]] · [[bottle-brush]] - [[tesi]] · [[bibliografia]] diff --git a/wiki/techniques/cv-risultati-bottle-brush.md b/wiki/techniques/cv-risultati-bottle-brush.md new file mode 100644 index 0000000..83ab1ba --- /dev/null +++ b/wiki/techniques/cv-risultati-bottle-brush.md @@ -0,0 +1,35 @@ +--- +title: CV - risultati sui polimeri bottle brush (3.1b-3.3c) +type: technique +tags: [cv, bandgap, homo-lumo, bottle-brush] +created: 2026-10-09 +updated: 2026-10-09 +tesi_loc: "§4.4.4 r.1230-1251" +refs: [] +figures: [] +status: draft +--- + +# CV - risultati sui polimeri bottle brush (3.1b-3.3c) + +Risultati della [[ciclovoltammetria]] sui [[bottle-brush-3-x]]. Metodo: [[ciclovoltammetria]]. Termine di confronto: [[cv-risultati-copolimeri]]. + +**Tabella 14** - *dati voltammetrici dei polimeri sintetizzati* + +| Polimero | Eonsetox (V) | Eonsetred (V) | HOMO (eV) | LUMO (eV) | Bandgap (eV) | +| --- | --- | --- | --- | --- | --- | +| 3.1.b | -0,183 | -1,22 | -4,617 | -3,580 | 1,037 | +| 3.2.b | -0,175 | -1,273 | -4,625 | -3,527 | 1,098 | +| 3.3.b | -0,17 | -1,202 | -4,630 | -3,598 | 1,032 | +| 3.1.c | -0,0259 | -1,547 | -4,774 | -3,253 | 1,521 | +| 3.2.c | -0,112 | -1,531 | -4,688 | -3,269 | 1,419 | +| 3.3.c | -0,321 | -1,25 | -4,479 | -3,550 | 0,929 | + +- I bottle brush **mantengono l'elettroattività** dello scheletro: i processi redox avvengono a carico del core DPP-3HT, mentre i rami alifatici fungono da **matrice dielettrica** circostante. +- Le ingombranti catene laterali modificano HOMO e LUMO rispetto ai lineari, quindi l'ampiezza del bandgap. Attribuzione: effetti di ingombro sterico dei rami di PCL sul **grado di coplanarità locale** dello scheletro → estensione effettiva della delocalizzazione. +- Bandgap dei bottle brush in 0,929-1,521 eV: l'ingegnerizzazione con PCL «non compromette le spiccate potenzialità optoelettroniche». +- Il confronto con i lineari nel testo rimanda a «paragrafo XX (XX)», segnaposto non risolto ([[difetti-noti]]). + +## Collegamenti +- [[ciclovoltammetria]] · [[cv-risultati-copolimeri]] · [[bottle-brush-3-x]] · [[bottle-brush]] +- [[tesi]] · [[difetti-noti]] diff --git a/wiki/techniques/cv-risultati-copolimeri.md b/wiki/techniques/cv-risultati-copolimeri.md new file mode 100644 index 0000000..ba6fccb --- /dev/null +++ b/wiki/techniques/cv-risultati-copolimeri.md @@ -0,0 +1,58 @@ +--- +title: CV - risultati sui copolimeri lineari (3a, 3b, 3c) +type: technique +tags: [cv, bandgap, homo-lumo, onset, p3ht] +created: 2026-10-09 +updated: 2026-10-09 +tesi_loc: "§4.4.3 r.1175-1227; §5 r.1289" +refs: [] +figures: ["fig-071", "fig-072", "fig-073"] +status: draft +--- + +# CV - risultati sui copolimeri lineari (3a, 3b, 3c) + +Risultati della [[ciclovoltammetria]] sugli scheletri [[copolimeri-3a-3b-3c]]. Metodo di analisi (onset, ferrocene, Eq. 11-12, irreversibilità EC): [[ciclovoltammetria]]. Confronto con i bottle brush: [[cv-risultati-bottle-brush]]. Incoerenze delle Conclusioni su bandgap e R²: [[difetti-noti]] (punto 6). + +Scopo: capire come la **frazione reale di DPP** modula l'architettura energetica dello scheletro coniugato puro, senza gli effetti sterici/conformazionali dell'innesto. + +**Tabella 13** - *dati voltammetrici dei copolimeri sintetizzati* + +| Polimero | % reale DPP | Eonsetox (V) | Eonsetred (V) | HOMO (eV) | LUMO (eV) | Bandgap (eV) | +| --- | --- | --- | --- | --- | --- | --- | +| 3a | 25 | 0,238 | -0,732 | -5,038 | -4,068 | 0,970 | +| 3b | 32 | 0,054 | -1,262 | -4,854 | -3,538 | 1,316 | +| 3c | 35 | 0,0006 | -1,372 | -4,799 | -3,428 | 1,371 | + +### Bandgap vs % DPP ([[fig-071|Fig. 71]]) +- All'aumentare del DPP si osserva un **allargamento progressivo del bandgap**: la variazione è governata dalla composizione stechiometrica effettiva. +- La netta pendenza positiva della retta di interpolazione indica forte sensibilità alla composizione: incrementi modesti di DPP aumentano molto l'energia per le transizioni elettroniche. Lettura della tesi: l'unità DPP **riduce la lunghezza di coniugazione effettiva**, limitando la delocalizzazione π e aumentando la separazione HOMO-LUMO. +- Dimostra la fattibilità di un controllo mirato del band gap calibrando il rapporto fra i due monomeri. + +![[immagini/6c7bd8393eb8c1a329f65b7fc74e5f338a866e514455c0122a43d13ca340ded5.jpg|560]] +*Figura 71 - correlazione tra bandgap elettrochimico e frazione reale di DPP nei copolimeri sintetizzati* · [[fig-071|nota figura]] + +### Potenziali di picco vs % DPP ([[fig-072|Fig. 72]]) +- **Riduzione (n-doping)**: variazione più marcata. Da 25% DPP (Epc ≈ −1 V) a 32-35% il picco si sposta tra **−1,6 V e −1,8 V**: l'inserzione di elettroni diventa termodinamicamente più sfavorita, con sovratensioni maggiori per formare i radical-anioni. +- **Ossidazione (p-doping)**: impatto minore; Epa passa da ≈ **0,4 V** (minor DPP) a ≈ **0,2/0,25 V** per frazioni maggiori. +- Effetto combinato: aumento della separazione tra i picchi con la % di DPP, coerente con l'aumento del bandgap. + +![[immagini/d7a3694f2d97dcaa84465aeed07d8d26adca6a8f8ed64f7ea2bf86943b918b66.jpg|560]] +*Figura 72 - correlazione tra Epicco e frazione reale di DPP nei copolimeri sintetizzati* · [[fig-072|nota figura]] + +### Potenziali di onset vs % DPP ([[fig-073|Fig. 73]]) +- Eonsetred (LUMO): da ≈ **−0,75 V** (basso DPP) a ≈ **−1,4 V** (frazioni maggiori). +- Eonsetox (HOMO): da ≈ **0,25 V** a quasi **0 V** (lieve traslazione). +- La progressiva separazione fra i due onset conferma l'allargamento del bandgap: la composizione agisce sistematicamente sui livelli di frontiera. + +![[immagini/b2931ebedd31df7df3b344c25fcbb4a64aceb7b356181adecf39363e49dcb0fe.jpg|560]] +*Figura 73 - correlazione tra Eonset e frazione reale di DPP nei copolimeri sintetizzati* · [[fig-073|nota figura]] + +### Confronto con P3HT (r.1223-1227) +- Il P3HT omopolimero è molto elettron-ricco: ossidazione (p-doping) a potenziali accessibili, **nessun contributo faradico significativo** per la riduzione (n-doping) nella consueta finestra dei solventi organici. +- Nei copolimeri il DPP, forte porzione elettron-attrattrice in un'architettura D-A, **stabilizza il LUMO**: rende favorevole l'iniezione di elettroni e giustifica le onde catodiche assenti nel P3HT. L'abbassamento del LUMO, con la modulazione dell'HOMO ad opera dei segmenti di 3HT, determina il **restringimento del bandgap** rispetto all'omopolimero. +- Conclusione della tesi: la sistematicità con cui la composizione influenza la risposta termodinamica convalida l'approccio come strumento di ingegnerizzazione del materiale. + +## Collegamenti +- [[ciclovoltammetria]] · [[cv-risultati-bottle-brush]] · [[copolimeri-3a-3b-3c]] · [[optoelettronica-oled-donatore-accettore]] +- [[tesi]] · [[difetti-noti]] diff --git a/wiki/techniques/dsc.md b/wiki/techniques/dsc.md index 591e803..3c5ff97 100644 --- a/wiki/techniques/dsc.md +++ b/wiki/techniques/dsc.md @@ -16,6 +16,7 @@ status: draft **TA Q2000**, atmosfera inerte di **azoto**. Due cicli di riscaldamento da **−50 °C a 250 °C** a **20 °C/min**, intervallati da un ciclo di raffreddamento da 250 °C a −50 °C a **−10 °C/min**. ## Risultati + | Campioni | Risultato | Interpretazione della tesi | |---|---|---| | Copolimeri lineari [[copolimeri-3a-3b-3c]] (r.954) | Tg intorno a **−10 °C** per tutti; **nessuna transizione di fusione** (a differenza del 3HT) | copolimero **random**; elevato disordine impedisce la cristallizzazione nonostante i bassi pesi molecolari | diff --git a/wiki/techniques/ft-ir.md b/wiki/techniques/ft-ir.md index 20a0b43..8181b39 100644 --- a/wiki/techniques/ft-ir.md +++ b/wiki/techniques/ft-ir.md @@ -16,6 +16,7 @@ status: draft Spettroscopia infrarossa a **riflettanza totale attenuata** (ATR) con spettrofotometro **ATR-IR Bruker alpha I**. ## Bande diagnostiche usate nella tesi + | Banda | Assegnazione | Campione | Pagina | |---|---|---|---| | 3400 / 3300-3400 cm⁻¹ (larga) | O-H terminale | [[dpp-2]], **3a-c** (più debole in 3a) | [[dpp-2]], [[copolimeri-3a-3b-3c]] | diff --git a/wiki/techniques/nmr-1h.md b/wiki/techniques/nmr-1h.md index 1767903..b5eeb9b 100644 --- a/wiki/techniques/nmr-1h.md +++ b/wiki/techniques/nmr-1h.md @@ -16,6 +16,7 @@ status: draft Spettri ¹H-NMR in soluzione con spettrometro **Varian Mercury 400 (400 MHz)**, **TMS** come standard interno. Solventi dei dati: d6-DMSO per [[dpp-1]]; CDCl3 per [[dpp-2]], copolimeri e bottle brush. ## Dove sono i dati + | Campione | Spettro | Contenuto | Pagina | |---|---|---|---| | DPP **1** | [[fig-044\|Fig. 44]] (DMSO) | NH ~11 ppm; tiofene: dd, d, dd | [[dpp-1]] | diff --git a/wiki/techniques/uv-vis-fluorescenza.md b/wiki/techniques/uv-vis-fluorescenza.md index d122e2d..cbdd395 100644 --- a/wiki/techniques/uv-vis-fluorescenza.md +++ b/wiki/techniques/uv-vis-fluorescenza.md @@ -6,7 +6,7 @@ created: 2026-10-09 updated: 2026-10-09 tesi_loc: "§3.1 r.579-581; §4.1 r.768-823; §4.2 r.906-928; §4.3 r.1024-1043; §4.5 r.1266-1276" refs: [51] -figures: ["fig-045", "fig-050", "fig-051", "fig-058", "fig-059", "fig-060", "fig-067", "fig-074"] +figures: ["fig-051", "fig-074"] status: draft --- @@ -18,6 +18,7 @@ status: draft - Solvente delle misure di soluzione: **THF** (per ε di **2**: CHCl3). ## Riepilogo dei dati in soluzione (da tabelle della tesi) + | Campione | λmax,abs (nm) | λmax,em/ex (nm) | Stokes shift (nm) | Fonte | |---|---|---|---|---| | [[dpp-1]] | 531 | 542 | 11 | Tab. 5 | diff --git a/wiki/tesi.md b/wiki/tesi.md index 9803a95..a88e29b 100644 --- a/wiki/tesi.md +++ b/wiki/tesi.md @@ -16,7 +16,7 @@ Sintesi e caratterizzazione di copolimeri bottle brush foto-elettro attivi. Cand Il contenuto della tesi è riorganizzato per argomento, non per capitolo. Ogni dato sta in una sola pagina (la pagina dove la tesi lo discute), le altre rimandano. - **Concetti**: [[bottle-brush]] (hub), [[acq-e-stato-solido]], [[dpp-struttura-e-proprieta]], [[dpp-sintesi-letteratura]], [[dpp-reattivita]], [[fluorescenza]], [[fluorofori-in-polimeri]], [[optoelettronica-oled-donatore-accettore]], [[polimerizzazione-ossidativa-fecl3]], [[rop-pcl]] - **Composti**: [[dpp-1]], [[dpp-2]], [[copolimeri-3a-3b-3c]], [[bottle-brush-3-x]], [[reagenti-e-materiali]] -- **Tecniche**: [[nmr-1h]], [[ft-ir]], [[gpc]], [[uv-vis-fluorescenza]], [[dsc]], [[ciclovoltammetria]] +- **Tecniche**: [[nmr-1h]], [[ft-ir]], [[gpc]], [[uv-vis-fluorescenza]], [[dsc]], [[ciclovoltammetria]], [[cv-risultati-copolimeri]], [[cv-risultati-bottle-brush]] - **Altro**: [[overview]], [[bibliografia]], [[difetti-noti]], le note delle 78 figure in `wiki/figures/` (generate da `raw/immagini.json`) ## Mappa sezioni → pagine → figure @@ -47,8 +47,8 @@ Figure: numero della tesi con link alla nota (`fig-NNN`); «schema» = i 4 file | 4.4 | Ciclovoltammetrie | r.1100 | [[ciclovoltammetria]] | - | | 4.4.1 | Ciclovoltammetrie su polimeri elettroattivi | r.1107 | [[ciclovoltammetria]] | - | | 4.4.2 | Metodologie di analisi voltammetrica | r.1118 | [[ciclovoltammetria]] | [[fig-069|69]], [[fig-070|70]] | -| 4.4.3 | Proprietà elettrochimiche dei copolimeri lienari | r.1175 | [[ciclovoltammetria]] | [[fig-071|71]], [[fig-072|72]], [[fig-073|73]] | -| 4.4.4 | Effetto del design bottle brush | r.1230 | [[ciclovoltammetria]] | - | +| 4.4.3 | Proprietà elettrochimiche dei copolimeri lienari | r.1175 | [[cv-risultati-copolimeri]] | [[fig-071|71]], [[fig-072|72]], [[fig-073|73]] | +| 4.4.4 | Effetto del design bottle brush | r.1230 | [[cv-risultati-bottle-brush]] | - | | 4.5 | Caratterizzazione spettroscopica allo stato solido | r.1254 | [[acq-e-stato-solido]] | [[fig-074|74]] | | 5 | Conclusioni | r.1279 | [[overview]], [[bottle-brush]] | - | From 8e9bee49d4fe1e5c17f879e5bd1559758f0ac7cc Mon Sep 17 00:00:00 2001 From: Davide Grilli Date: Fri, 9 Oct 2026 22:57:16 +0200 Subject: [PATCH 4/5] Riorganizza la wiki: spezza dpp-reattivita, unisce cv-risultati, sposta reagenti-e-materiali - dpp-reattivita -> dpp-reattivita + dpp-arilazione-litiazione-snar - cv-risultati-copolimeri + cv-risultati-bottle-brush -> cv-risultati - reagenti-e-materiali da compounds/ a techniques/ - rimossi i .gitkeep; aggiornati index, tesi, CLAUDE.md, log Co-Authored-By: Claude Sonnet 5.5 --- CLAUDE.md | 2 +- index.md | 8 +-- log.md | 6 ++ wiki/analyses/.gitkeep | 0 wiki/analyses/difetti-noti.md | 2 +- wiki/compounds/.gitkeep | 0 wiki/compounds/bottle-brush-3-x.md | 4 +- wiki/compounds/copolimeri-3a-3b-3c.md | 4 +- wiki/concepts/.gitkeep | 0 wiki/concepts/bottle-brush.md | 2 +- .../dpp-arilazione-litiazione-snar.md | 62 +++++++++++++++++++ wiki/concepts/dpp-reattivita.md | 55 +++------------- ...optoelettronica-oled-donatore-accettore.md | 2 +- wiki/dati.md | 4 +- wiki/overview.md | 2 +- wiki/techniques/.gitkeep | 0 wiki/techniques/ciclovoltammetria.md | 4 +- wiki/techniques/cv-risultati-bottle-brush.md | 35 ----------- ...isultati-copolimeri.md => cv-risultati.md} | 40 +++++++++--- .../reagenti-e-materiali.md | 0 wiki/tesi.md | 12 ++-- 21 files changed, 128 insertions(+), 116 deletions(-) delete mode 100644 wiki/analyses/.gitkeep delete mode 100644 wiki/compounds/.gitkeep delete mode 100644 wiki/concepts/.gitkeep create mode 100644 wiki/concepts/dpp-arilazione-litiazione-snar.md delete mode 100644 wiki/techniques/.gitkeep delete mode 100644 wiki/techniques/cv-risultati-bottle-brush.md rename wiki/techniques/{cv-risultati-copolimeri.md => cv-risultati.md} (63%) rename wiki/{compounds => techniques}/reagenti-e-materiali.md (100%) diff --git a/CLAUDE.md b/CLAUDE.md index d75b358..8fc1b1f 100644 --- a/CLAUDE.md +++ b/CLAUDE.md @@ -81,7 +81,7 @@ status: draft | stable - `compounds` nel catalogo sono numeri della tesi; `concepts` sono slug candidati, non nomi definitivi: crea la pagina solo se la regola dei ≥2 usi è soddisfatta. ## Regole di organizzazione dei dati -- Pagine sopra ~1.500 parole vanno spezzate per argomento (es. `ciclovoltammetria` = metodo; i risultati in `cv-risultati-*`). +- Pagine sopra ~1.500 parole vanno spezzate per argomento (es. `ciclovoltammetria` = metodo; i risultati in `cv-risultati`). - Una tabella o un dato sta in **una sola pagina**: quella dove la tesi lo discute (per es. Tab. 5 in `dpp-2`, Tab. 13-14 in `ciclovoltammetria`). Le altre pagine rimandano con wikilink; fanno eccezione i riepiloghi comparativi (es. in `uv-vis-fluorescenza`), che citano la tabella di origine. - Le pagine riorganizzano per argomento, non per capitolo, senza eliminare informazioni: procedure con quantità in tabella, condizioni, assegnazioni e ragionamenti della tesi restano, con `tesi_loc` e righe. - Composti sperimentali: `dpp-1`, `dpp-2`, `copolimeri-3a-3b-3c`, `bottle-brush-3-x`. La numerazione dei composti del cap. 1 (1-48) è un'altra: non confonderle. diff --git a/index.md b/index.md index c72ac41..e2a88c6 100644 --- a/index.md +++ b/index.md @@ -13,7 +13,8 @@ _Catalogo di tutte le pagine. Aggiornato a ogni ingest/query. Pagine curate: 28 ## Concetti - [[acq-e-stato-solido]] — ACQ, evidenza sui film, aggregati H/J, misura sul polimero 3.2b - [[bottle-brush]] — logica di progetto, sequenza di sintesi, cosa dimostrano i dati -- [[dpp-reattivita]] — siti reattivi, N-alchilazione, cross-coupling, arilazioni, litiazione, SNAr +- [[dpp-arilazione-litiazione-snar]] — arilazione diretta e ossidativa, litiazione in C5, SNAr +- [[dpp-reattivita]] — siti reattivi, N-alchilazione, SE-Ar, cross-coupling Suzuki/Stille - [[dpp-sintesi-letteratura]] — Farnum, Iqbal, Closs-Gompper, Sprake, Langhals - [[dpp-struttura-e-proprieta]] — struttura, impaccamento, Tab. 2, lavoro precedente del gruppo - [[fluorescenza]] — Jablonski, Stokes, resa quantica, tempi di vita (Eq. 1-5) @@ -27,16 +28,15 @@ _Catalogo di tutte le pagine. Aggiornato a ogni ingest/query. Pagine curate: 28 - [[copolimeri-3a-3b-3c]] — copolimeri DPP-3HT (Tab. 3, 6-8, procedura) - [[dpp-1]] — DPP tiofenico (procedura, pseudo-Stobbe, spettri) - [[dpp-2]] — monomero bis-idrossiesil (procedura, N-alchilazione, Tab. 5) -- [[reagenti-e-materiali]] — reagenti per passaggio e trattamento dei solventi ## Tecniche - [[ciclovoltammetria]] — teoria (Eq. 6-8), procedura, metodo di analisi (Eq. 11-12) -- [[cv-risultati-bottle-brush]] — Tab. 14, bandgap 0,929-1,521 eV -- [[cv-risultati-copolimeri]] — Tab. 13, correlazione bandgap/% DPP, confronto con P3HT +- [[cv-risultati]] — Tab. 13 (bandgap 0,970-1,371 eV, correlazione con % DPP, confronto con P3HT) e Tab. 14 (bottle brush, 0,929-1,521 eV) - [[dsc]] — programma termico e risultati - [[ft-ir]] — bande diagnostiche - [[gpc]] — condizioni e interpretazione della sottostima - [[nmr-1h]] — %DPP (Eq. 9) e peso molecolare (Eq. 10) +- [[reagenti-e-materiali]] — reagenti per passaggio e trattamento dei solventi - [[uv-vis-fluorescenza]] — riepilogo dei dati ottici in soluzione ## Figure diff --git a/log.md b/log.md index 2d6c897..d1ca4bc 100644 --- a/log.md +++ b/log.md @@ -39,3 +39,9 @@ _Append-only. Formato: `## [YYYY-MM-DD] tipo | titolo`_ - `ciclovoltammetria` (2.065 parole) -> `ciclovoltammetria` (teoria, procedura, metodo) + `cv-risultati-copolimeri` (Tab. 13) + `cv-risultati-bottle-brush` (Tab. 14) - `wiki/dati.md`: indice grandezza -> pagina; regola: pagine > ~1.500 parole si spezzano; lint con `scripts/lint.py` + +## [2026-10-09] schema | Riorganizzazione file wiki (approvata dall'utente) +- `dpp-reattivita` (1.620 parole) -> `dpp-reattivita` (siti reattivi, N-alchilazione, SE-Ar, Suzuki/Stille; r.247-331) + `dpp-arilazione-litiazione-snar` (arilazione diretta/ossidativa, litiazione, SNAr; r.333-369) +- `cv-risultati-copolimeri` + `cv-risultati-bottle-brush` -> `techniques/cv-risultati` (Tab. 13 e 14); link in entrata aggiornati +- `compounds/reagenti-e-materiali` -> `techniques/reagenti-e-materiali` (non è un composto numerato) +- Rimossi i `.gitkeep`; CLAUDE.md, `index.md`, `wiki/tesi.md` aggiornati. Lasciate invariate `dpp-sintesi-letteratura` (1.515) e `fluorofori-in-polimeri` diff --git a/wiki/analyses/.gitkeep b/wiki/analyses/.gitkeep deleted file mode 100644 index e69de29..0000000 diff --git a/wiki/analyses/difetti-noti.md b/wiki/analyses/difetti-noti.md index e2152f7..988720e 100644 --- a/wiki/analyses/difetti-noti.md +++ b/wiki/analyses/difetti-noti.md @@ -57,7 +57,7 @@ Anche: la didascalia di [[fig-004|Fig. 4]] dice «sale di zinco derivato dall'in 3. **Dati ottici di [[dpp-2]].** §3.2 (r.624-626): UV-Vis 541 nm, fluorescenza **540 nm**. Tabella 5: λabs 541, λex **555**, Stokes 14. Inoltre il testo (r.810) dice «Stokes shift ... simile per entrambi i fluorofori e vale circa 14 nm», mentre la tabella dà 11 nm per 1 e 14 nm per 2. 4. **Integrazioni ¹H-NMR in §3.2.** Per **1** (r.602): 4H + 4H + 4H = 12H, mentre il DPP 1 ha 6 H tiofenici (più 2 NH, non riportati nella lista). Per **2** (r.620): aromatici 1H + 1H + 2H = 4H, mentre i tiofeni sono 6 H. _(verifica sulla struttura; i dati originali non sono disponibili in `raw/`)_ 5. **Fusione dei copolimeri lineari.** §4.2 (r.954): DSC senza transizioni di fusione, Tg ≈ −10 °C. Conclusioni (r.1283): «transizioni vetrose intorno a −10 °C e temperature di fusione superiori a 110 °C». Vedi [[dsc]]. -6. **Bandgap nelle Conclusioni.** r.1289: correlazione lineare con R² = 0,9719 «tra la percentuale reale di DPP ... e l'allargamento del bandgap (da 3,42 eV a oltre 4,30 eV)». Tabella 13 ([[cv-risultati-copolimeri]]): 0,970 / 1,316 / 1,371 eV. R² non compare altrove nel testo. +6. **Bandgap nelle Conclusioni.** r.1289: correlazione lineare con R² = 0,9719 «tra la percentuale reale di DPP ... e l'allargamento del bandgap (da 3,42 eV a oltre 4,30 eV)». Tabella 13 ([[cv-risultati]]): 0,970 / 1,316 / 1,371 eV. R² non compare altrove nel testo. 7. **Pesi molecolari via ¹H-NMR (Tab. 12).** Il testo (r.1078) li definisce «molto più vicini ai valori teorici» rispetto alla GPC, ma 3.3b = 88000 Da vs 34500 teorico (≈2,5×), 3.1c = 18200 vs 10000, 3.3c = 41300 vs 55000 (inferiore al teorico). Vedi [[bottle-brush-3-x]]. 8. **Aritmetica CV.** Le Tabelle 13 e 14 sono state ricalcolate con le Eq. 11-12 (HOMO = −(Eonsetox + 4,8), LUMO = −(Eonsetred + 4,8), Eg = LUMO − HOMO): tutte le righe tornano entro l'arrotondamento, **tranne 3c** (Tab. 13), dove Eonsetox = 0,0006 V darebbe HOMO ≈ −4,8006 eV (tabella: −4,799) e Eg ≈ 1,373 eV (tabella: 1,371). Differenza di pochi millielettronvolt. _(controllo eseguito in questo ingest)_ 9. **Tabelle UV.** Gli Stokes shift delle Tabelle 7 e 10 coincidono con la differenza λex − λabs (controllato). diff --git a/wiki/compounds/.gitkeep b/wiki/compounds/.gitkeep deleted file mode 100644 index e69de29..0000000 diff --git a/wiki/compounds/bottle-brush-3-x.md b/wiki/compounds/bottle-brush-3-x.md index 036a377..52ccb7f 100644 --- a/wiki/compounds/bottle-brush-3-x.md +++ b/wiki/compounds/bottle-brush-3-x.md @@ -133,9 +133,9 @@ Transizioni principali pressoché costanti per tutti i polimeri, dominate dal PC ![[immagini/d2ed44d32060aa9ee04e73304940b111e53bf65cf115a93ace696933048e308b.jpg|560]] *Figura 68 - esempio di termogramma dei polimeri bottle brush realizzati (in figura l'analisi del campione 3.1c)* · [[fig-068|nota figura]] -## Ciclovoltammetria (§4.4.4) → [[cv-risultati-bottle-brush]] +## Ciclovoltammetria (§4.4.4) → [[cv-risultati]] Tabella 14: bandgap 0,929-1,521 eV. ## Collegamenti -- [[copolimeri-3a-3b-3c]] · [[rop-pcl]] · [[bottle-brush]] · [[acq-e-stato-solido]] · [[nmr-1h]] · [[ft-ir]] · [[uv-vis-fluorescenza]] · [[gpc]] · [[dsc]] · [[ciclovoltammetria]] · [[cv-risultati-bottle-brush]] · [[reagenti-e-materiali]] +- [[copolimeri-3a-3b-3c]] · [[rop-pcl]] · [[bottle-brush]] · [[acq-e-stato-solido]] · [[nmr-1h]] · [[ft-ir]] · [[uv-vis-fluorescenza]] · [[gpc]] · [[dsc]] · [[ciclovoltammetria]] · [[cv-risultati]] · [[reagenti-e-materiali]] - [[tesi]] · [[bibliografia]] diff --git a/wiki/compounds/copolimeri-3a-3b-3c.md b/wiki/compounds/copolimeri-3a-3b-3c.md index f5d95be..d0f6246 100644 --- a/wiki/compounds/copolimeri-3a-3b-3c.md +++ b/wiki/compounds/copolimeri-3a-3b-3c.md @@ -116,9 +116,9 @@ Mn 1400-2150 Da. Dati: ## DSC (r.954) → [[dsc]] Per tutti i campioni **Tg intorno a −10 °C**; a differenza del 3HT **nessuna transizione di fusione**: conferma il copolimero **random**; l'elevato disordine impedisce la cristallizzazione nonostante i bassi pesi molecolari. (Le Conclusioni parlano invece di «temperature di fusione superiori a 110 °C»: [[difetti-noti]].) -## Ciclovoltammetria → [[cv-risultati-copolimeri]] +## Ciclovoltammetria → [[cv-risultati]] Tabella 13 (bandgap 0,970 / 1,316 / 1,371 eV per 3a/3b/3c). ## Collegamenti -- [[dpp-2]] · [[polimerizzazione-ossidativa-fecl3]] · [[bottle-brush-3-x]] · [[bottle-brush]] · [[nmr-1h]] · [[ft-ir]] · [[uv-vis-fluorescenza]] · [[gpc]] · [[dsc]] · [[ciclovoltammetria]] · [[cv-risultati-copolimeri]] · [[reagenti-e-materiali]] +- [[dpp-2]] · [[polimerizzazione-ossidativa-fecl3]] · [[bottle-brush-3-x]] · [[bottle-brush]] · [[nmr-1h]] · [[ft-ir]] · [[uv-vis-fluorescenza]] · [[gpc]] · [[dsc]] · [[ciclovoltammetria]] · [[cv-risultati]] · [[reagenti-e-materiali]] - [[tesi]] · [[bibliografia]] diff --git a/wiki/concepts/.gitkeep b/wiki/concepts/.gitkeep deleted file mode 100644 index e69de29..0000000 diff --git a/wiki/concepts/bottle-brush.md b/wiki/concepts/bottle-brush.md index 8c19e90..1f57e71 100644 --- a/wiki/concepts/bottle-brush.md +++ b/wiki/concepts/bottle-brush.md @@ -45,7 +45,7 @@ Serie preparate da **3b** e **3c**; il copolimero **3a** non è stato usato per | Integrità del core in soluzione | λmax abs 544-554 nm, em 557-564 nm, Stokes shift 8-14 nm | [[uv-vis-fluorescenza]] | | Emissione allo stato solido | spettro SS di 3.2b: abs 570-580 nm, em ~650-660 nm | [[acq-e-stato-solido]] | | Proprietà termiche | dominate dal PCL: Tm 55-60 °C, Tc 25-35 °C | [[dsc]] | -| Elettroattività | processi redox EC irreversibili; bandgap 0,929-1,521 eV | [[ciclovoltammetria]], [[cv-risultati-bottle-brush]] | +| Elettroattività | processi redox EC irreversibili; bandgap 0,929-1,521 eV | [[ciclovoltammetria]], [[cv-risultati]] | ## Messaggio conclusivo (§5, r.1291) «L'approccio ortogonale basato su scheletri semiconduttori DPP-3HT modificati mediante catene laterali di PCL consente di combinare proprietà elettrochimiche modulabili e capacità emissiva allo stato solido.» diff --git a/wiki/concepts/dpp-arilazione-litiazione-snar.md b/wiki/concepts/dpp-arilazione-litiazione-snar.md new file mode 100644 index 0000000..602c44b --- /dev/null +++ b/wiki/concepts/dpp-arilazione-litiazione-snar.md @@ -0,0 +1,62 @@ +--- +title: DPP - arilazione, litiazione e SNAr +type: concept +tags: [dpp, arilazione, litiazione, snar] +created: 2026-10-09 +updated: 2026-10-09 +tesi_loc: "§1.1.2 r.333-369" +refs: [27, 28, 29, 30, 31, 32] +figures: ["fig-021", "fig-025", "fig-026", "fig-027", "fig-029", "fig-030"] +status: draft +--- + +# DPP - arilazione, litiazione e SNAr + +Terza parte del §1.1.2; prosegue [[dpp-reattivita]] (siti reattivi, N-alchilazione, SE-Ar, cross-coupling Suzuki/Stille). Numerazione dei composti: quella del cap. 1, non quella dei composti sperimentali ([[dpp-1]], [[dpp-2]]). Figure con numerazione dubbia: [[fig-026|Fig. 26]], [[fig-027|Fig. 27]], [[fig-029|Fig. 29]] (vedi [[difetti-noti]]). + +## 3b. Arilazione diretta (r.333-341) +- Accoppiamento di alogenuri arilici (spesso bromuri) con areni **senza pre-attivazione**, con catalizzatore al Pd e base: un CH del primo arene si condensa con l'unità C-Br del secondo, formando un legame arilico e HBr (neutralizzato dalla base). La regioselettività dipende da distribuzione di densità elettronica, acidità degli H, eteroatomi o altri gruppi funzionali (rif. [[27-mcglacken-2009|27]]). +- Marder e Chen (rif. [[29-liu-2013|29]]), due studi indipendenti: precursore **29** con diversi bromoareni ([[fig-025|Fig. 25]]). +- **Condizioni**: Pd(OAc)2 + acido pivalico, K2CO3 (neutralizza HBr), solvente **DMA** → prodotti **38 (a-h)**. Arilazione **selettiva in C5 dell'anello tiofenico**, nessun regioisomero identificato. +- Gryko et al.: efficace sia con bromoareni elettron-ricchi sia elettron-poveri, anche quando il bromuro è il DPP stesso (rese minori) ([[fig-026|Fig. 26]]). + +![[immagini/b60b2ed0441c7e89ab38e779618c5eee49a9df36d82e5122da708a9b7c78cbd2.jpg|560]] +*Figura 25 - reazione di arilazione diretta del DPP 29 con diversi bromoarili* · [[fig-025|nota figura]] + +![[immagini/5968c5669dcfd68fd60100a31f5074a12c690f0b4cc45063e8f2b25b4afd949d.jpg|560]] +*Figura 26 - arilazione dei DPP di-brorumati con diversi areni* · [[fig-026|nota figura]] + +## 3b. Arilazione ossidativa (r.347-361) +- Procede per attivazione dei legami C-H di entrambi i reagenti, senza pre-attivazione (rif. [[28-ofial-2011|28]]); il legame biarilico si forma per ossidazione di due C-H aromatici attivati dal Pd. Usato da Marder per il DPP **29**. +- Con polifluorurati poveri di elettroni, **Pd(OAc)2** e **Ag2CO3** (ossidante) → derivati coniugati **42 (a-c)** ([[fig-027|Fig. 27]]). +- Resa migliore **79%** per il composto **45a** (tetrafluoropiridina + DPP **29**). Reattività minore con pentafluorobenzene (**23%**) e tetrafluorobenzonitrile (**45%**). +- Criticità: l'uso massiccio di ossidanti come Ag2CO3. Alternativa più economica per polimeri coniugati con DPP affiancato da tiofeni (come **29**): polimerizzazione ossidativa con FeCl3 → [[polimerizzazione-ossidativa-fecl3]]. + +![[immagini/8344868ae6e8de1151d7f70a43a30b2c1557784a0e8b48edd4a99431390092bd.jpg|560]] +*Figura 27 - reazione di arilazione ossidativa* · [[fig-027|nota figura]] + +## 4. Litiazione in C5 (r.363) +I DPP **29**, **30**, **31** ([[fig-021|Fig. 21]]) reagiscono con **LDA** ([[fig-029|Fig. 29]]): + +| Elettrofilo | Prodotto | Rif. | +|---|---|---| +| formammidi (N-formilpiperidina o DMF) | dialdeide **43** | [[30-hong-2012\|30]] | +| 2-isopropossi-4,4,5,5-tetrametil-1,3,2-diossaborolano | diestere boronico **44** | [[31-burckstummer-2011\|31]] | +| cloruro di trimetilstagno | stannano **45** | [[32-hu-2012\|32]] | +| I2 (quenching) | di-iodurato **46** (buone rese) | [[31-burckstummer-2011\|31]] | + +**44** e **45** sono utili per successivi cross-coupling. Nell'immagine di [[fig-029|Fig. 29]], **45** è il derivato SnMe3; controllare la numerazione (nota del catalogo). + +![[immagini/eed9eb52dc858b172c4f6739c7b9f352bfa0e7ab10e422129a877a929c4e45bf.jpg|560]] +*Figura 29 - reazione di litiazione e funzionalizzazione con successiva reazione con elettrofili* · [[fig-029|nota figura]] + +## 5. Sostituzione nucleofila aromatica, SNAr (r.369) +- Avviene senza catalizzatori al Pd, su DPP con buoni gruppi uscenti sugli anelli aromatici. Il core di-lattamico è elettron-attrattore. +- Numerosi esempi in letteratura in cui i composti **27** e **47** reagiscono con ammine secondarie, ad alta temperatura in autoclave, dando i sistemi amminici **48 (a-d)** ([[fig-030|Fig. 30]]). + +![[immagini/5efb58f7f7d27a0467d9f14cd5191b3aeb168710c69f6fb0a27ac0cb188b2eac.jpg|560]] +*Figura 30 - sostituzione aromatica classica su derivati di DPP* · [[fig-030|nota figura]] + +## Collegamenti +- [[dpp-reattivita]] · [[dpp-struttura-e-proprieta]] · [[dpp-sintesi-letteratura]] · [[polimerizzazione-ossidativa-fecl3]] +- [[tesi]] · [[bibliografia]] diff --git a/wiki/concepts/dpp-reattivita.md b/wiki/concepts/dpp-reattivita.md index 7b4795b..3737484 100644 --- a/wiki/concepts/dpp-reattivita.md +++ b/wiki/concepts/dpp-reattivita.md @@ -1,12 +1,12 @@ --- title: DPP - reattività e funzionalizzazione type: concept -tags: [dpp, reattività, n-alchilazione, cross-coupling, arilazione, litiazione, snar] +tags: [dpp, reattività, n-alchilazione, cross-coupling] created: 2026-10-09 updated: 2026-10-09 -tesi_loc: "§1.1.2 r.247-373" -refs: [2, 5, 7, 21, 22, 23, 24, 25, 26, 27, 28, 29, 30, 31, 32] -figures: ["fig-017", "fig-018", "fig-019", "fig-020", "fig-021", "fig-022", "fig-023", "fig-024", "fig-025", "fig-026", "fig-027", "fig-029", "fig-030"] +tesi_loc: "§1.1.2 r.247-331" +refs: [2, 5, 7, 21, 22, 23, 24, 25, 26, 27, 28] +figures: ["fig-017", "fig-018", "fig-019", "fig-020", "fig-021", "fig-022", "fig-023", "fig-024"] status: draft --- @@ -14,7 +14,7 @@ status: draft Seconda parte del §1.1.2. «Nei paragrafi successivi sono riportate le reazioni che più comunemente vengono effettuate su questa famiglia di molecole, alcune delle quali utilizzate nel corso dell'attività sperimentale» (r.257). La reattività è varia per via dei diversi centri reattivi e del grande numero di sostituenti introducibili sull'anello aromatico (rif. [[07-grzybowski-2015|7]], r.247). -> **Numerazione.** I composti di questa pagina (22-48...) usano la numerazione del cap. 1, diversa da quella dei composti sperimentali 1 e 2 ([[dpp-1]], [[dpp-2]]). Figure con numerazione dubbia: [[fig-026|Fig. 26]], [[fig-027|Fig. 27]], [[fig-029|Fig. 29]] (vedi [[difetti-noti]]). +> **Numerazione.** I composti di questa pagina (22-48...) usano la numerazione del cap. 1, diversa da quella dei composti sperimentali 1 e 2 ([[dpp-1]], [[dpp-2]]). ## Mappa dei siti reattivi ([[fig-017|Fig. 17]], r.249-255; rif. [[02-shaikh-2022|2]]) Due macrocategorie. @@ -80,50 +80,9 @@ I sostituenti arilici derivanti dai benzonitrili di partenza sono considerati pa ![[immagini/967a337ba86d6286aa8b01f0989b91a248a31a2a91baafc916325bc124f4bb46.jpg|560]] *Figura 24 - sintesi generica di polimeri a base di DPP mediante reazioni di cross coupling* · [[fig-024|nota figura]] -### Arilazione diretta (r.333-341) -- Accoppiamento di alogenuri arilici (spesso bromuri) con areni **senza pre-attivazione**, con catalizzatore al Pd e base: un CH del primo arene si condensa con l'unità C-Br del secondo, formando un legame arilico e HBr (neutralizzato dalla base). La regioselettività dipende da distribuzione di densità elettronica, acidità degli H, eteroatomi o altri gruppi funzionali (rif. [[27-mcglacken-2009|27]]). -- Marder e Chen (rif. [[29-liu-2013|29]]), due studi indipendenti: precursore **29** con diversi bromoareni ([[fig-025|Fig. 25]]). -- **Condizioni**: Pd(OAc)2 + acido pivalico, K2CO3 (neutralizza HBr), solvente **DMA** → prodotti **38 (a-h)**. Arilazione **selettiva in C5 dell'anello tiofenico**, nessun regioisomero identificato. -- Gryko et al.: efficace sia con bromoareni elettron-ricchi sia elettron-poveri, anche quando il bromuro è il DPP stesso (rese minori) ([[fig-026|Fig. 26]]). - -![[immagini/b60b2ed0441c7e89ab38e779618c5eee49a9df36d82e5122da708a9b7c78cbd2.jpg|560]] -*Figura 25 - reazione di arilazione diretta del DPP 29 con diversi bromoarili* · [[fig-025|nota figura]] - -![[immagini/5968c5669dcfd68fd60100a31f5074a12c690f0b4cc45063e8f2b25b4afd949d.jpg|560]] -*Figura 26 - arilazione dei DPP di-brorumati con diversi areni* · [[fig-026|nota figura]] - -### Arilazione ossidativa (r.347-361) -- Procede per attivazione dei legami C-H di entrambi i reagenti, senza pre-attivazione (rif. [[28-ofial-2011|28]]); il legame biarilico si forma per ossidazione di due C-H aromatici attivati dal Pd. Usato da Marder per il DPP **29**. -- Con polifluorurati poveri di elettroni, **Pd(OAc)2** e **Ag2CO3** (ossidante) → derivati coniugati **42 (a-c)** ([[fig-027|Fig. 27]]). -- Resa migliore **79%** per il composto **45a** (tetrafluoropiridina + DPP **29**). Reattività minore con pentafluorobenzene (**23%**) e tetrafluorobenzonitrile (**45%**). -- Criticità: l'uso massiccio di ossidanti come Ag2CO3. Alternativa più economica per polimeri coniugati con DPP affiancato da tiofeni (come **29**): polimerizzazione ossidativa con FeCl3 → [[polimerizzazione-ossidativa-fecl3]]. - -![[immagini/8344868ae6e8de1151d7f70a43a30b2c1557784a0e8b48edd4a99431390092bd.jpg|560]] -*Figura 27 - reazione di arilazione ossidativa* · [[fig-027|nota figura]] - -## 4. Litiazione in C5 (r.363) -I DPP **29**, **30**, **31** ([[fig-021|Fig. 21]]) reagiscono con **LDA** ([[fig-029|Fig. 29]]): - -| Elettrofilo | Prodotto | Rif. | -|---|---|---| -| formammidi (N-formilpiperidina o DMF) | dialdeide **43** | [[30-hong-2012\|30]] | -| 2-isopropossi-4,4,5,5-tetrametil-1,3,2-diossaborolano | diestere boronico **44** | [[31-burckstummer-2011\|31]] | -| cloruro di trimetilstagno | stannano **45** | [[32-hu-2012\|32]] | -| I2 (quenching) | di-iodurato **46** (buone rese) | [[31-burckstummer-2011\|31]] | - -**44** e **45** sono utili per successivi cross-coupling. Nell'immagine di [[fig-029|Fig. 29]], **45** è il derivato SnMe3; controllare la numerazione (nota del catalogo). - -![[immagini/eed9eb52dc858b172c4f6739c7b9f352bfa0e7ab10e422129a877a929c4e45bf.jpg|560]] -*Figura 29 - reazione di litiazione e funzionalizzazione con successiva reazione con elettrofili* · [[fig-029|nota figura]] - -## 5. Sostituzione nucleofila aromatica, SNAr (r.369) -- Avviene senza catalizzatori al Pd, su DPP con buoni gruppi uscenti sugli anelli aromatici. Il core di-lattamico è elettron-attrattore. -- Numerosi esempi in letteratura in cui i composti **27** e **47** reagiscono con ammine secondarie, ad alta temperatura in autoclave, dando i sistemi amminici **48 (a-d)** ([[fig-030|Fig. 30]]). - -![[immagini/5efb58f7f7d27a0467d9f14cd5191b3aeb168710c69f6fb0a27ac0cb188b2eac.jpg|560]] -*Figura 30 - sostituzione aromatica classica su derivati di DPP* · [[fig-030|nota figura]] +Seguito (arilazione diretta e ossidativa, litiazione in C5, SNAr): [[dpp-arilazione-litiazione-snar]]. ## Collegamenti -- [[dpp-struttura-e-proprieta]] · [[dpp-sintesi-letteratura]] · [[polimerizzazione-ossidativa-fecl3]] +- [[dpp-arilazione-litiazione-snar]] · [[dpp-struttura-e-proprieta]] · [[dpp-sintesi-letteratura]] - [[dpp-2]] (N-alchilazione applicata in tesi) - [[tesi]] · [[bibliografia]] diff --git a/wiki/concepts/optoelettronica-oled-donatore-accettore.md b/wiki/concepts/optoelettronica-oled-donatore-accettore.md index b5073ef..d3c8ed9 100644 --- a/wiki/concepts/optoelettronica-oled-donatore-accettore.md +++ b/wiki/concepts/optoelettronica-oled-donatore-accettore.md @@ -34,7 +34,7 @@ Cap. 1.4 «Applicazioni». Sul perché serve evitare l'ACQ in questi dispositivi ## Scelta DPP + 3HT nella tesi (r.520-522) - Il nucleo elettron-accettore del DPP è combinato con unità di **3-esiltiofene (3HT)**, fortemente elettron-donatrici. - Il tiofene è partner elettronico ideale per ibridare gli orbitali di frontiera del DPP e, con la catena esilica laterale, garantisce **solubilità** e quindi processabilità (rif. [[49-hendriks-2013|49]]). -- La sinergia D-A DPP/3HT permette di sintonizzare la struttura a bande: requisiti per un impiego come **strato elettro-luminescente in OLED**. Dati reali del band gap: [[cv-risultati-copolimeri]], [[cv-risultati-bottle-brush]]. Sintesi: [[copolimeri-3a-3b-3c]]. +- La sinergia D-A DPP/3HT permette di sintonizzare la struttura a bande: requisiti per un impiego come **strato elettro-luminescente in OLED**. Dati reali del band gap: [[cv-risultati]]. Sintesi: [[copolimeri-3a-3b-3c]]. ## Struttura di un OLED (r.524-528) - Architettura multistrato (sandwich) per ottimizzare iniezione, trasporto e ricombinazione di carica. I primi dispositivi a singolo strato avevano efficienze ridotte per forte sbilanciamento tra mobilità di elettroni e lacune. diff --git a/wiki/dati.md b/wiki/dati.md index 9858742..78c0985 100644 --- a/wiki/dati.md +++ b/wiki/dati.md @@ -49,8 +49,8 @@ Mappa «grandezza → dove sta». I valori restano nelle pagine indicate (una ta |---|---|---|---| | Tg | 3a-c | ≈ −10 °C | [[dsc]] | | Tm, Tc | 3.1b-3.3c | 55-60 °C; 25-35 °C | [[dsc]] | -| Eonset, HOMO, LUMO, bandgap (Tab. 13) | 3a-c | bandgap 0,970-1,371 eV | [[cv-risultati-copolimeri]] | -| Idem (Tab. 14) | 3.1b-3.3c | bandgap 0,929-1,521 eV | [[cv-risultati-bottle-brush]] | +| Eonset, HOMO, LUMO, bandgap (Tab. 13) | 3a-c | bandgap 0,970-1,371 eV | [[cv-risultati]] | +| Idem (Tab. 14) | 3.1b-3.3c | bandgap 0,929-1,521 eV | [[cv-risultati]] | | Condizioni CV (elettrodi, solvente, elettrolita, scan rate) | tutti | - | [[ciclovoltammetria]] | ## Spettroscopia di struttura diff --git a/wiki/overview.md b/wiki/overview.md index 8cf0237..8223ce6 100644 --- a/wiki/overview.md +++ b/wiki/overview.md @@ -32,7 +32,7 @@ I semiconduttori π-coniugati usati nella soft optoelectronics perdono emissione | Termico | dominato dal PCL: Tm 55-60 °C, Tc 25-35 °C | [[dsc]] | | Ottico in soluzione | core DPP intatto: λabs 544-554 nm, λem 557-564 nm, Stokes shift 8-14 nm | [[uv-vis-fluorescenza]] | | Ottico allo stato solido | film lineari non emissivi; bottle brush 3.2b: assorbimento 570-580 nm, emissione ~650-660 nm; emissione nel rosso apprezzabile | [[acq-e-stato-solido]] | -| Elettrochimico | processi EC irreversibili; bandgap 0,970-1,371 eV (lineari, crescente con la % di DPP) e 0,929-1,521 eV (bottle brush) | [[ciclovoltammetria]], [[cv-risultati-copolimeri]], [[cv-risultati-bottle-brush]] | +| Elettrochimico | processi EC irreversibili; bandgap 0,970-1,371 eV (lineari, crescente con la % di DPP) e 0,929-1,521 eV (bottle brush) | [[ciclovoltammetria]], [[cv-risultati]] | ## Conclusione della tesi (§5, r.1291) L'approccio ortogonale basato su scheletri semiconduttori DPP-3HT modificati con catene laterali di PCL combina **proprietà elettrochimiche modulabili** e **capacità emissiva allo stato solido**, con potenziale per dispositivi optoelettronici. diff --git a/wiki/techniques/.gitkeep b/wiki/techniques/.gitkeep deleted file mode 100644 index e69de29..0000000 diff --git a/wiki/techniques/ciclovoltammetria.md b/wiki/techniques/ciclovoltammetria.md index 72c6c9a..cdd1004 100644 --- a/wiki/techniques/ciclovoltammetria.md +++ b/wiki/techniques/ciclovoltammetria.md @@ -12,7 +12,7 @@ status: draft # Ciclovoltammetria (CV) -La CV è una tecnica elettrochimica dinamica della famiglia delle voltammetriche, usata per studiare i processi redox; per materiali macromolecolari e coniugati serve a indagare trasferimento elettronico, stabilità elettrochimica e **gap energetico elettrochimico** (§4.4, r.1102-1104). Questa pagina contiene teoria, procedura e metodo di analisi. Risultati: [[cv-risultati-copolimeri]] (Tab. 13) e [[cv-risultati-bottle-brush]] (Tab. 14). +La CV è una tecnica elettrochimica dinamica della famiglia delle voltammetriche, usata per studiare i processi redox; per materiali macromolecolari e coniugati serve a indagare trasferimento elettronico, stabilità elettrochimica e **gap energetico elettrochimico** (§4.4, r.1102-1104). Questa pagina contiene teoria, procedura e metodo di analisi. Risultati: [[cv-risultati]] (Tab. 13 e 14). ## 1. Principi teorici (§3.3, r.668-699) - A differenza delle tecniche in stato stazionario il potenziale varia in modo continuo nel tempo (strumento utile per i meccanismi di trasferimento elettronico). @@ -108,5 +108,5 @@ $$ **Equazione 12** - *bandgap elettrochimico* ## Collegamenti -- [[cv-risultati-copolimeri]] · [[cv-risultati-bottle-brush]] · [[copolimeri-3a-3b-3c]] · [[bottle-brush-3-x]] · [[optoelettronica-oled-donatore-accettore]] · [[bottle-brush]] +- [[cv-risultati]] · [[copolimeri-3a-3b-3c]] · [[bottle-brush-3-x]] · [[optoelettronica-oled-donatore-accettore]] · [[bottle-brush]] - [[tesi]] · [[bibliografia]] diff --git a/wiki/techniques/cv-risultati-bottle-brush.md b/wiki/techniques/cv-risultati-bottle-brush.md deleted file mode 100644 index 83ab1ba..0000000 --- a/wiki/techniques/cv-risultati-bottle-brush.md +++ /dev/null @@ -1,35 +0,0 @@ ---- -title: CV - risultati sui polimeri bottle brush (3.1b-3.3c) -type: technique -tags: [cv, bandgap, homo-lumo, bottle-brush] -created: 2026-10-09 -updated: 2026-10-09 -tesi_loc: "§4.4.4 r.1230-1251" -refs: [] -figures: [] -status: draft ---- - -# CV - risultati sui polimeri bottle brush (3.1b-3.3c) - -Risultati della [[ciclovoltammetria]] sui [[bottle-brush-3-x]]. Metodo: [[ciclovoltammetria]]. Termine di confronto: [[cv-risultati-copolimeri]]. - -**Tabella 14** - *dati voltammetrici dei polimeri sintetizzati* - -| Polimero | Eonsetox (V) | Eonsetred (V) | HOMO (eV) | LUMO (eV) | Bandgap (eV) | -| --- | --- | --- | --- | --- | --- | -| 3.1.b | -0,183 | -1,22 | -4,617 | -3,580 | 1,037 | -| 3.2.b | -0,175 | -1,273 | -4,625 | -3,527 | 1,098 | -| 3.3.b | -0,17 | -1,202 | -4,630 | -3,598 | 1,032 | -| 3.1.c | -0,0259 | -1,547 | -4,774 | -3,253 | 1,521 | -| 3.2.c | -0,112 | -1,531 | -4,688 | -3,269 | 1,419 | -| 3.3.c | -0,321 | -1,25 | -4,479 | -3,550 | 0,929 | - -- I bottle brush **mantengono l'elettroattività** dello scheletro: i processi redox avvengono a carico del core DPP-3HT, mentre i rami alifatici fungono da **matrice dielettrica** circostante. -- Le ingombranti catene laterali modificano HOMO e LUMO rispetto ai lineari, quindi l'ampiezza del bandgap. Attribuzione: effetti di ingombro sterico dei rami di PCL sul **grado di coplanarità locale** dello scheletro → estensione effettiva della delocalizzazione. -- Bandgap dei bottle brush in 0,929-1,521 eV: l'ingegnerizzazione con PCL «non compromette le spiccate potenzialità optoelettroniche». -- Il confronto con i lineari nel testo rimanda a «paragrafo XX (XX)», segnaposto non risolto ([[difetti-noti]]). - -## Collegamenti -- [[ciclovoltammetria]] · [[cv-risultati-copolimeri]] · [[bottle-brush-3-x]] · [[bottle-brush]] -- [[tesi]] · [[difetti-noti]] diff --git a/wiki/techniques/cv-risultati-copolimeri.md b/wiki/techniques/cv-risultati.md similarity index 63% rename from wiki/techniques/cv-risultati-copolimeri.md rename to wiki/techniques/cv-risultati.md index ba6fccb..c4806fb 100644 --- a/wiki/techniques/cv-risultati-copolimeri.md +++ b/wiki/techniques/cv-risultati.md @@ -1,19 +1,20 @@ --- -title: CV - risultati sui copolimeri lineari (3a, 3b, 3c) +title: CV - risultati sui polimeri sintetizzati type: technique -tags: [cv, bandgap, homo-lumo, onset, p3ht] +tags: [cv, bandgap, homo-lumo, onset, p3ht, bottle-brush] created: 2026-10-09 updated: 2026-10-09 -tesi_loc: "§4.4.3 r.1175-1227; §5 r.1289" +tesi_loc: "§4.4.3 r.1175-1227; §4.4.4 r.1230-1251; §5 r.1289" refs: [] figures: ["fig-071", "fig-072", "fig-073"] status: draft --- -# CV - risultati sui copolimeri lineari (3a, 3b, 3c) +# CV - risultati sui polimeri sintetizzati -Risultati della [[ciclovoltammetria]] sugli scheletri [[copolimeri-3a-3b-3c]]. Metodo di analisi (onset, ferrocene, Eq. 11-12, irreversibilità EC): [[ciclovoltammetria]]. Confronto con i bottle brush: [[cv-risultati-bottle-brush]]. Incoerenze delle Conclusioni su bandgap e R²: [[difetti-noti]] (punto 6). +Risultati della [[ciclovoltammetria]] sugli scheletri [[copolimeri-3a-3b-3c]] (Tab. 13) e sui [[bottle-brush-3-x]] (Tab. 14). Metodo di analisi (onset, ferrocene, Eq. 11-12, irreversibilità EC): [[ciclovoltammetria]]. Incoerenze delle Conclusioni su bandgap e R²: [[difetti-noti]] (punto 6). +## Copolimeri lineari 3a, 3b, 3c (§4.4.3) Scopo: capire come la **frazione reale di DPP** modula l'architettura energetica dello scheletro coniugato puro, senza gli effetti sterici/conformazionali dell'innesto. **Tabella 13** - *dati voltammetrici dei copolimeri sintetizzati* @@ -24,7 +25,7 @@ Scopo: capire come la **frazione reale di DPP** modula l'architettura energetica | 3b | 32 | 0,054 | -1,262 | -4,854 | -3,538 | 1,316 | | 3c | 35 | 0,0006 | -1,372 | -4,799 | -3,428 | 1,371 | -### Bandgap vs % DPP ([[fig-071|Fig. 71]]) +#### Bandgap vs % DPP ([[fig-071|Fig. 71]]) - All'aumentare del DPP si osserva un **allargamento progressivo del bandgap**: la variazione è governata dalla composizione stechiometrica effettiva. - La netta pendenza positiva della retta di interpolazione indica forte sensibilità alla composizione: incrementi modesti di DPP aumentano molto l'energia per le transizioni elettroniche. Lettura della tesi: l'unità DPP **riduce la lunghezza di coniugazione effettiva**, limitando la delocalizzazione π e aumentando la separazione HOMO-LUMO. - Dimostra la fattibilità di un controllo mirato del band gap calibrando il rapporto fra i due monomeri. @@ -32,7 +33,7 @@ Scopo: capire come la **frazione reale di DPP** modula l'architettura energetica ![[immagini/6c7bd8393eb8c1a329f65b7fc74e5f338a866e514455c0122a43d13ca340ded5.jpg|560]] *Figura 71 - correlazione tra bandgap elettrochimico e frazione reale di DPP nei copolimeri sintetizzati* · [[fig-071|nota figura]] -### Potenziali di picco vs % DPP ([[fig-072|Fig. 72]]) +#### Potenziali di picco vs % DPP ([[fig-072|Fig. 72]]) - **Riduzione (n-doping)**: variazione più marcata. Da 25% DPP (Epc ≈ −1 V) a 32-35% il picco si sposta tra **−1,6 V e −1,8 V**: l'inserzione di elettroni diventa termodinamicamente più sfavorita, con sovratensioni maggiori per formare i radical-anioni. - **Ossidazione (p-doping)**: impatto minore; Epa passa da ≈ **0,4 V** (minor DPP) a ≈ **0,2/0,25 V** per frazioni maggiori. - Effetto combinato: aumento della separazione tra i picchi con la % di DPP, coerente con l'aumento del bandgap. @@ -40,7 +41,7 @@ Scopo: capire come la **frazione reale di DPP** modula l'architettura energetica ![[immagini/d7a3694f2d97dcaa84465aeed07d8d26adca6a8f8ed64f7ea2bf86943b918b66.jpg|560]] *Figura 72 - correlazione tra Epicco e frazione reale di DPP nei copolimeri sintetizzati* · [[fig-072|nota figura]] -### Potenziali di onset vs % DPP ([[fig-073|Fig. 73]]) +#### Potenziali di onset vs % DPP ([[fig-073|Fig. 73]]) - Eonsetred (LUMO): da ≈ **−0,75 V** (basso DPP) a ≈ **−1,4 V** (frazioni maggiori). - Eonsetox (HOMO): da ≈ **0,25 V** a quasi **0 V** (lieve traslazione). - La progressiva separazione fra i due onset conferma l'allargamento del bandgap: la composizione agisce sistematicamente sui livelli di frontiera. @@ -48,11 +49,30 @@ Scopo: capire come la **frazione reale di DPP** modula l'architettura energetica ![[immagini/b2931ebedd31df7df3b344c25fcbb4a64aceb7b356181adecf39363e49dcb0fe.jpg|560]] *Figura 73 - correlazione tra Eonset e frazione reale di DPP nei copolimeri sintetizzati* · [[fig-073|nota figura]] -### Confronto con P3HT (r.1223-1227) +#### Confronto con P3HT (r.1223-1227) - Il P3HT omopolimero è molto elettron-ricco: ossidazione (p-doping) a potenziali accessibili, **nessun contributo faradico significativo** per la riduzione (n-doping) nella consueta finestra dei solventi organici. - Nei copolimeri il DPP, forte porzione elettron-attrattrice in un'architettura D-A, **stabilizza il LUMO**: rende favorevole l'iniezione di elettroni e giustifica le onde catodiche assenti nel P3HT. L'abbassamento del LUMO, con la modulazione dell'HOMO ad opera dei segmenti di 3HT, determina il **restringimento del bandgap** rispetto all'omopolimero. - Conclusione della tesi: la sistematicità con cui la composizione influenza la risposta termodinamica convalida l'approccio come strumento di ingegnerizzazione del materiale. +## Bottle brush 3.1b-3.3c (§4.4.4) +Termine di confronto: i copolimeri lineari sopra. + +**Tabella 14** - *dati voltammetrici dei polimeri sintetizzati* + +| Polimero | Eonsetox (V) | Eonsetred (V) | HOMO (eV) | LUMO (eV) | Bandgap (eV) | +| --- | --- | --- | --- | --- | --- | +| 3.1.b | -0,183 | -1,22 | -4,617 | -3,580 | 1,037 | +| 3.2.b | -0,175 | -1,273 | -4,625 | -3,527 | 1,098 | +| 3.3.b | -0,17 | -1,202 | -4,630 | -3,598 | 1,032 | +| 3.1.c | -0,0259 | -1,547 | -4,774 | -3,253 | 1,521 | +| 3.2.c | -0,112 | -1,531 | -4,688 | -3,269 | 1,419 | +| 3.3.c | -0,321 | -1,25 | -4,479 | -3,550 | 0,929 | + +- I bottle brush **mantengono l'elettroattività** dello scheletro: i processi redox avvengono a carico del core DPP-3HT, mentre i rami alifatici fungono da **matrice dielettrica** circostante. +- Le ingombranti catene laterali modificano HOMO e LUMO rispetto ai lineari, quindi l'ampiezza del bandgap. Attribuzione: effetti di ingombro sterico dei rami di PCL sul **grado di coplanarità locale** dello scheletro → estensione effettiva della delocalizzazione. +- Bandgap dei bottle brush in 0,929-1,521 eV: l'ingegnerizzazione con PCL «non compromette le spiccate potenzialità optoelettroniche». +- Il confronto con i lineari nel testo rimanda a «paragrafo XX (XX)», segnaposto non risolto ([[difetti-noti]]). + ## Collegamenti -- [[ciclovoltammetria]] · [[cv-risultati-bottle-brush]] · [[copolimeri-3a-3b-3c]] · [[optoelettronica-oled-donatore-accettore]] +- [[ciclovoltammetria]] · [[copolimeri-3a-3b-3c]] · [[bottle-brush-3-x]] · [[bottle-brush]] · [[optoelettronica-oled-donatore-accettore]] - [[tesi]] · [[difetti-noti]] diff --git a/wiki/compounds/reagenti-e-materiali.md b/wiki/techniques/reagenti-e-materiali.md similarity index 100% rename from wiki/compounds/reagenti-e-materiali.md rename to wiki/techniques/reagenti-e-materiali.md diff --git a/wiki/tesi.md b/wiki/tesi.md index a88e29b..2e34607 100644 --- a/wiki/tesi.md +++ b/wiki/tesi.md @@ -14,9 +14,9 @@ Sintesi e caratterizzazione di copolimeri bottle brush foto-elettro attivi. Cand ## Come è organizzata la wiki Il contenuto della tesi è riorganizzato per argomento, non per capitolo. Ogni dato sta in una sola pagina (la pagina dove la tesi lo discute), le altre rimandano. -- **Concetti**: [[bottle-brush]] (hub), [[acq-e-stato-solido]], [[dpp-struttura-e-proprieta]], [[dpp-sintesi-letteratura]], [[dpp-reattivita]], [[fluorescenza]], [[fluorofori-in-polimeri]], [[optoelettronica-oled-donatore-accettore]], [[polimerizzazione-ossidativa-fecl3]], [[rop-pcl]] -- **Composti**: [[dpp-1]], [[dpp-2]], [[copolimeri-3a-3b-3c]], [[bottle-brush-3-x]], [[reagenti-e-materiali]] -- **Tecniche**: [[nmr-1h]], [[ft-ir]], [[gpc]], [[uv-vis-fluorescenza]], [[dsc]], [[ciclovoltammetria]], [[cv-risultati-copolimeri]], [[cv-risultati-bottle-brush]] +- **Concetti**: [[bottle-brush]] (hub), [[acq-e-stato-solido]], [[dpp-struttura-e-proprieta]], [[dpp-sintesi-letteratura]], [[dpp-reattivita]], [[dpp-arilazione-litiazione-snar]], [[fluorescenza]], [[fluorofori-in-polimeri]], [[optoelettronica-oled-donatore-accettore]], [[polimerizzazione-ossidativa-fecl3]], [[rop-pcl]] +- **Composti**: [[dpp-1]], [[dpp-2]], [[copolimeri-3a-3b-3c]], [[bottle-brush-3-x]] +- **Tecniche**: [[nmr-1h]], [[ft-ir]], [[gpc]], [[uv-vis-fluorescenza]], [[dsc]], [[ciclovoltammetria]], [[cv-risultati]], [[reagenti-e-materiali]] - **Altro**: [[overview]], [[bibliografia]], [[difetti-noti]], le note delle 78 figure in `wiki/figures/` (generate da `raw/immagini.json`) ## Mappa sezioni → pagine → figure @@ -27,7 +27,7 @@ Figure: numero della tesi con link alla nota (`fig-NNN`); «schema» = i 4 file | 1 | Introduzione | r.66 | - | - | | 1.1 | Dichetopirrolopirroli | r.69 | [[dpp-struttura-e-proprieta]] | [[fig-001|1]] | | 1.1.1 | Storia e sintesi | r.84 | [[dpp-sintesi-letteratura]] | [[fig-002|2]], [[fig-003|3]], [[fig-004|4]], [[fig-005|5]], [[fig-006|6]], [[fig-007|7]], [[fig-008|8]], [[fig-009|9]], [[fig-010|10]], [[fig-011|11]], [[fig-012|12]], [[fig-013|13]], [[fig-014|14]] | -| 1.1.2 | Struttura e reattività | r.203 | [[dpp-struttura-e-proprieta]] (struttura), [[dpp-reattivita]] (reattività), [[polimerizzazione-ossidativa-fecl3]] | [[fig-015|15]], [[fig-016|16]], [[fig-017|17]], [[fig-018|18]], [[fig-019|19]], [[fig-020|20]], [[fig-021|21]], [[fig-022|22]], [[fig-023|23]], [[fig-024|24]], [[fig-025|25]], [[fig-026|26]], [[fig-027|27]], [[fig-028|28]], [[fig-029|29]], [[fig-030|30]] | +| 1.1.2 | Struttura e reattività | r.203 | [[dpp-struttura-e-proprieta]] (struttura), [[dpp-reattivita]] (reattività; r.333-369 in [[dpp-arilazione-litiazione-snar]]), [[polimerizzazione-ossidativa-fecl3]] | [[fig-015|15]], [[fig-016|16]], [[fig-017|17]], [[fig-018|18]], [[fig-019|19]], [[fig-020|20]], [[fig-021|21]], [[fig-022|22]], [[fig-023|23]], [[fig-024|24]], [[fig-025|25]], [[fig-026|26]], [[fig-027|27]], [[fig-028|28]], [[fig-029|29]], [[fig-030|30]] | | 1.2 | Fluorescenza | r.376 | [[fluorescenza]] | [[fig-031|31]], [[fig-032|32]], [[fig-033|33]] | | 1.2.1 | Shift di Stokes | r.418 | [[fluorescenza]] | [[fig-034|34]] | | 1.2.2 | Resa quantica | r.429 | [[fluorescenza]] | - | @@ -47,8 +47,8 @@ Figure: numero della tesi con link alla nota (`fig-NNN`); «schema» = i 4 file | 4.4 | Ciclovoltammetrie | r.1100 | [[ciclovoltammetria]] | - | | 4.4.1 | Ciclovoltammetrie su polimeri elettroattivi | r.1107 | [[ciclovoltammetria]] | - | | 4.4.2 | Metodologie di analisi voltammetrica | r.1118 | [[ciclovoltammetria]] | [[fig-069|69]], [[fig-070|70]] | -| 4.4.3 | Proprietà elettrochimiche dei copolimeri lienari | r.1175 | [[cv-risultati-copolimeri]] | [[fig-071|71]], [[fig-072|72]], [[fig-073|73]] | -| 4.4.4 | Effetto del design bottle brush | r.1230 | [[cv-risultati-bottle-brush]] | - | +| 4.4.3 | Proprietà elettrochimiche dei copolimeri lienari | r.1175 | [[cv-risultati]] | [[fig-071|71]], [[fig-072|72]], [[fig-073|73]] | +| 4.4.4 | Effetto del design bottle brush | r.1230 | [[cv-risultati]] | - | | 4.5 | Caratterizzazione spettroscopica allo stato solido | r.1254 | [[acq-e-stato-solido]] | [[fig-074|74]] | | 5 | Conclusioni | r.1279 | [[overview]], [[bottle-brush]] | - | From b905a14ef59c122be0eea6efb484090d40fb359d Mon Sep 17 00:00:00 2001 From: Davide Grilli Date: Fri, 9 Oct 2026 23:39:52 +0200 Subject: [PATCH 5/5] Aggiunge presentazione per la discussione e riassunto della tesi; aggiorna indice, log e figure Include slide Marp, discorso e figure in presentazione/, il riassunto in wiki/analyses/ e le modifiche pendenti a index, log, raw/ e wiki/figures. Co-Authored-By: Claude Sonnet 5.5 --- .obsidian/graph.json | 2 +- index.md | 3 +- log.md | 12 ++ presentazione/Riassunto_tesi.docx | Bin 0 -> 180393 bytes presentazione/discorso.md | 170 ++++++++++++++++ presentazione/discussione.pptx | Bin 0 -> 286172 bytes presentazione/immagini/fig1-dpp.jpg | Bin 0 -> 13200 bytes presentazione/immagini/fig2-sintesi-dpp1.jpg | Bin 0 -> 21393 bytes .../immagini/fig3-alchilazione-dpp2.jpg | Bin 0 -> 21403 bytes .../immagini/fig4-copolimerizzazione.jpg | Bin 0 -> 23421 bytes .../immagini/fig5-rop-bottle-brush.jpg | Bin 0 -> 32846 bytes presentazione/immagini/fig6-uv-em-3.2b.jpg | Bin 0 -> 52818 bytes .../immagini/fig7-bandgap-vs-dpp.jpg | Bin 0 -> 31109 bytes presentazione/riassunto_tesi.md | 110 ++++++++++ presentazione/slides.md | 189 ++++++++++++++++++ wiki/analyses/riassunto-tesi.md | 141 +++++++++++++ 16 files changed, 625 insertions(+), 2 deletions(-) create mode 100644 presentazione/Riassunto_tesi.docx create mode 100644 presentazione/discorso.md create mode 100644 presentazione/discussione.pptx create mode 100644 presentazione/immagini/fig1-dpp.jpg create mode 100644 presentazione/immagini/fig2-sintesi-dpp1.jpg create mode 100644 presentazione/immagini/fig3-alchilazione-dpp2.jpg create mode 100644 presentazione/immagini/fig4-copolimerizzazione.jpg create mode 100644 presentazione/immagini/fig5-rop-bottle-brush.jpg create mode 100644 presentazione/immagini/fig6-uv-em-3.2b.jpg create mode 100644 presentazione/immagini/fig7-bandgap-vs-dpp.jpg create mode 100644 presentazione/riassunto_tesi.md create mode 100644 presentazione/slides.md create mode 100644 wiki/analyses/riassunto-tesi.md diff --git a/.obsidian/graph.json b/.obsidian/graph.json index 83ecb44..0baffdb 100644 --- a/.obsidian/graph.json +++ b/.obsidian/graph.json @@ -17,6 +17,6 @@ "repelStrength": 10, "linkStrength": 1, "linkDistance": 250, - "scale": 0.2588386562181621, + "scale": 0.3628873693012104, "close": true } \ No newline at end of file diff --git a/index.md b/index.md index e2a88c6..aa60475 100644 --- a/index.md +++ b/index.md @@ -1,6 +1,6 @@ # Indice della wiki -_Catalogo di tutte le pagine. Aggiornato a ogni ingest/query. Pagine curate: 28 · Figure generate: 78 · Fonti ingerite: 1 (la tesi)_ +_Catalogo di tutte le pagine. Aggiornato a ogni ingest/query. Pagine curate: 29 · Figure generate: 78 · Fonti ingerite: 1 (la tesi)_ ## Overview - [[overview]] — problema, strategia, risultati dichiarati e limiti della tesi @@ -44,3 +44,4 @@ _Catalogo di tutte le pagine. Aggiornato a ogni ingest/query. Pagine curate: 28 ## Analisi - [[difetti-noti]] — difetti noti della tesi e incoerenze rilevate nell'ingest +- [[riassunto-tesi]] — riassunto in formato 10 pagine (testo continuo, 7 figure, 3 tabelle, 10 riferimenti) diff --git a/log.md b/log.md index d1ca4bc..7e3c5fb 100644 --- a/log.md +++ b/log.md @@ -45,3 +45,15 @@ _Append-only. Formato: `## [YYYY-MM-DD] tipo | titolo`_ - `cv-risultati-copolimeri` + `cv-risultati-bottle-brush` -> `techniques/cv-risultati` (Tab. 13 e 14); link in entrata aggiornati - `compounds/reagenti-e-materiali` -> `techniques/reagenti-e-materiali` (non è un composto numerato) - Rimossi i `.gitkeep`; CLAUDE.md, `index.md`, `wiki/tesi.md` aggiornati. Lasciate invariate `dpp-sintesi-letteratura` (1.515) e `fluorofori-in-polimeri` + +## [2026-10-09] query | Riassunto della tesi in formato 10 pagine +- Richiesta: riassunto secondo le regole del formato (copertina placeholder, testo continuo senza sottotitoli/elenchi, max 10 pagine, bibliografia a parte, usare la Figura 74) +- Salvato in `wiki/analyses/riassunto-tesi.md` (Fig. 74 della tesi = Figura 6 del riassunto); 7 figure, 3 tabelle, 10 riferimenti dalle schede `raw/fonti/` +- Esclusi i valori di band gap/R² delle Conclusioni (incoerenti con Tab. 13) e la durata del reflusso ROP (4 h/24 h): vedi `difetti-noti` + +## [2026-10-09] query | Seconda stesura del riassunto in registro da ricercatore +- `wiki/analyses/riassunto-tesi.md` riscritto: affermazioni non supportate rimosse (es. «forte fluorescenza in soluzione»), emissione solida di 3.2b qualificata come da specie aggregate (ACQ attenuato, non eliminato), aggiunte note critiche (copolimeri oligomerici, correlazione bandgap su 3 punti, scarto gap elettrochimico/ottico) +- Le inferenze dell'autore sono elencate nella sezione Collegamenti della pagina + +## [2026-10-09] query | Terza stesura del riassunto, allineata alla tesi +- `wiki/analyses/riassunto-tesi.md`: rimosse le inferenze della seconda stesura; contenuti e interpretazioni solo dalla tesi (limiti e prospettive dalle sezioni 4.2-4.3 e Conclusioni); per le incoerenze interne si usa il capitolo dei risultati (vedi `difetti-noti`, punti 5-7) diff --git a/presentazione/Riassunto_tesi.docx b/presentazione/Riassunto_tesi.docx new file mode 100644 index 0000000000000000000000000000000000000000..31864beed8aa7327caa5fe34934514240fcce663 GIT binary patch literal 180393 zcmZ^Kb8si^vv0VuwXtn&%#Cf^w(aB_+qP}nwry_g8HA$ z{&Y`|oFph1G|)endxg06zr=rT;D4X4whl)0a{pfznEz(cbuhMa{2xZhe|6d@?h&Clp*laK$3i}Stb}#>tMz^o0gf`M_#b+Q1 zZPvH|22iH=&_@gdv|9x+CgW2UHv{)hC0r5s-WQG`rX<e?@haCoztJ1 zd1}o0xF55R=SSEARL$W87lXtOQbQSaoA;D80%KVT&BA;cGm}`sl%3HjPUfE{%-!Ud 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zwm%gxFTeHbo3-TiS2?Rehx5Z9d92q8XV#1@trO8C%=D5Hr!7K@H{R?m|AT zL-vq?4_M=Oc|e!Cbknn%Qh}KBP*fh7YI|i**_G&MskpBsa9(`VW50ra&)%Wr36hlm zLceICWz>snUB1E1CR-raGOnSmmsQ~>FOf-3Oh|>6WD_3jg!f*3P9}89@8Lvy-~a{>7Jr2!To{SEyAep z$k~;MqvqF=^LUKWt}?ZqFP-|UU>vj)t2d=4(mk}X4d(F`G`hmc5~e-17P=2BE;$7+N;HGK8T`yUaeV}K)bFxJ=FEIg5fD37_QeBR4>tm zle-pX>RleUD8Wa)Uo77~4nD}yacZcSMHSkKq-myye5B7t0oy-`S?D`aqU&fqgGDN= zoupNrreDJvm;+A|9fx)XXRpS|?wnT_Fta4YS@4q&1mS{wF1yC#p3&7GZ2VwdVz}g` z1 Per impiegarli in un dispositivo occorre governarne le proprietà ottiche ed elettroniche, cioè ingegnerizzare il band gap. La strategia d'elezione è l'approccio donatore-accettore (D-A), che alterna unità fortemente elettron-deficienti e unità elettron-ricche lungo lo scheletro π-coniugato: l'orbitale HOMO è determinato principalmente dalla porzione donatrice e il LUMO dall'unità accettrice, e il trasferimento di carica intramolecolare che ne deriva riduce il salto energetico e permette di centrare assorbimento ed emissione nel visibile.2 + +I materiali semiconduttori π-coniugati perdono spesso le proprietà ottiche allo stato solido. La natura altamente planare del loro scheletro induce intense interazioni di π-stacking tra le catene adiacenti, che causano la drastica dissipazione non radiativa dell'energia eccitonica e lo smorzamento della fluorescenza: è l'ACQ. Questo limita le applicazioni pratiche dei materiali, perché nello strato emissivo di un OLED è richiesta proprio l'emissione. Per ovviare al problema, la tesi propone una strategia di design macromolecolare basata su architetture a spazzola (bottle brush), il cui scopo è promuovere la separazione fisica dei segmenti planari coniugati, ripristinando le proprietà emissive allo stato solido e preservando integrità elettrochimica e stabilità del sistema. + +Come unità accettrice è stato scelto il DPP, formato da due anelli lattamici a cinque termini condensati, con sostituenti aromatici o eteroaromatici in posizione 3 e 6 *(Figura 1)*. Nato come pigmento rosso industriale, il DPP ha punto di fusione superiore a 350 °C e solubilità molto bassa, dovute a un fitto network di legami a idrogeno ammidici e di π-stacking tra i piani molecolari.3 Il nucleo è planare e fortemente elettron-deficiente, e la rigidità dello scheletro limita il rilassamento vibrazionale e lo Stokes shift. Nel passaggio dalla soluzione al film il DPP mostra un allargamento della banda di assorbimento e un marcato effetto batocromico, con spostamento del picco di circa 30 nm. + +![](immagini/fig1-dpp.jpg) + +Figura 1. Struttura generica di un dichetopirrolopirrolo. + +L'inserimento di un fluoroforo in un sistema polimerico richiede un accurato design molecolare, perché l'architettura scelta influenza drasticamente le proprietà finali. Nei sistemi host-guest il fluoroforo è disperso fisicamente nella matrice: la preparazione è semplice, ma la scarsa stabilità a lungo termine, con migrazione e aggregazione dell'ospite, porta a perdita di resa quantica. Nei sistemi main-chain il fluoroforo è parte integrante della catena principale, con sintesi più complessa; una strategia riuscita è il grafting-from, in cui un DPP bifunzionalizzato con gruppi ossidrilici inizia la crescita di due catene di PCL, dando PCL-DPP-PCL.4 Nei sistemi side-chain le unità luminescenti sono catene laterali, spesso con uno spaziatore flessibile che limita le interazioni tra cromofori; nei sistemi cross-linked il cromoforo è ancorato da ponti chimici e non aggrega, ma l'eccessiva rigidità rende il materiale fragile, insolubile e difficile da lavorare. La tesi adotta il grafting-from per innestare catene laterali di PCL su uno scheletro semiconduttore DPP-3HT. + +Il monomero è un derivato del DPP definito ortogonale e tetrafunzionale: gli anelli tiofenici forniscono i siti per la polimerizzazione ossidativa dello scheletro, mentre i due gruppi ossidrilici primari, portati dalle catene esiliche sugli azoti lattamici, fungono da iniziatori per la polimerizzazione ad apertura di anello (ROP). Il gruppo aveva già studiato fluorofori DPP con sostituenti diversi in para sull'anello benzonitrilico: quelli elettron-attrattori davano sistemi altamente emissivi, quelli elettron-donatori un isomero strutturale (iso-DPP) a fluorescenza inibita. In questo lavoro i benzeni sono sostituiti da tiofeni e i gruppi ammidici sono N-alchilati, con aumento della solubilità e una procedura semplice e scalabile. Il 3HT è il comonomero donatore: i politiofeni sono tra i più efficienti polimeri semiconduttori organici5 e la catena esilica aumenta la solubilità nei solventi organici. La polimerizzazione ossidativa con FeCl3 è stata preferita ai cross-coupling al palladio perché non richiede pre-funzionalizzazione dei monomeri, opera a temperatura e pressione ambiente ed è scalabile, a fronte di un controllo minore su polidispersità e regioregolarità. La distribuzione statistica dei monomeri aumenta l'entropia conformazionale, limita il packing e rende più accessibili gli ossidrili per la funzionalizzazione. + +Il PCL è stato scelto sulla base di studi precedenti del gruppo, per la bassa temperatura di transizione vetrosa e la buona solubilità nei solventi organici; la ROP dell'ε-caprolattone catalizzata da stagno ottanoato (Sn(Oct)2) è un processo lineare ed efficiente, procede per coordinazione-inserzione con un alcol come coiniziatore e permette di regolare il peso molecolare e di mantenere bassa la dispersità delle catene.6 La lunghezza delle catene si modula con il rapporto molare monomero/ossidrili, con valori nominali di 1500, 5000 e 10000 Da. I copolimeri sono stati alimentati con il 20%, 50% e 80% in moli di DPP; i bottle brush sono stati preparati da **3b** e **3c**, mentre **3a** non è stato usato a causa della scarsa efficienza della sua via sintetica, con basse rese e difficoltà di work-up, e di volumi di solventi e costi di reagenti troppo elevati per isolarne quantità utili. + +Lo scopo del progetto è sintetizzare e caratterizzare copolimeri bottle brush foto-elettro attivi a base di DPP e 3HT con catene laterali di PCL, al fine di superare l'ACQ allo stato solido mantenendo l'integrità elettrochimica del nucleo DPP. Il lavoro comprende due macroaree: la sintesi del monomero ortogonale e l'ottenimento dei materiali, cioè scheletro coniugato e catene innestate. + +Il DPP tiofenico **1** *(Figura 2)* è stato ottenuto per ciclizzazione pseudo-Stobbe tra 2-cianotiofene e diisopropil succinato.7 La base forte è il teramilato di sodio, ottenuto dal sodio in alcol ter-amilico con FeCl3 catalitico: deprotona il succinato in α al carbonile, il carbanione attacca il carbonio nitrilico e il composto imminico tautomerizza a enammina, che attacca il carbonile estereo chiudendo il primo anello a cinque termini; una seconda deprotonazione e l'attacco di una seconda molecola di tiofene portano al secondo anello. Il succinato è stato aggiunto lentamente, perché una concentrazione locale troppo alta in condizioni basiche induce autocondensazione di Claisen, e si è scelto il diisopropil succinato per aumentare l'ingombro intorno al carbonile e ridurre questa reazione.8 Il prodotto, un solido rosso scuro violaceo, è stato purificato sfruttando la netta differenza di solubilità tra reagenti e prodotto, con lavaggi in acqua e metanolo. Il 1H-NMR in DMSO mostra a circa 11 ppm il singoletto allargato dei protoni ammidici; in THF **1** ha massimo di assorbimento a 531 nm, di emissione a 542 nm e Stokes shift di 11 nm. + +![](immagini/fig2-sintesi-dpp1.jpg) + +Figura 2. Sintesi del DPP **1** da 2-cianotiofene e diisopropil succinato con teramilato di sodio e FeCl3 catalitico. + +L'N-alchilazione di **1** con 6-bromo-1-esanolo *(Figura 3)* sfrutta la reattività dei gruppi ammidici, deprotonati da ter-butossido di potassio in DMSO, che attaccano per sostituzione nucleofila il carbonio adiacente al bromo, e dà il monomero **2** con due braccia idrossiesiliche. La tesi segnala come reazione collaterale la ciclizzazione del 6-bromo-1-esanolo, favorita da un eccesso di base. Il prodotto è stato lavato con soluzione satura di KCl e purificato per cristallizzazione da etanolo a −20 °C. L'N-alchilazione è confermata nel 1H-NMR dai multipletti alifatici a 4,1 ppm (metileni legati all'azoto lattamico) e a 3,6 ppm (metileni adiacenti all'ossidrile terminale), e nel FT-IR dalla banda larga dell'O-H a circa 3400 cm-1 insieme al C=O lattamico a circa 1650 cm-1. Il massimo di assorbimento passa da 531 nm (**1**) a 541 nm (**2**): lo spostamento batocromico è attribuito all'effetto induttivo elettron-donatore delle catene alifatiche, che arricchiscono di densità elettronica gli azoti, destabilizzano l'HOMO e restringono il band gap ottico. + +![](immagini/fig3-alchilazione-dpp2.jpg) + +Figura 3. N-alchilazione del DPP **1** con 6-bromo-1-esanolo (DMSO, ter-butossido di potassio, 40 °C) a dare il monomero **2** con due catene idrossiesiliche. + +Il monomero **2** è stato copolimerizzato con 3HT per via ossidativa, con FeCl3 in nitrometano e cloroformio anidro *(Figura 4)*. Il FeCl3, in eccesso stechiometrico, estrae per trasferimento mono-elettronico un elettrone dagli anelli tiofenici, generando cationi radicalici delocalizzati che formano i nuovi legami C-C. Il nitrometano rompe i dimeri di FeCl3 e ne modera acidità di Lewis e potere ossidante, prevenendo sovraossidazione e difetti di reticolazione; il cloroformio anidro evita che l'acqua si coordini al FeCl3 e spenga per attacco nucleofilo gli intermedi cationico-radicalici. L'ossidante è stato rimosso con lavaggi con HCl 0,6 M fino a saggio negativo del tiocianato, perché tracce di metalli di transizione abbatterebbero la mobilità dei portatori e spegnerebbero la fluorescenza, e l'omopolimero del 3HT è stato eliminato per precipitazione in metanolo freddo. L'integrazione di DPP si è limitata a un massimo del 35% *(Tabella 1)*: la tesi lo attribuisce alla differenza nei rapporti di reattività dei comonomeri, influenzata dall'ingombro sterico del DPP, mentre il tiofene, più reattivo e meno voluminoso, addiziona preferenzialmente. Le percentuali reali sono state determinate via 1H-NMR. + +![](immagini/fig4-copolimerizzazione.jpg) + +Figura 4. Copolimerizzazione ossidativa del DPP **2** con 3-esiltiofene con FeCl3 a dare i copolimeri **3a**, **3b** e **3c**. + +Tabella 1. Composizione dei copolimeri e pesi molecolari da GPC. + +| **Copolimero** | **% DPP teorica (mol/mol)** | **% DPP reale (mol/mol)** | **Mn (Da)** | **Mw (Da)** | **PD** | +|---|---|---|---|---|---| +| **3a** | 20 | 25,2 | 2149 | 5526 | 2,571 | +| **3b** | 50 | 32,6 | 1402 | 6439 | 4,592 | +| **3c** | 80 | 35,3 | 2134 | 4223 | 1,979 | + +I copolimeri hanno Mn tra 1402 e 2149 Da. Valori di PD intorno a 2 o superiori sono attesi per una polimerizzazione non controllata, con distribuzione più probabile di Flory; **3c** ha la distribuzione più omogenea (PD 1,979), mentre **3b**, con Mn più bassa ma Mw più alta, indica una frazione significativa di oligomeri a catena corta accanto a macromolecole di peso molecolare più elevato. Il FT-IR conferma l'incorporazione del DPP con il C=O lattamico a circa 1650 cm-1, e la DSC mostra per tutti i campioni una transizione vetrosa intorno a −10 °C e nessuna transizione di fusione, a conferma della natura random dei copolimeri, il cui disordine impedisce la cristallizzazione. In soluzione di THF i tre copolimeri hanno profili ottici pressoché identici, simili a quello del monomero: assorbimento tra 540 e 544 nm, emissione intorno a 550 nm e Stokes shift tra 6 e 10 nm. Allo stato solido il comportamento è drasticamente diverso: l'intenso impaccamento delle catene forma aggregati che disattivano i fluorofori per decadimento non radiativo, e i film su vetrino sotto lampada UV non mostrano emissione apprezzabile. È la principale criticità dei sistemi lineari per l'uso in dispositivi optoelettronici e giustifica il passaggio al design bottle brush. + +I sei bottle brush **3.1b**, **3.2b**, **3.3b**, **3.1c**, **3.2c** e **3.3c** sono stati ottenuti per ROP dell'ε-caprolattone dagli ossidrili di **3b** e **3c**, in toluene a 110 °C con Sn(Oct)2 catalitico, con il monomero dosato sul numero di ossidrili per ottenere catene di 1500, 5000 e 10000 Da *(Figura 5)*. L'avvenuto innesto è verificato dal 1H-NMR, con il tripletto del PCL a circa 4,0 ppm (CH2-O adiacente all'ossigeno estereo) e il segnale a 2,3 ppm dei protoni in α al carbonile, e dal FT-IR, in cui la banda dell'O-H a 3600-3200 cm-1 dei macroiniziatori scompare e compare il C=O estereo a circa 1720 cm-1. La GPC fornisce Mn tra 12188 e 21269 Da e indici di dispersità contenuti (1,238-1,521). + +![](immagini/fig5-rop-bottle-brush.jpg) + +Figura 5. Polimerizzazione ad apertura di anello dell'ε-caprolattone sui gruppi OH dei copolimeri DPP-3HT, a dare i bottle brush con catene di PCL. + +I pesi molecolari da GPC *(Tabella 2)* sono significativamente sottostimati rispetto ai teorici: la GPC separa per volume idrodinamico e restituisce valori relativi agli standard di polistirene lineare, mentre un polimero altamente ramificato assume in soluzione una conformazione compatta, con volume idrodinamico nettamente inferiore. I dati non indicano quindi il peso molecolare assoluto né una bassa resa, ma confermano indirettamente una struttura ramificata altamente impaccata e permettono il confronto tra i polimeri. Il campione **3.3c** si discosta dall'andamento generale; la tesi ipotizza che, essendo il materiale di partenza random, elevate concentrazioni locali di DPP e di ossidrili abbiano ridotto la crescita delle catene laterali per ingombro sterico, e indica che le discrepanze saranno investigate in futuro con ulteriori analisi. Per superare i limiti della GPC è stato calcolato il peso molecolare via 1H-NMR dal grado di polimerizzazione delle catene di PCL, ottenendo una stima descritta come più vicina ai valori teorici. Dal punto di vista termico, la DSC mostra per tutti i bottle brush transizioni dominate dal PCL, con fusione tra 55 e 60 °C e cristallizzazione tra 25 e 35 °C. + +Tabella 2. Pesi molecolari dei bottle brush da GPC e da 1H-NMR, con il valore teorico. + +| **Polimero** | **Mn PCL teorico (Da)** | **Mn GPC (Da)** | **PD** | **Peso molecolare teorico (Da)** | **Peso molecolare da 1H-NMR (Da)** | +|---|---|---|---|---|---| +| **3.1b** | 1500 | 12188 | 1,521 | 6500 | 8900 | +| **3.2b** | 5000 | 17302 | 1,314 | 18000 | 20500 | +| **3.3b** | 10000 | 21269 | 1,238 | 34500 | 88000 | +| **3.1c** | 1500 | 13999 | 1,301 | 10000 | 18200 | +| **3.2c** | 5000 | 19119 | 1,275 | 28500 | 35500 | +| **3.3c** | 10000 | 14445 | 1,351 | 55000 | 41300 | + +La caratterizzazione ottica in soluzione di THF mostra che la funzionalizzazione sterica non perturba l'integrità elettronica del core DPP: i massimi di assorbimento cadono tra 544 e 554 nm, quelli di emissione tra 557 e 564 nm e gli Stokes shift tra 8 e 14 nm. Le piccole fluttuazioni nelle due serie non seguono un andamento lineare con il peso molecolare del PCL e sono trascurabili, quindi l'ingombro sterico non perturba livelli energetici e natura delle transizioni. Il basso Stokes shift conferma la conservazione dell'assetto planare del cromoforo e la minima riorganizzazione tra stato fondamentale ed eccitato, e i domini flessibili di PCL allontanano le catene principali, riducendo l'impaccamento senza distorcere la geometria del backbone. + +La caratterizzazione allo stato solido è stata condotta sul campione **3.2b**, confrontando soluzione e solido *(Figura 6)*. Le misure in soluzione diluita indagano la singola catena isolata e solvatata; allo stato solido la vicinanza tra le macromolecole genera forti interazioni intermolecolari che alterano i livelli energetici e i processi di assorbimento ed emissione. In soluzione il massimo di assorbimento è a circa 550 nm e quello di emissione a circa 560-565 nm, con banda stretta e strutturata. Allo stato solido l'assorbimento mostra un significativo allargamento e un marcato effetto batocromico, con il massimo nell'intervallo 570-580 nm, attribuito alla planarizzazione dello scheletro, che estende la lunghezza di coniugazione effettiva. L'emissione è notevolmente allargata e fortemente spostata verso il rosso, con massimo centrato intorno a 650-660 nm e Stokes shift di circa 80-90 nm, probabilmente legato al maggiore ingombro delle catene, che obbliga gli anelli aromatici a torsioni maggiori, ed evidenza di una forte aggregazione intermolecolare. Secondo la tesi, dopo la fotoeccitazione l'energia migra verso siti a minore energia generati dalla vicinanza dei piani coniugati e il rilassamento radiativo avviene prevalentemente da stati aggregati o specie eccimeriche, nel quadro dell'accoppiamento eccitonico di Kasha tra aggregati H e J.9,10 Nonostante questi riarrangiamenti, l'architettura bottle brush mantiene un'apprezzabile emissione nel rosso, attenuando i percorsi di disattivazione non radiativa tipici dell'ACQ non controllato, in accordo con il ruolo del PCL come spaziatore sterico. + +![](immagini/fig6-uv-em-3.2b.jpg) + +Figura 6. Confronto tra spettri UV-Vis (in nero) ed emissione (in rosso) del polimero **3.2b** in soluzione (linea continua) e allo stato solido (linea tratteggiata). + +La ciclovoltammetria mostra per i polimeri un trasferimento di carica irreversibile di tipo elettrochimico-chimico, dovuto all'elevata reattività dei cationi e degli anioni radicali all'interfaccia elettrodica. Dagli onset di ossidazione e riduzione, calibrati sul ferrocene (posto a −4,8 eV rispetto al livello del vuoto), sono stati ricavati HOMO, LUMO e band gap elettrochimico *(Tabella 3)*. Nei copolimeri lineari si osserva un allargamento progressivo del band gap all'aumentare della frazione reale di DPP, da 0,970 a 1,371 eV *(Figura 7)*, con correlazione lineare (R² = 0,9719) guidata soprattutto dallo spostamento del potenziale di riduzione verso valori più negativi. La tesi lo interpreta come riduzione della lunghezza di coniugazione effettiva dovuta all'unità DPP, che limita la delocalizzazione π e aumenta la separazione HOMO-LUMO, e vi riconosce la possibilità di un controllo mirato del band gap calibrando il rapporto tra i monomeri. Rispetto al poli-3HT, che si ossida a potenziali accessibili ma non mostra contributi faradici in riduzione, nei copolimeri il DPP, forte porzione elettron-attrattrice in un'architettura D-A, stabilizza il LUMO e rende favorevole l'iniezione di elettroni. + +![](immagini/fig7-bandgap-vs-dpp.jpg) + +Figura 7. Correlazione tra band gap elettrochimico e frazione reale di DPP nei copolimeri lineari. + +Tabella 3. Livelli HOMO, LUMO e band gap elettrochimici dei copolimeri lineari e dei bottle brush. + +| **Polimero** | **HOMO (eV)** | **LUMO (eV)** | **Bandgap (eV)** | +|---|---|---|---| +| **3a** | -5,038 | -4,068 | 0,970 | +| **3b** | -4,854 | -3,538 | 1,316 | +| **3c** | -4,799 | -3,428 | 1,371 | +| **3.1b** | -4,617 | -3,580 | 1,037 | +| **3.2b** | -4,625 | -3,527 | 1,098 | +| **3.3b** | -4,630 | -3,598 | 1,032 | +| **3.1c** | -4,774 | -3,253 | 1,521 | +| **3.2c** | -4,688 | -3,269 | 1,419 | +| **3.3c** | -4,479 | -3,550 | 0,929 | + +I bottle brush mantengono l'elettroattività dello scheletro: i processi redox avvengono a carico del core DPP-3HT, mentre i rami alifatici fungono da matrice dielettrica circostante. Le ingombranti catene laterali modificano HOMO e LUMO rispetto ai lineari, e quindi l'ampiezza del band gap, che nei bottle brush è compresa tra 0,929 e 1,521 eV; la tesi attribuisce l'effetto all'ingombro sterico dei rami di PCL sul grado di coplanarità locale dello scheletro, e quindi sull'estensione effettiva della delocalizzazione. L'ingegnerizzazione con PCL non compromette, secondo la tesi, le spiccate potenzialità optoelettroniche del sistema. + +In conclusione, i risultati confermano secondo la tesi la validità del design proposto: l'approccio ortogonale basato su scheletri semiconduttori DPP-3HT modificati con catene laterali di PCL combina proprietà elettrochimiche modulabili e capacità emissiva allo stato solido. Dal punto di vista sintetico, monomeri ortogonali derivati dal DPP, polimerizzazione ossidativa con FeCl3 e ROP hanno portato a tre copolimeri statistici e a due serie di bottle brush con catene laterali di PCL di lunghezza nominale crescente. Il nucleo DPP conserva in soluzione le proprietà ottiche e, allo stato solido, il bottle brush **3.2b** mantiene un'apprezzabile emissione nel rosso; la composizione monomerica si rivela un parametro di controllo del band gap. I limiti dichiarati nel testo sono l'integrazione di DPP non superiore al 35%, l'esclusione di **3a** dall'innesto, la sottostima dei pesi molecolari da GPC e le discrepanze di **3.3c**, da indagare con ulteriori analisi. La prospettiva indicata dalla tesi è l'impiego di questi materiali in dispositivi optoelettronici, in particolare come strato elettro-luminescente in OLED. + +**Bibliografia** +- Ostroverkhova, O. Organic Optoelectronic Materials: Mechanisms and Applications. *Chem. Rev.* **2016**, *116*, 13279-13412. https://doi.org/10.1021/acs.chemrev.6b00127 +- Kroon, R.; Lenes, M.; Hummelen, J. C.; Blom, P. W. M.; de Boer, B. Small Bandgap Polymers for Organic Solar Cells (Polymer Material Development in the Last 5 Years). *Polym. Rev.* **2008**, *48*, 531-582. https://doi.org/10.1080/15583720802231833 +- Bao, W. W.; Li, R.; Dai, Z. C.; Tang, J. X.; Shi, X.; Geng, J. T.; Deng, Z. F.; Hua, J. Diketopyrrolopyrrole (DPP)-Based Materials and Its Applications: A Review. *Front. Chem.* **2020**, *8*, 679. https://doi.org/10.3389/fchem.2020.00679 +- Wang, K. Y.; Luo, Y.; Huang, S.; Yang, H.; Liu, B.; Wang, M. Highly Fluorescent Polycaprolactones Decorated with Di(thiophene-2-yl)-diketopyrrolopyrrole: A Covalent Strategy of Tuning Fluorescence Properties in Solid States. *J. Polym. Sci., Part A: Polym. Chem.* **2015**, *53*, 1032-1042. https://doi.org/10.1002/pola.27531 +- Abdel Aziz, I.; Tullii, G.; Antognazza, M. R.; Criado-Gonzalez, M. Poly(3-hexylthiophene) as a Versatile Semiconducting Polymer for Cutting-Edge Bioelectronics. *Mater. Horiz.* **2025**, *12*, 5570-5593. https://doi.org/10.1039/d5mh00096c +- Labet, M.; Thielemans, W. Synthesis of Polycaprolactone: A Review. *Chem. Soc. Rev.* **2009**, *38*, 3484. https://doi.org/10.1039/b820162p +- Iqbal, A. F. M.; Jost, M.; Kirchmayr, R.; Pfenninger, J.; Rochat, A.; Wallquist, O. The Synthesis and Properties of 1,4-Diketo-pyrrolo[3,4-C]pyrroles. *Bull. Soc. Chim. Belg.* **1988**, *97*, 615-644. https://doi.org/10.1002/bscb.19880970804 +- Grzybowski, M.; Gryko, D. T. Diketopyrrolopyrroles: Synthesis, Reactivity, and Optical Properties. *Adv. Opt. Mater.* **2015**, *3*, 280-320. https://doi.org/10.1002/adom.201400559 +- Kasha, M.; Rawls, H. R.; El-Bayoumi, M. A. The Exciton Model in Molecular Spectroscopy. *Pure Appl. Chem.* **1965**, *11*, 371-392. https://doi.org/10.1351/pac196511030371 +- Spano, F. C.; Silva, C. H- and J-Aggregate Behavior in Polymeric Semiconductors. *Annu. Rev. Phys. Chem.* **2014**, *65*, 477-500. https://doi.org/10.1146/annurev-physchem-040513-103639 diff --git a/presentazione/slides.md b/presentazione/slides.md new file mode 100644 index 0000000..d185ae1 --- /dev/null +++ b/presentazione/slides.md @@ -0,0 +1,189 @@ +--- +marp: true +theme: default +paginate: true +size: 16:9 +style: | + section { font-size: 26px; } + h1 { color: #8b1a1a; } + h2 { color: #8b1a1a; } + img { display: block; margin: 0 auto; } + .cols { display: grid; grid-template-columns: 1fr 1fr; gap: 1em; align-items: center; } + small { font-size: 0.6em; } +--- + + + +# Sintesi e caratterizzazione di copolimeri *bottle brush* foto-elettro attivi + +Aurora Luzi +Relatore: Dr. Stefano Scurti + +Tesi magistrale in Chimica Industriale — Università di Bologna, Dip. "Toso Montanari" — a.a. 2025-2026 + + + +--- + +## Contesto: perché polimeri π-coniugati emissivi + +- Optoelettronica organica (OLED, fotovoltaico): materiali leggeri, flessibili, depositabili da soluzione a bassa T +- Band gap ingegnerizzato con l'approccio **donatore-accettore (D-A)**: HOMO sul donatore, LUMO sull'accettore, trasferimento di carica intramolecolare +- **Problema: ACQ** (Aggregation-Caused Quenching) — il π-stacking delle catene planari dissipa l'energia in modo non radiativo → niente emissione nel film, proprio dove serve (strato emissivo OLED) + + + +--- + +## Scopo e strategia + +**Research question:** un'architettura *bottle brush* può superare l'ACQ allo stato solido, mantenendo l'integrità elettrochimica del core DPP? + +- Scheletro semiconduttore **DPP-3HT** (polimerizzazione ossidativa, FeCl3) +- Catene laterali di **PCL** per ROP dell'ε-caprolattone (*grafting-from*) dagli OH pendenti +- Il PCL agisce da **spaziatore sterico**: separa i segmenti planari coniugati + + + +--- + +## Il building block: il DPP + +

        + + + +--- + +## Sintesi del monomero DPP **1** → **2** + +![h:230](immagini/fig2-sintesi-dpp1.jpg) +![h:230](immagini/fig3-alchilazione-dpp2.jpg) + +- **1**: ciclizzazione pseudo-Stobbe (2-cianotiofene + diisopropil succinato, teramilato di sodio); λabs 531 nm, λem 542 nm (THF) +- **2**: N-alchilazione con 6-bromo-1-esanolo; NMR 4,1 e 3,6 ppm, IR O–H ~3400 cm-1; λabs 541 nm + + + +--- + +## Copolimeri lineari DPP-3HT (**3a**, **3b**, **3c**) + +![h:190](immagini/fig4-copolimerizzazione.jpg) + +| | % DPP teorica | % DPP reale | Mn (Da) | PD | +|---|---|---|---|---| +| **3a** | 20 | 25,2 | 2149 | 2,571 | +| **3b** | 50 | 32,6 | 1402 | 4,592 | +| **3c** | 80 | 35,3 | 2134 | 1,979 | + +- FeCl3 / nitrometano / CHCl3; DPP incorporato ≤ 35% (reattività e ingombro) +- DSC: Tg ~ −10 °C, nessuna fusione → struttura random +- Allo stato solido: **nessuna emissione apprezzabile** → ACQ + + + +--- + +## Bottle brush: innesto del PCL per ROP + +![h:250](immagini/fig5-rop-bottle-brush.jpg) + +- ROP di ε-caprolattone, Sn(Oct)2, toluene 110 °C, da **3b** e **3c** +- Catene nominali 1500 / 5000 / 10000 Da → 6 campioni (**3.1b–3.3b**, **3.1c–3.3c**) +- Conferma: NMR (~4,0 e 2,3 ppm), IR (scompare O–H, compare C=O estereo ~1720 cm-1) + + + +--- + +## Pesi molecolari e proprietà termiche + +| Polimero | Mn PCL teor. | Mn GPC | PD | Peso mol. teorico | Peso mol. da NMR | +|---|---|---|---|---|---| +| **3.1b** | 1500 | 12188 | 1,521 | 6500 | 8900 | +| **3.2b** | 5000 | 17302 | 1,314 | 18000 | 20500 | +| **3.3b** | 10000 | 21269 | 1,238 | 34500 | 88000 | +| **3.2c** | 5000 | 19119 | 1,275 | 28500 | 35500 | + +Selezione di 4 campioni su 6; tabella completa nel riassunto (Tab. 2). + +- GPC **sottostima** (standard PS lineari; volume idrodinamico compatto) → conferma indiretta della struttura ramificata +- Stima da 1H-NMR più vicina ai teorici; **3.3c** anomalo (da indagare) +- DSC: dominata dal PCL, Tf 55–60 °C, Tc 25–35 °C + + + +--- + +## Risultato 1 — emissione allo stato solido (**3.2b**) + +![h:330](immagini/fig6-uv-em-3.2b.jpg) + +- Soluzione (THF): abs ~550 nm, em ~560–565 nm, banda stretta +- Solido: abs 570–580 nm; **em ~650–660 nm**, allargata, Stokes shift ~80–90 nm → aggregati H/J (Kasha) +- Il bottle brush **mantiene emissione nel rosso**, a differenza dei lineari + + + +--- + +## Risultato 2 — proprietà elettrochimiche (CV) + +
        +
        + +![w:440](immagini/fig7-bandgap-vs-dpp.jpg) + +
        +
        + +- Trasferimento di carica irreversibile (EC); HOMO/LUMO calibrati sul ferrocene +- Lineari: band gap **0,970 → 1,371 eV** al crescere del % DPP reale (R² = 0,9719) +- Bottle brush: 0,929–1,521 eV; core DPP-3HT resta elettroattivo, PCL = matrice dielettrica + +
        +
        + + + +--- + +## Conclusioni e limiti + +**Conclusioni** +- Approccio ortogonale DPP-3HT + PCL → 3 copolimeri e 6 bottle brush +- PCL come spaziatore sterico: **emissione rossa allo stato solido** (3.2b) +- Band gap modulabile con la composizione; integrità elettrochimica preservata + +**Limiti dichiarati** +- DPP ≤ 35%; **3a** non innestato; GPC sottostimata; **3.3c** anomalo + +**Prospettive:** strato elettroluminescente in OLED + + + +--- + +## Grazie per l'attenzione + +Domande? + +Riferimenti principali: Ostroverkhova, *Chem. Rev.* 2016 · Bao et al., *Front. Chem.* 2020 · Wang et al., *J. Polym. Sci. A* 2015 · Labet & Thielemans, *Chem. Soc. Rev.* 2009 · Spano & Silva, *Annu. Rev. Phys. Chem.* 2014 + + diff --git a/wiki/analyses/riassunto-tesi.md b/wiki/analyses/riassunto-tesi.md new file mode 100644 index 0000000..4f86ea3 --- /dev/null +++ b/wiki/analyses/riassunto-tesi.md @@ -0,0 +1,141 @@ +--- +title: Riassunto della tesi (formato 10 pagine) +type: analysis +tags: [riassunto, query, tesi] +created: 2026-10-09 +updated: 2026-10-09 +tesi_loc: "Riassunto r.13-23; Abstract r.25-33; §1 r.66-542; §2 r.545-559; §3 r.562-715; §4 r.717-1277; §5 r.1279-1291" +refs: [45, 48, 1, 42, 52, 56, 5, 7, 58, 59] +figures: ["fig-001", "fig-x-185efd", "fig-x-f6eeb1", "fig-x-cc3f54", "fig-x-136800", "fig-071", "fig-074"] +status: draft +--- + + + +_[PAGINA 1 - COPERTINA: da inserire a parte]_ + +--- + +Il lavoro è stato svolto presso il Dipartimento di Chimica Industriale "Toso Montanari" dell'Università di Bologna, in un gruppo specializzato in materiali polimerici ingegnerizzati, con attenzione alla soft optoelectronics, il ramo interdisciplinare che combina emissione e rilevamento della luce con dispositivi flessibili e adattabili. L'obiettivo generale è sviluppare semiconduttori polimerici emissivi π-coniugati che superino le limitazioni imposte dall'Aggregation-Caused Quenching (ACQ). Il lavoro si è articolato in quattro fasi: sintesi di un monomero a base di dichetopirrolopirrolo (DPP), copolimerizzazione ossidativa con 3-esiltiofene (3HT) per ottenere lo scheletro coniugato, innesto di catene laterali di poli(ε-caprolattone) (PCL) e caratterizzazione dei materiali. La scelta del 3HT deriva dalla collaborazione con il gruppo del Prof. Lanzi, la cui esperienza pregressa ha convalidato la polimerizzazione ossidativa su questa classe di derivati tiofenici. + +L'optoelettronica organica studia dispositivi basati sull'interazione tra radiazione elettromagnetica e semiconduttori: conversione di segnali elettrici in fotoni, come nei diodi organici a emissione di luce (OLED), o viceversa, come nelle celle fotovoltaiche. Rispetto ai semiconduttori inorganici rigidi, come il silicio, i materiali organici con estesi sistemi π-coniugati sono leggeri e meccanicamente flessibili e si depositano da soluzione a basse temperature, con tecniche come lo spin-coating e la stampa su larga scala, con riduzione dei costi e dell'impatto ambientale.1 Per impiegarli in un dispositivo occorre governarne le proprietà ottiche ed elettroniche, cioè ingegnerizzare il band gap. La strategia d'elezione è l'approccio donatore-accettore (D-A), che alterna unità fortemente elettron-deficienti e unità elettron-ricche lungo lo scheletro π-coniugato: l'orbitale HOMO è determinato principalmente dalla porzione donatrice e il LUMO dall'unità accettrice, e il trasferimento di carica intramolecolare che ne deriva riduce il salto energetico e permette di centrare assorbimento ed emissione nel visibile.2 + +I materiali semiconduttori π-coniugati perdono spesso le proprietà ottiche allo stato solido. La natura altamente planare del loro scheletro induce intense interazioni di π-stacking tra le catene adiacenti, che causano la drastica dissipazione non radiativa dell'energia eccitonica e lo smorzamento della fluorescenza: è l'ACQ. Questo limita le applicazioni pratiche dei materiali, perché nello strato emissivo di un OLED è richiesta proprio l'emissione. Per ovviare al problema, la tesi propone una strategia di design macromolecolare basata su architetture a spazzola (bottle brush), il cui scopo è promuovere la separazione fisica dei segmenti planari coniugati, ripristinando le proprietà emissive allo stato solido e preservando integrità elettrochimica e stabilità del sistema. + +Come unità accettrice è stato scelto il DPP, formato da due anelli lattamici a cinque termini condensati, con sostituenti aromatici o eteroaromatici in posizione 3 e 6 *(Figura 1)*. Nato come pigmento rosso industriale, il DPP ha punto di fusione superiore a 350 °C e solubilità molto bassa, dovute a un fitto network di legami a idrogeno ammidici e di π-stacking tra i piani molecolari.3 Il nucleo è planare e fortemente elettron-deficiente, e la rigidità dello scheletro limita il rilassamento vibrazionale e lo Stokes shift. Nel passaggio dalla soluzione al film il DPP mostra un allargamento della banda di assorbimento e un marcato effetto batocromico, con spostamento del picco di circa 30 nm. + +![[immagini/455dd3d0c7bf0fe6ac581ee70795075c998d4dc7156eaa77a4576774f6fd8050.jpg|300]] + +Figura 1. Struttura generica di un dichetopirrolopirrolo. + +L'inserimento di un fluoroforo in un sistema polimerico richiede un accurato design molecolare, perché l'architettura scelta influenza drasticamente le proprietà finali. Nei sistemi host-guest il fluoroforo è disperso fisicamente nella matrice: la preparazione è semplice, ma la scarsa stabilità a lungo termine, con migrazione e aggregazione dell'ospite, porta a perdita di resa quantica. Nei sistemi main-chain il fluoroforo è parte integrante della catena principale, con sintesi più complessa; una strategia riuscita è il grafting-from, in cui un DPP bifunzionalizzato con gruppi ossidrilici inizia la crescita di due catene di PCL, dando PCL-DPP-PCL.4 Nei sistemi side-chain le unità luminescenti sono catene laterali, spesso con uno spaziatore flessibile che limita le interazioni tra cromofori; nei sistemi cross-linked il cromoforo è ancorato da ponti chimici e non aggrega, ma l'eccessiva rigidità rende il materiale fragile, insolubile e difficile da lavorare. La tesi adotta il grafting-from per innestare catene laterali di PCL su uno scheletro semiconduttore DPP-3HT. + +Il monomero è un derivato del DPP definito ortogonale e tetrafunzionale: gli anelli tiofenici forniscono i siti per la polimerizzazione ossidativa dello scheletro, mentre i due gruppi ossidrilici primari, portati dalle catene esiliche sugli azoti lattamici, fungono da iniziatori per la polimerizzazione ad apertura di anello (ROP). Il gruppo aveva già studiato fluorofori DPP con sostituenti diversi in para sull'anello benzonitrilico: quelli elettron-attrattori davano sistemi altamente emissivi, quelli elettron-donatori un isomero strutturale (iso-DPP) a fluorescenza inibita. In questo lavoro i benzeni sono sostituiti da tiofeni e i gruppi ammidici sono N-alchilati, con aumento della solubilità e una procedura semplice e scalabile. Il 3HT è il comonomero donatore: i politiofeni sono tra i più efficienti polimeri semiconduttori organici5 e la catena esilica aumenta la solubilità nei solventi organici. La polimerizzazione ossidativa con FeCl3 è stata preferita ai cross-coupling al palladio perché non richiede pre-funzionalizzazione dei monomeri, opera a temperatura e pressione ambiente ed è scalabile, a fronte di un controllo minore su polidispersità e regioregolarità. La distribuzione statistica dei monomeri aumenta l'entropia conformazionale, limita il packing e rende più accessibili gli ossidrili per la funzionalizzazione. + +Il PCL è stato scelto sulla base di studi precedenti del gruppo, per la bassa temperatura di transizione vetrosa e la buona solubilità nei solventi organici; la ROP dell'ε-caprolattone catalizzata da stagno ottanoato (Sn(Oct)2) è un processo lineare ed efficiente, procede per coordinazione-inserzione con un alcol come coiniziatore e permette di regolare il peso molecolare e di mantenere bassa la dispersità delle catene.6 La lunghezza delle catene si modula con il rapporto molare monomero/ossidrili, con valori nominali di 1500, 5000 e 10000 Da. I copolimeri sono stati alimentati con il 20%, 50% e 80% in moli di DPP; i bottle brush sono stati preparati da **3b** e **3c**, mentre **3a** non è stato usato a causa della scarsa efficienza della sua via sintetica, con basse rese e difficoltà di work-up, e di volumi di solventi e costi di reagenti troppo elevati per isolarne quantità utili. + +Lo scopo del progetto è sintetizzare e caratterizzare copolimeri bottle brush foto-elettro attivi a base di DPP e 3HT con catene laterali di PCL, al fine di superare l'ACQ allo stato solido mantenendo l'integrità elettrochimica del nucleo DPP. Il lavoro comprende due macroaree: la sintesi del monomero ortogonale e l'ottenimento dei materiali, cioè scheletro coniugato e catene innestate. + +Il DPP tiofenico **1** *(Figura 2)* è stato ottenuto per ciclizzazione pseudo-Stobbe tra 2-cianotiofene e diisopropil succinato.7 La base forte è il teramilato di sodio, ottenuto dal sodio in alcol ter-amilico con FeCl3 catalitico: deprotona il succinato in α al carbonile, il carbanione attacca il carbonio nitrilico e il composto imminico tautomerizza a enammina, che attacca il carbonile estereo chiudendo il primo anello a cinque termini; una seconda deprotonazione e l'attacco di una seconda molecola di tiofene portano al secondo anello. Il succinato è stato aggiunto lentamente, perché una concentrazione locale troppo alta in condizioni basiche induce autocondensazione di Claisen, e si è scelto il diisopropil succinato per aumentare l'ingombro intorno al carbonile e ridurre questa reazione.8 Il prodotto, un solido rosso scuro violaceo, è stato purificato sfruttando la netta differenza di solubilità tra reagenti e prodotto, con lavaggi in acqua e metanolo. Il 1H-NMR in DMSO mostra a circa 11 ppm il singoletto allargato dei protoni ammidici; in THF **1** ha massimo di assorbimento a 531 nm, di emissione a 542 nm e Stokes shift di 11 nm. + +![[immagini/185efd9de96189fb7fefd271e19709d672e7eda09572a645d13092c3196248e1.jpg|400]] + +Figura 2. Sintesi del DPP **1** da 2-cianotiofene e diisopropil succinato con teramilato di sodio e FeCl3 catalitico. + +L'N-alchilazione di **1** con 6-bromo-1-esanolo *(Figura 3)* sfrutta la reattività dei gruppi ammidici, deprotonati da ter-butossido di potassio in DMSO, che attaccano per sostituzione nucleofila il carbonio adiacente al bromo, e dà il monomero **2** con due braccia idrossiesiliche. La tesi segnala come reazione collaterale la ciclizzazione del 6-bromo-1-esanolo, favorita da un eccesso di base. Il prodotto è stato lavato con soluzione satura di KCl e purificato per cristallizzazione da etanolo a −20 °C. L'N-alchilazione è confermata nel 1H-NMR dai multipletti alifatici a 4,1 ppm (metileni legati all'azoto lattamico) e a 3,6 ppm (metileni adiacenti all'ossidrile terminale), e nel FT-IR dalla banda larga dell'O-H a circa 3400 cm-1 insieme al C=O lattamico a circa 1650 cm-1. Il massimo di assorbimento passa da 531 nm (**1**) a 541 nm (**2**): lo spostamento batocromico è attribuito all'effetto induttivo elettron-donatore delle catene alifatiche, che arricchiscono di densità elettronica gli azoti, destabilizzano l'HOMO e restringono il band gap ottico. + +![[immagini/f6eeb10de88591bd0358f146073c675489133b4c8bb70f71131b343bb8a25794.jpg|400]] + +Figura 3. N-alchilazione del DPP **1** con 6-bromo-1-esanolo (DMSO, ter-butossido di potassio, 40 °C) a dare il monomero **2** con due catene idrossiesiliche. + +Il monomero **2** è stato copolimerizzato con 3HT per via ossidativa, con FeCl3 in nitrometano e cloroformio anidro *(Figura 4)*. Il FeCl3, in eccesso stechiometrico, estrae per trasferimento mono-elettronico un elettrone dagli anelli tiofenici, generando cationi radicalici delocalizzati che formano i nuovi legami C-C. Il nitrometano rompe i dimeri di FeCl3 e ne modera acidità di Lewis e potere ossidante, prevenendo sovraossidazione e difetti di reticolazione; il cloroformio anidro evita che l'acqua si coordini al FeCl3 e spenga per attacco nucleofilo gli intermedi cationico-radicalici. L'ossidante è stato rimosso con lavaggi con HCl 0,6 M fino a saggio negativo del tiocianato, perché tracce di metalli di transizione abbatterebbero la mobilità dei portatori e spegnerebbero la fluorescenza, e l'omopolimero del 3HT è stato eliminato per precipitazione in metanolo freddo. L'integrazione di DPP si è limitata a un massimo del 35% *(Tabella 1)*: la tesi lo attribuisce alla differenza nei rapporti di reattività dei comonomeri, influenzata dall'ingombro sterico del DPP, mentre il tiofene, più reattivo e meno voluminoso, addiziona preferenzialmente. Le percentuali reali sono state determinate via 1H-NMR. + +![[immagini/cc3f5409e11922aee7835c8eb96ff0f9826afea68af08f1473159279af625b8a.jpg|400]] + +Figura 4. Copolimerizzazione ossidativa del DPP **2** con 3-esiltiofene con FeCl3 a dare i copolimeri **3a**, **3b** e **3c**. + +Tabella 1. Composizione dei copolimeri e pesi molecolari da GPC. + +| Copolimero | % DPP teorica (mol/mol) | % DPP reale (mol/mol) | Mn (Da) | Mw (Da) | PD | +| --- | --- | --- | --- | --- | --- | +| **3a** | 20 | 25,2 | 2149 | 5526 | 2,571 | +| **3b** | 50 | 32,6 | 1402 | 6439 | 4,592 | +| **3c** | 80 | 35,3 | 2134 | 4223 | 1,979 | + +I copolimeri hanno Mn tra 1402 e 2149 Da. Valori di PD intorno a 2 o superiori sono attesi per una polimerizzazione non controllata, con distribuzione più probabile di Flory; **3c** ha la distribuzione più omogenea (PD 1,979), mentre **3b**, con Mn più bassa ma Mw più alta, indica una frazione significativa di oligomeri a catena corta accanto a macromolecole di peso molecolare più elevato. Il FT-IR conferma l'incorporazione del DPP con il C=O lattamico a circa 1650 cm-1, e la DSC mostra per tutti i campioni una transizione vetrosa intorno a −10 °C e nessuna transizione di fusione, a conferma della natura random dei copolimeri, il cui disordine impedisce la cristallizzazione. In soluzione di THF i tre copolimeri hanno profili ottici pressoché identici, simili a quello del monomero: assorbimento tra 540 e 544 nm, emissione intorno a 550 nm e Stokes shift tra 6 e 10 nm. Allo stato solido il comportamento è drasticamente diverso: l'intenso impaccamento delle catene forma aggregati che disattivano i fluorofori per decadimento non radiativo, e i film su vetrino sotto lampada UV non mostrano emissione apprezzabile. È la principale criticità dei sistemi lineari per l'uso in dispositivi optoelettronici e giustifica il passaggio al design bottle brush. + +I sei bottle brush **3.1b**, **3.2b**, **3.3b**, **3.1c**, **3.2c** e **3.3c** sono stati ottenuti per ROP dell'ε-caprolattone dagli ossidrili di **3b** e **3c**, in toluene a 110 °C con Sn(Oct)2 catalitico, con il monomero dosato sul numero di ossidrili per ottenere catene di 1500, 5000 e 10000 Da *(Figura 5)*. L'avvenuto innesto è verificato dal 1H-NMR, con il tripletto del PCL a circa 4,0 ppm (CH2-O adiacente all'ossigeno estereo) e il segnale a 2,3 ppm dei protoni in α al carbonile, e dal FT-IR, in cui la banda dell'O-H a 3600-3200 cm-1 dei macroiniziatori scompare e compare il C=O estereo a circa 1720 cm-1. La GPC fornisce Mn tra 12188 e 21269 Da e indici di dispersità contenuti (1,238-1,521). + +![[immagini/136800375cf0b441570672093e255d90a47c45a009bd254929fb74b1f17b382d.jpg|400]] + +Figura 5. Polimerizzazione ad apertura di anello dell'ε-caprolattone sui gruppi OH dei copolimeri DPP-3HT, a dare i bottle brush con catene di PCL. + +I pesi molecolari da GPC *(Tabella 2)* sono significativamente sottostimati rispetto ai teorici: la GPC separa per volume idrodinamico e restituisce valori relativi agli standard di polistirene lineare, mentre un polimero altamente ramificato assume in soluzione una conformazione compatta, con volume idrodinamico nettamente inferiore. I dati non indicano quindi il peso molecolare assoluto né una bassa resa, ma confermano indirettamente una struttura ramificata altamente impaccata e permettono il confronto tra i polimeri. Il campione **3.3c** si discosta dall'andamento generale; la tesi ipotizza che, essendo il materiale di partenza random, elevate concentrazioni locali di DPP e di ossidrili abbiano ridotto la crescita delle catene laterali per ingombro sterico, e indica che le discrepanze saranno investigate in futuro con ulteriori analisi. Per superare i limiti della GPC è stato calcolato il peso molecolare via 1H-NMR dal grado di polimerizzazione delle catene di PCL, ottenendo una stima descritta come più vicina ai valori teorici. Dal punto di vista termico, la DSC mostra per tutti i bottle brush transizioni dominate dal PCL, con fusione tra 55 e 60 °C e cristallizzazione tra 25 e 35 °C. + +Tabella 2. Pesi molecolari dei bottle brush da GPC e da 1H-NMR, con il valore teorico. + +| Polimero | Mn PCL teorico (Da) | Mn GPC (Da) | PD | Peso molecolare teorico (Da) | Peso molecolare da 1H-NMR (Da) | +| --- | --- | --- | --- | --- | --- | +| **3.1b** | 1500 | 12188 | 1,521 | 6500 | 8900 | +| **3.2b** | 5000 | 17302 | 1,314 | 18000 | 20500 | +| **3.3b** | 10000 | 21269 | 1,238 | 34500 | 88000 | +| **3.1c** | 1500 | 13999 | 1,301 | 10000 | 18200 | +| **3.2c** | 5000 | 19119 | 1,275 | 28500 | 35500 | +| **3.3c** | 10000 | 14445 | 1,351 | 55000 | 41300 | + +La caratterizzazione ottica in soluzione di THF mostra che la funzionalizzazione sterica non perturba l'integrità elettronica del core DPP: i massimi di assorbimento cadono tra 544 e 554 nm, quelli di emissione tra 557 e 564 nm e gli Stokes shift tra 8 e 14 nm. Le piccole fluttuazioni nelle due serie non seguono un andamento lineare con il peso molecolare del PCL e sono trascurabili, quindi l'ingombro sterico non perturba livelli energetici e natura delle transizioni. Il basso Stokes shift conferma la conservazione dell'assetto planare del cromoforo e la minima riorganizzazione tra stato fondamentale ed eccitato, e i domini flessibili di PCL allontanano le catene principali, riducendo l'impaccamento senza distorcere la geometria del backbone. + +La caratterizzazione allo stato solido è stata condotta sul campione **3.2b**, confrontando soluzione e solido *(Figura 6)*. Le misure in soluzione diluita indagano la singola catena isolata e solvatata; allo stato solido la vicinanza tra le macromolecole genera forti interazioni intermolecolari che alterano i livelli energetici e i processi di assorbimento ed emissione. In soluzione il massimo di assorbimento è a circa 550 nm e quello di emissione a circa 560-565 nm, con banda stretta e strutturata. Allo stato solido l'assorbimento mostra un significativo allargamento e un marcato effetto batocromico, con il massimo nell'intervallo 570-580 nm, attribuito alla planarizzazione dello scheletro, che estende la lunghezza di coniugazione effettiva. L'emissione è notevolmente allargata e fortemente spostata verso il rosso, con massimo centrato intorno a 650-660 nm e Stokes shift di circa 80-90 nm, probabilmente legato al maggiore ingombro delle catene, che obbliga gli anelli aromatici a torsioni maggiori, ed evidenza di una forte aggregazione intermolecolare. Secondo la tesi, dopo la fotoeccitazione l'energia migra verso siti a minore energia generati dalla vicinanza dei piani coniugati e il rilassamento radiativo avviene prevalentemente da stati aggregati o specie eccimeriche, nel quadro dell'accoppiamento eccitonico di Kasha tra aggregati H e J.9,10 Nonostante questi riarrangiamenti, l'architettura bottle brush mantiene un'apprezzabile emissione nel rosso, attenuando i percorsi di disattivazione non radiativa tipici dell'ACQ non controllato, in accordo con il ruolo del PCL come spaziatore sterico. + +![[immagini/04f625a8b25744bf2d07d569e55558174b59a5cb564c8bdd0a53c704dfbde545.jpg|420]] + +Figura 6. Confronto tra spettri UV-Vis (in nero) ed emissione (in rosso) del polimero **3.2b** in soluzione (linea continua) e allo stato solido (linea tratteggiata). + +La ciclovoltammetria mostra per i polimeri un trasferimento di carica irreversibile di tipo elettrochimico-chimico, dovuto all'elevata reattività dei cationi e degli anioni radicali all'interfaccia elettrodica. Dagli onset di ossidazione e riduzione, calibrati sul ferrocene (posto a −4,8 eV rispetto al livello del vuoto), sono stati ricavati HOMO, LUMO e band gap elettrochimico *(Tabella 3)*. Nei copolimeri lineari si osserva un allargamento progressivo del band gap all'aumentare della frazione reale di DPP, da 0,970 a 1,371 eV *(Figura 7)*, con correlazione lineare (R² = 0,9719) guidata soprattutto dallo spostamento del potenziale di riduzione verso valori più negativi. La tesi lo interpreta come riduzione della lunghezza di coniugazione effettiva dovuta all'unità DPP, che limita la delocalizzazione π e aumenta la separazione HOMO-LUMO, e vi riconosce la possibilità di un controllo mirato del band gap calibrando il rapporto tra i monomeri. Rispetto al poli-3HT, che si ossida a potenziali accessibili ma non mostra contributi faradici in riduzione, nei copolimeri il DPP, forte porzione elettron-attrattrice in un'architettura D-A, stabilizza il LUMO e rende favorevole l'iniezione di elettroni. + +![[immagini/6c7bd8393eb8c1a329f65b7fc74e5f338a866e514455c0122a43d13ca340ded5.jpg|380]] + +Figura 7. Correlazione tra band gap elettrochimico e frazione reale di DPP nei copolimeri lineari. + +Tabella 3. Livelli HOMO, LUMO e band gap elettrochimici dei copolimeri lineari e dei bottle brush. + +| Polimero | HOMO (eV) | LUMO (eV) | Bandgap (eV) | +| --- | --- | --- | --- | +| **3a** | -5,038 | -4,068 | 0,970 | +| **3b** | -4,854 | -3,538 | 1,316 | +| **3c** | -4,799 | -3,428 | 1,371 | +| **3.1b** | -4,617 | -3,580 | 1,037 | +| **3.2b** | -4,625 | -3,527 | 1,098 | +| **3.3b** | -4,630 | -3,598 | 1,032 | +| **3.1c** | -4,774 | -3,253 | 1,521 | +| **3.2c** | -4,688 | -3,269 | 1,419 | +| **3.3c** | -4,479 | -3,550 | 0,929 | + +I bottle brush mantengono l'elettroattività dello scheletro: i processi redox avvengono a carico del core DPP-3HT, mentre i rami alifatici fungono da matrice dielettrica circostante. Le ingombranti catene laterali modificano HOMO e LUMO rispetto ai lineari, e quindi l'ampiezza del band gap, che nei bottle brush è compresa tra 0,929 e 1,521 eV; la tesi attribuisce l'effetto all'ingombro sterico dei rami di PCL sul grado di coplanarità locale dello scheletro, e quindi sull'estensione effettiva della delocalizzazione. L'ingegnerizzazione con PCL non compromette, secondo la tesi, le spiccate potenzialità optoelettroniche del sistema. + +In conclusione, i risultati confermano secondo la tesi la validità del design proposto: l'approccio ortogonale basato su scheletri semiconduttori DPP-3HT modificati con catene laterali di PCL combina proprietà elettrochimiche modulabili e capacità emissiva allo stato solido. Dal punto di vista sintetico, monomeri ortogonali derivati dal DPP, polimerizzazione ossidativa con FeCl3 e ROP hanno portato a tre copolimeri statistici e a due serie di bottle brush con catene laterali di PCL di lunghezza nominale crescente. Il nucleo DPP conserva in soluzione le proprietà ottiche e, allo stato solido, il bottle brush **3.2b** mantiene un'apprezzabile emissione nel rosso; la composizione monomerica si rivela un parametro di controllo del band gap. I limiti dichiarati nel testo sono l'integrazione di DPP non superiore al 35%, l'esclusione di **3a** dall'innesto, la sottostima dei pesi molecolari da GPC e le discrepanze di **3.3c**, da indagare con ulteriori analisi. La prospettiva indicata dalla tesi è l'impiego di questi materiali in dispositivi optoelettronici, in particolare come strato elettro-luminescente in OLED. + +--- + +Bibliografia + +1. Ostroverkhova, O. Organic Optoelectronic Materials: Mechanisms and Applications. *Chem. Rev.* **2016**, *116*, 13279-13412. https://doi.org/10.1021/acs.chemrev.6b00127 +2. Kroon, R.; Lenes, M.; Hummelen, J. C.; Blom, P. W. M.; de Boer, B. Small Bandgap Polymers for Organic Solar Cells (Polymer Material Development in the Last 5 Years). *Polym. Rev.* **2008**, *48*, 531-582. https://doi.org/10.1080/15583720802231833 +3. Bao, W. W.; Li, R.; Dai, Z. C.; Tang, J. X.; Shi, X.; Geng, J. T.; Deng, Z. F.; Hua, J. Diketopyrrolopyrrole (DPP)-Based Materials and Its Applications: A Review. *Front. Chem.* **2020**, *8*, 679. https://doi.org/10.3389/fchem.2020.00679 +4. Wang, K. Y.; Luo, Y.; Huang, S.; Yang, H.; Liu, B.; Wang, M. Highly Fluorescent Polycaprolactones Decorated with Di(thiophene-2-yl)-diketopyrrolopyrrole: A Covalent Strategy of Tuning Fluorescence Properties in Solid States. *J. Polym. Sci., Part A: Polym. Chem.* **2015**, *53*, 1032-1042. https://doi.org/10.1002/pola.27531 +5. Abdel Aziz, I.; Tullii, G.; Antognazza, M. R.; Criado-Gonzalez, M. Poly(3-hexylthiophene) as a Versatile Semiconducting Polymer for Cutting-Edge Bioelectronics. *Mater. Horiz.* **2025**, *12*, 5570-5593. https://doi.org/10.1039/d5mh00096c +6. Labet, M.; Thielemans, W. Synthesis of Polycaprolactone: A Review. *Chem. Soc. Rev.* **2009**, *38*, 3484. https://doi.org/10.1039/b820162p +7. Iqbal, A. F. M.; Jost, M.; Kirchmayr, R.; Pfenninger, J.; Rochat, A.; Wallquist, O. The Synthesis and Properties of 1,4-Diketo-pyrrolo[3,4-C]pyrroles. *Bull. Soc. Chim. Belg.* **1988**, *97*, 615-644. https://doi.org/10.1002/bscb.19880970804 +8. Grzybowski, M.; Gryko, D. T. Diketopyrrolopyrroles: Synthesis, Reactivity, and Optical Properties. *Adv. Opt. Mater.* **2015**, *3*, 280-320. https://doi.org/10.1002/adom.201400559 +9. Kasha, M.; Rawls, H. R.; El-Bayoumi, M. A. The Exciton Model in Molecular Spectroscopy. *Pure Appl. Chem.* **1965**, *11*, 371-392. https://doi.org/10.1351/pac196511030371 +10. Spano, F. C.; Silva, C. H- and J-Aggregate Behavior in Polymeric Semiconductors. *Annu. Rev. Phys. Chem.* **2014**, *65*, 477-500. https://doi.org/10.1146/annurev-physchem-040513-103639 + +--- + +## Collegamenti +_(sezione solo wiki, non parte del riassunto)_ +- [[overview]] · [[tesi]] · [[bottle-brush]] · [[acq-e-stato-solido]] · [[fluorofori-in-polimeri]] · [[dpp-struttura-e-proprieta]] +- [[dpp-1]] · [[dpp-2]] · [[copolimeri-3a-3b-3c]] · [[bottle-brush-3-x]] · [[cv-risultati]] · [[difetti-noti]] +- Figure usate: 1 = [[fig-001]]; 2-5 = [[fig-x-185efd|schema DPP 1]], [[fig-x-f6eeb1|schema DPP 2]], [[fig-x-cc3f54|schema copolimeri]], [[fig-x-136800|schema bottle brush]]; 6 = [[fig-074]]; 7 = [[fig-071]] +- Allineamento alla tesi (terza stesura): contenuti e interpretazioni sono quelli della tesi; rimosse le inferenze della seconda stesura (stima delle unità ripetitive, confronto gap elettrochimico/ottico, commenti sul numero di campioni, giudizi sulle misure di massa molare). Dove la tesi è incoerente con sé stessa si è scelto il capitolo dei risultati: non sono riportati «da 3,42 eV a oltre 4,30 eV» e «fusione oltre 110 °C» delle Conclusioni ([[difetti-noti]], punti 5-6); la stima NMR è citata come la descrive la tesi, i dati sono in Tabella 2 ([[difetti-noti]], punto 7); l'assorbimento solido di 3.2b è dato come nel testo (570-580 nm), mentre il grafico mostra massimi a circa 550 e 580 nm ([[fig-074]]). La durata del reflusso ROP non è riportata (4 h nello schema, 24 h nel testo). +- Le citazioni 1-10 provengono dalle schede in `raw/fonti/` (non riverificate su fonte originale), numerate per ordine di apparizione.

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