From 3855b21d6d94c4e16ccd0826e1ea10dd1805fc7c Mon Sep 17 00:00:00 2001 From: Davide Grilli Date: Tue, 13 Oct 2026 15:05:14 +0200 Subject: [PATCH] Aggiorna tesi.md, catalogo figure, bibliografia e wiki alla nuova versione (tesi_new.docx) - raw/tesi.md allineato al docx; aggiunta Figura 52 e nuovo riferimento 51 - raw/immagini.json, raw/bibliografia.json e raw/fonti rinumerati; wiki/figures e wiki/bibliografia rigenerate - pagine wiki, difetti-noti, CLAUDE.md e log aggiornati Co-Authored-By: Claude Sonnet 5.5 --- CLAUDE.md | 18 +- index.md | 12 +- log.md | 22 + raw/bibliografia.json | 230 ++-- raw/fonti/05-iqbal-1988.md | 2 +- raw/fonti/07-grzybowski-2015.md | 4 +- raw/fonti/50-cardona-2011.md | 2 +- raw/fonti/51-scurti-2026.md | 47 + .../{51-wang-2022.md => 52-wang-2022.md} | 12 +- ...del-aziz-2025.md => 53-abdel-aziz-2025.md} | 12 +- .../{53-paganin-nd.md => 54-paganin-nd.md} | 10 +- .../{54-odian-2004.md => 55-odian-2004.md} | 10 +- ...5-woodruff-2010.md => 56-woodruff-2010.md} | 12 +- .../{56-labet-2009.md => 57-labet-2009.md} | 12 +- .../{57-floyd-2021.md => 58-floyd-2021.md} | 10 +- .../{58-kasha-1965.md => 59-kasha-1965.md} | 12 +- .../{59-spano-2014.md => 60-spano-2014.md} | 12 +- raw/immagini.json | 1031 +++++++++-------- ...ad43408c4b39ab24ba521cc098fbda40f50699.jpg | Bin 0 -> 21775 bytes raw/tesi.md | 323 +++--- raw/tesi_new.docx | Bin 0 -> 7142387 bytes scripts/gen_bibliografia.py | 4 +- wiki/analyses/difetti-noti.md | 47 +- wiki/analyses/riassunto-tesi.md | 50 +- wiki/bibliografia.md | 33 +- wiki/compounds/bottle-brush-3-x.md | 99 +- wiki/compounds/copolimeri-3a-3b-3c.md | 81 +- wiki/compounds/dpp-1.md | 20 +- wiki/compounds/dpp-2.md | 44 +- wiki/concepts/acq-e-stato-solido.md | 34 +- wiki/concepts/bottle-brush.md | 14 +- wiki/concepts/dpp-sintesi-letteratura.md | 4 +- wiki/concepts/dpp-struttura-e-proprieta.md | 6 +- wiki/concepts/fluorescenza.md | 2 +- ...optoelettronica-oled-donatore-accettore.md | 10 +- .../polimerizzazione-ossidativa-fecl3.md | 26 +- wiki/concepts/rop-pcl.md | 24 +- wiki/dati.md | 21 +- wiki/figures/fig-009.md | 4 +- wiki/figures/fig-033.md | 4 +- wiki/figures/fig-035.md | 4 +- wiki/figures/fig-039.md | 4 +- wiki/figures/fig-040.md | 6 +- wiki/figures/fig-041.md | 6 +- wiki/figures/fig-042.md | 6 +- wiki/figures/fig-043.md | 6 +- wiki/figures/fig-044.md | 6 +- wiki/figures/fig-045.md | 8 +- wiki/figures/fig-046.md | 6 +- wiki/figures/fig-047.md | 6 +- wiki/figures/fig-048.md | 6 +- wiki/figures/fig-049.md | 6 +- wiki/figures/fig-050.md | 10 +- wiki/figures/fig-051.md | 10 +- wiki/figures/fig-052.md | 41 +- wiki/figures/fig-053.md | 32 +- wiki/figures/fig-054.md | 34 +- wiki/figures/fig-055.md | 28 +- wiki/figures/fig-056.md | 24 +- wiki/figures/fig-057.md | 44 +- wiki/figures/fig-058.md | 44 +- wiki/figures/fig-059.md | 24 +- wiki/figures/fig-060.md | 24 +- wiki/figures/fig-061.md | 33 +- wiki/figures/fig-062.md | 43 +- wiki/figures/fig-063.md | 42 +- wiki/figures/fig-064.md | 32 +- wiki/figures/fig-065.md | 42 +- wiki/figures/fig-066.md | 30 +- wiki/figures/fig-067.md | 44 +- wiki/figures/fig-068.md | 35 +- wiki/figures/fig-069.md | 37 +- wiki/figures/fig-070.md | 26 +- wiki/figures/fig-071.md | 32 +- wiki/figures/fig-072.md | 26 +- wiki/figures/fig-073.md | 26 +- wiki/figures/fig-074.md | 36 +- wiki/figures/fig-075.md | 42 + wiki/figures/fig-x-136800.md | 2 +- wiki/overview.md | 16 +- wiki/techniques/ciclovoltammetria.md | 28 +- wiki/techniques/cv-risultati.md | 39 +- wiki/techniques/dsc.md | 12 +- wiki/techniques/ft-ir.md | 8 +- wiki/techniques/gpc.md | 16 +- wiki/techniques/nmr-1h.md | 24 +- wiki/techniques/reagenti-e-materiali.md | 2 +- wiki/techniques/uv-vis-fluorescenza.md | 32 +- wiki/tesi.md | 34 +- 89 files changed, 1866 insertions(+), 1578 deletions(-) create mode 100644 raw/fonti/51-scurti-2026.md rename raw/fonti/{51-wang-2022.md => 52-wang-2022.md} (97%) rename raw/fonti/{52-abdel-aziz-2025.md => 53-abdel-aziz-2025.md} (97%) rename raw/fonti/{53-paganin-nd.md => 54-paganin-nd.md} (90%) rename raw/fonti/{54-odian-2004.md => 55-odian-2004.md} (97%) rename raw/fonti/{55-woodruff-2010.md => 56-woodruff-2010.md} (98%) rename raw/fonti/{56-labet-2009.md => 57-labet-2009.md} (97%) rename raw/fonti/{57-floyd-2021.md => 58-floyd-2021.md} (97%) rename raw/fonti/{58-kasha-1965.md => 59-kasha-1965.md} (97%) rename raw/fonti/{59-spano-2014.md => 60-spano-2014.md} (96%) create mode 100644 raw/immagini/c43b5f5dac544853f6c17aff18ad43408c4b39ab24ba521cc098fbda40f50699.jpg create mode 100644 raw/tesi_new.docx create mode 100644 wiki/figures/fig-075.md diff --git a/CLAUDE.md b/CLAUDE.md index 8fc1b1f..a162d9a 100644 --- a/CLAUDE.md +++ b/CLAUDE.md @@ -17,10 +17,10 @@ Tesi magistrale in Chimica Industriale (Università di Bologna, Dipartimento "To ## 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/tesi.md` | Sorgente canonico (1432 righe; aggiornato il 2026-10-13 alla nuova versione `tesi_new.docx`). Cap. 1 Introduzione (r.66), 2 Scopo (r.545), 3 Procedure sperimentali (r.562), 4 Discussione dei risultati (r.714), 5 Conclusioni (r.1298); bibliografia in fondo (r.1312) | +| `raw/immagini/` | 80 file figura (nomi = hash) | +| `raw/immagini.json` | Catalogo di 79 figure logiche: pannelli, didascalia stampata e generata, testo visibile, composti, concetti, contesto, qualità | +| `raw/bibliografia.json` | 60 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) | 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. @@ -38,7 +38,7 @@ 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/ + bibliografia.md i 60 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 @@ -77,17 +77,17 @@ status: draft | stable ## Figure - `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. +- 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, 58, 63, 66, 67, 69 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 - 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. +- Una tabella o un dato sta in **una sola pagina**: quella dove la tesi lo discute (per es. Tab. 5 in `dpp-2`, Tab. 14-15 in `cv-risultati`). 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. +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, 54 incomplete; DOI errati nelle voci 47, 48 (corretto 10.1080/15583720802231833) e 49; voci 47, 49, 54 non identificabili; segnaposto "paragrafo XX (XX)" in 4.4.4 (risolto nella versione del 2026-10-13); discrepanze figura/testo sopra elencate. ## Workflow @@ -107,7 +107,7 @@ Leggi `index.md` e le pagine rilevanti (non rileggere `raw/` se la wiki basta); 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. +- `index.md`: catalogo per categoria (Overview, Tesi e bibliografia, Concetti, Composti, Tecniche, Figure, Analisi), voci `- [[pagina]] — riga di sintesi`, ordine alfabetico, conteggi aggiornati. Le 79 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 diff --git a/index.md b/index.md index aa60475..a4ae825 100644 --- a/index.md +++ b/index.md @@ -1,13 +1,13 @@ # Indice della wiki -_Catalogo di tutte le pagine. Aggiornato a ogni ingest/query. Pagine curate: 29 · Figure generate: 78 · Fonti ingerite: 1 (la tesi)_ +_Catalogo di tutte le pagine. Aggiornato a ogni ingest/query. Pagine curate: 29 · Figure generate: 79 · 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) +- [[bibliografia]] — i 60 riferimenti con link alle schede in `raw/fonti/` (generata) - [[tesi]] — mappa sezione → pagine wiki → figure ## Concetti @@ -24,14 +24,14 @@ _Catalogo di tutte le pagine. Aggiornato a ogni ingest/query. Pagine curate: 29 - [[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) +- [[bottle-brush-3-x]] — i sei bottle brush 3.1b-3.3c (Tab. 4, 10-13, procedura) +- [[copolimeri-3a-3b-3c]] — copolimeri DPP-3HT (Tab. 3, 7-9, procedura) - [[dpp-1]] — DPP tiofenico (procedura, pseudo-Stobbe, spettri) - [[dpp-2]] — monomero bis-idrossiesil (procedura, N-alchilazione, Tab. 5) ## Tecniche - [[ciclovoltammetria]] — teoria (Eq. 6-8), procedura, metodo di analisi (Eq. 11-12) -- [[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) +- [[cv-risultati]] — Tab. 14 (bandgap 0,970-1,371 eV, correlazione con % DPP, confronto con P3HT) e Tab. 15 (bottle brush, 0,929-1,521 eV) - [[dsc]] — programma termico e risultati - [[ft-ir]] — bande diagnostiche - [[gpc]] — condizioni e interpretazione della sottostima @@ -40,7 +40,7 @@ _Catalogo di tutte le pagine. Aggiornato a ogni ingest/query. Pagine curate: 29 - [[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); elenco per sezione in [[tesi]] +- `wiki/figures/` — 79 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, 3 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 7e3c5fb..2f577e1 100644 --- a/log.md +++ b/log.md @@ -57,3 +57,25 @@ _Append-only. Formato: `## [YYYY-MM-DD] tipo | titolo`_ ## [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) + +## [2026-10-13] ingest | raw/tesi.md aggiornato alla nuova versione (tesi_new.docx) +- Su richiesta esplicita dell'utente `raw/tesi.md` è stato modificato (eccezione alla regola «raw/ sola lettura»); i numeri di riga citati nella wiki (`tesi_loc`, `md_line`, `cited_in_md_lines`) sono ora disallineati e la wiki non è ancora stata aggiornata +- Novità: §4.1 CV del prodotto 2 (Fig. 52, Tab. 6; l'immagine non è stata estratta perché nel docx è un grafico Word nativo), Tab. 3/4/7/9/12/13/15 riformulate, Tab. 6-14 → 7-15, Fig. 52-74 → 53-75, nuova rif. 51 (Scurti et al.) e riferimenti 51-59 → 52-60, nuovi dati NMR di 1 e 2, λem/λecc, DSC, formula V_CL, decimali con il punto +- Copiati alla lettera anche refusi della nuova versione (es. «Gloss», «didiacetali», «alchidica», «asb», «3b. 3c», «l(MW_teor)»); non copiato il testo corrotto dei rif. 22 e 54 (lettere raddoppiate nel docx) + +## [2026-10-13] ingest | raw/immagini.json allineato alla nuova tesi.md +- Aggiunta `fig-052` (voltammogramma ciclico del prodotto 2, immagine `c43b5f5d…jpg`; descrizione letta dall'immagine, non verificata, `confidence: medium`); figure 52-74 rinumerate in 53-75 (id, number, label, caption_printed, search_text); 79 figure, 80 file immagine +- Riallineati tutti i numeri di riga (`md_line`, `caption_md_line`, `cited_in_md_lines`, sezioni) a `tesi.md` nuovo, le didascalie cambiate (es. λex, «Gloss», «Stati») e gli indici +- `wiki/figures/` NON rigenerata: i wikilink `[[fig-0NN]]` della wiki per N ≥ 52 puntano ancora alla numerazione vecchia + +## [2026-10-13] ingest | wiki/figures rigenerata e numerazioni figure/tabelle allineate +- `python scripts/gen_figures.py`: 79 note (nuova `fig-052`, `fig-053`…`fig-075` con la nuova numerazione) +- Nelle pagine wiki rinumerati per sostituzione meccanica `fig-0NN`, «Fig./Figura N» (N 52-74 → +1) e «Tab./Tabella N» (N 6-14 → +1); `dpp-2` ampliata con la CV di 2 (Fig. 52, Tab. 6) e `dati.md` con la riga Tab. 6 +- NON aggiornati: contenuto di pagine e `dati.md` per i dati cambiati nella tesi (Tab. 3/4/9/12/13/15, PD, NMR), numeri di riga `tesi_loc`/`r.NNN`, riferimenti bibliografici 51-59 → 52-60 (`raw/fonti`, `raw/bibliografia.json`, `wiki/bibliografia.md`); `lint.py` segnala i numeri non più presenti in `tesi.md` + +## [2026-10-13] ingest | wiki, bibliografia e schema allineati alla nuova versione della tesi +- Bibliografia: nuovo rif. 51 (Scurti et al., scheda `raw/fonti/51-scurti-2026.md` **parziale**, scritta da abstract e repository), vecchi 51-59 → 52-60 (file di `raw/fonti/` rinominati, `raw/bibliografia.json` e `wiki/bibliografia.md` rigenerati, wikilink e `refs:` delle pagine aggiornati); righe di `tesi.md` nelle schede mappate sul nuovo file +- Numeri di riga `r.NNN` di tutte le pagine rimappati (diff riga per riga tra vecchio e nuovo `tesi.md`; dove la riga è stata riscritta la corrispondenza è approssimata, ±qualche riga) +- Contenuti aggiornati: `copolimeri-3a-3b-3c` (Tab. 3, 7, 9, DSC), `bottle-brush-3-x` (Tab. 4, 12, 13, formula V_CL), `dpp-1`, `dpp-2` (NMR, λem/λecc), `cv-risultati` (Tab. 15 arrotondata), `nmr-1h`, `dsc`, `gpc`, `dati`, `riassunto-tesi`, `difetti-noti` (voci 2-5, 7, 10-13 riscritte o aggiunte; segnaposto XX risolto), concetti con piccoli ritocchi di testo +- `CLAUDE.md` (tipo `schema`): conteggi (1432 righe, 80 file, 79 figure, 60 riferimenti), righe dei capitoli, numeri delle figure con discrepanze, voce 54 +- Non verificato a mano: le sostituzioni meccaniche di Fig./Tab. nelle pagine; il lint segnala ancora numeri vecchi citati di proposito nelle note «versione precedente» diff --git a/raw/bibliografia.json b/raw/bibliografia.json index 518ac40..39eb202 100644 --- a/raw/bibliografia.json +++ b/raw/bibliografia.json @@ -3,8 +3,8 @@ "source": "tesi.md", "note": "Voce 1 assente nel markdown, recuperata da tesi.pdf p.108. Campi estratti con euristiche: 'text' e' la fonte di verita'.", "stats": { - "entries": 59, - "cited": 59, + "entries": 60, + "cited": 60, "with_doi": 5, "unparsed_authors": 1 }, @@ -12,7 +12,7 @@ { "id": 1, "anchor": "ref-1", - "md_line": 1295, + "md_line": 1314, "text": "Bao, W. W. *et al.* Diketopyrrolopyrrole (DPP)-Based Materials and Its Applications: A Review. *Front. Chem.* **8**, 679 (2020).", "authors": "Bao, W. W.", "year": 2020, @@ -42,7 +42,7 @@ { "id": 2, "anchor": "ref-2", - "md_line": 1297, + "md_line": 1316, "text": "Shaikh, S. A. L. *et al.* A minireview on diketopyrrolopyrrole chemistry: Historical perspective and recent developments. *Results Chem.* **4**, 100473 (2022).", "authors": "Shaikh, S. A. L.", "year": 2022, @@ -77,7 +77,7 @@ { "id": 3, "anchor": "ref-3", - "md_line": 1299, + "md_line": 1318, "text": "Auwalu, M. A. & Cheng, S. Diketopyrrolopyrrole Fluorescent Probes, Photophysical and Biological Applications. *Chemosensors* **9**, 44 (2021).", "authors": "Auwalu, M. A. & Cheng, S.", "year": 2021, @@ -107,7 +107,7 @@ { "id": 4, "anchor": "ref-4", - "md_line": 1301, + "md_line": 1320, "text": "Zhang, B. *et al.* Diketopyrrolopyrrole-based fluorescent probe for visualizing over-expressed carboxylesterase in fever via ratiometric imaging. *Talanta* **266**, 124971 (2024).", "authors": "Zhang, B.", "year": 2024, @@ -137,7 +137,7 @@ { "id": 5, "anchor": "ref-5", - "md_line": 1303, + "md_line": 1322, "text": "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).", "authors": "Iqbal, A.", "year": 1988, @@ -152,7 +152,7 @@ 150, 168, 271, - 742 + 739 ], "cited_in_sections": [ "1.1.1", @@ -173,7 +173,7 @@ { "id": 6, "anchor": "ref-6", - "md_line": 1305, + "md_line": 1324, "text": "Sprake, J. M. & Watson, K. D. 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R. & Criado-Gonzalez, M.", "year": 2025, @@ -1601,14 +1629,14 @@ "doi": null, "url": null, "cited_in_md_lines": [ - 832 + 847 ], "cited_in_sections": [ "4.2" ], "quality_flags": [], "fonte": { - "file": "fonti/52-abdel-aziz-2025.md", + "file": "fonti/53-abdel-aziz-2025.md", "stato": "verificata", "doi_verificato": "10.1039/d5mh00096c", "url": "https://doi.org/10.1039/d5mh00096c", @@ -1618,9 +1646,9 @@ } }, { - "id": 53, - "anchor": "ref-53", - "md_line": 1399, + "id": 54, + "anchor": "ref-54", + "md_line": 1420, "text": "Paganin, D. L., Bizzarri, P. C. & Lanzi, D. M. Sintesi e proprietà di nuovi polimeri tiofenici per applicazioni optoelettroniche.", "authors": "Paganin, D. L., Bizzarri, P. C. & Lanzi, D. M.", "year": null, @@ -1631,7 +1659,7 @@ "doi": null, "url": null, "cited_in_md_lines": [ - 840 + 855 ], "cited_in_sections": [ "4.2" @@ -1640,7 +1668,7 @@ "incomplete_in_source" ], "fonte": { - "file": "fonti/53-paganin-nd.md", + "file": "fonti/54-paganin-nd.md", "stato": "non_risolta", "doi_verificato": null, "url": null, @@ -1650,9 +1678,9 @@ } }, { - "id": 54, - "anchor": "ref-54", - "md_line": 1401, + "id": 55, + "anchor": "ref-55", + "md_line": 1422, "text": "Odian, G. G. *Principles of Polymerization*. (Wiley-Interscience, Hoboken, N.J, 2004).", "authors": "Odian, G. G.", "year": 2004, @@ -1663,14 +1691,14 @@ "doi": null, "url": null, "cited_in_md_lines": [ - 942 + 959 ], "cited_in_sections": [ "4.2" ], "quality_flags": [], "fonte": { - "file": "fonti/54-odian-2004.md", + "file": "fonti/55-odian-2004.md", "stato": "identificata_manualmente", "doi_verificato": "10.1002/047147875x", "url": "https://doi.org/10.1002/047147875x", @@ -1680,9 +1708,9 @@ } }, { - "id": 55, - "anchor": "ref-55", - "md_line": 1403, + "id": 56, + "anchor": "ref-56", + "md_line": 1424, "text": "Woodruff, M. A. & Hutmacher, D. W. The return of a forgotten polymer—Polycaprolactone in the 21st century. *Prog. Polym. Sci.* **35**, 1217–1256 (2010).", "authors": "Woodruff, M. A. & Hutmacher, D. W.", "year": 2010, @@ -1693,14 +1721,14 @@ "doi": null, "url": null, "cited_in_md_lines": [ - 967 + 986 ], "cited_in_sections": [ "4.3" ], "quality_flags": [], "fonte": { - "file": "fonti/55-woodruff-2010.md", + "file": "fonti/56-woodruff-2010.md", "stato": "verificata", "doi_verificato": "10.1016/j.progpolymsci.2010.04.002", "url": "https://doi.org/10.1016/j.progpolymsci.2010.04.002", @@ -1710,9 +1738,9 @@ } }, { - "id": 56, - "anchor": "ref-56", - "md_line": 1405, + "id": 57, + "anchor": "ref-57", + "md_line": 1426, "text": "Labet, M. & Thielemans, W. Synthesis of polycaprolactone: a review. *Chem. Soc. Rev.* **38**, 3484 (2009).", "authors": "Labet, M. & Thielemans, W.", "year": 2009, @@ -1723,15 +1751,15 @@ "doi": null, "url": null, "cited_in_md_lines": [ - 969, - 969 + 988, + 988 ], "cited_in_sections": [ "4.3" ], "quality_flags": [], "fonte": { - "file": "fonti/56-labet-2009.md", + "file": "fonti/57-labet-2009.md", "stato": "verificata", "doi_verificato": "10.1039/b820162p", "url": "https://doi.org/10.1039/b820162p", @@ -1741,9 +1769,9 @@ } }, { - "id": 57, - "anchor": "ref-57", - "md_line": 1407, + "id": 58, + "anchor": "ref-58", + "md_line": 1428, "text": "Floyd, T. G. *et al.* Cationic Bottlebrush Copolymers from Partially Hydrolyzed Poly(oxazoline)s. *Macromolecules* **54**, 9461–9473 (2021).", "authors": "Floyd, T. G.", "year": 2021, @@ -1754,14 +1782,14 @@ "doi": null, "url": null, "cited_in_md_lines": [ - 1060 + 1079 ], "cited_in_sections": [ "4.3" ], "quality_flags": [], "fonte": { - "file": "fonti/57-floyd-2021.md", + "file": "fonti/58-floyd-2021.md", "stato": "verificata", "doi_verificato": "10.1021/acs.macromol.1c01458", "url": "https://doi.org/10.1021/acs.macromol.1c01458", @@ -1771,9 +1799,9 @@ } }, { - "id": 58, - "anchor": "ref-58", - "md_line": 1409, + "id": 59, + "anchor": "ref-59", + "md_line": 1430, "text": "Kasha, M., Rawls, H. R. & Ashraf El-Bayoumi, M. The exciton model in molecular spectroscopy. *Pure Appl. Chem.* **11**, 371–392 (1965).", "authors": "Kasha, M., Rawls, H. R. & Ashraf El-Bayoumi, M.", "year": 1965, @@ -1784,14 +1812,14 @@ "doi": null, "url": null, "cited_in_md_lines": [ - 1260 + 1279 ], "cited_in_sections": [ "4.5" ], "quality_flags": [], "fonte": { - "file": "fonti/58-kasha-1965.md", + "file": "fonti/59-kasha-1965.md", "stato": "verificata", "doi_verificato": "10.1351/pac196511030371", "url": "https://doi.org/10.1351/pac196511030371", @@ -1801,9 +1829,9 @@ } }, { - "id": 59, - "anchor": "ref-59", - "md_line": 1411, + "id": 60, + "anchor": "ref-60", + "md_line": 1432, "text": "Spano, F. C. & Silva, C. H- and J-Aggregate Behavior in Polymeric Semiconductors. *Annu. Rev. Phys. Chem.* **65**, 477–500 (2014).", "authors": "Spano, F. C. & Silva, C.", "year": 2014, @@ -1814,14 +1842,14 @@ "doi": null, "url": null, "cited_in_md_lines": [ - 1262 + 1281 ], "cited_in_sections": [ "4.5" ], "quality_flags": [], "fonte": { - "file": "fonti/59-spano-2014.md", + "file": "fonti/60-spano-2014.md", "stato": "verificata", "doi_verificato": "10.1146/annurev-physchem-040513-103639", "url": "https://doi.org/10.1146/annurev-physchem-040513-103639", diff --git a/raw/fonti/05-iqbal-1988.md b/raw/fonti/05-iqbal-1988.md index 90ad2f8..dca8b3a 100644 --- a/raw/fonti/05-iqbal-1988.md +++ b/raw/fonti/05-iqbal-1988.md @@ -78,7 +78,7 @@ Il testo completo non è ad accesso aperto e non è stato consultato: sono dispo - **Sez. 1.1.1 Storia e sintesi** (`tesi.md` r. 150): Allo stesso tempo, è diventato necessario l'impiego di un eccesso di base per compensare la porzione consumata dal DPP; quest'ultimo, data la sua natura relativamente acida, tende infatti a sottrarre base al sistema durante la sintesi[5,7]. - **Sez. 1.1.1 Storia e sintesi** (`tesi.md` r. 168): Una variante metodologica all'approccio classico, anche questo descritto da Iqbal et al.[5], prevede il passaggio attraverso i tetraidrodichetopirrolopirroli, i quali vengono sottoposti a un processo di deidrogenazione per generare il nucleo DPP finale. - **Sez. 1.1.2 Struttura e reattività** (`tesi.md` r. 271): È stato studiato come l'aggiunta di un semplice gruppo metile al DPP aumenti la solubilità di 27 volte in DMF.[5] -- **Sez. 4.1 Dichetopirrolopirroli** (`tesi.md` r. 742): La sintesi del composto 1 è stata eseguita sulla base delle procedure sintetiche descritte in letteratura, seguendo un meccanismo di ciclizzazione di tipo pseudo-Stobbe[5,7]. +- **Sez. 4.1 Dichetopirrolopirroli** (`tesi.md` r. 739): La sintesi del composto 1 è stata eseguita sulla base delle procedure sintetiche descritte in letteratura, seguendo un meccanismo di ciclizzazione di tipo pseudo-Stobbe[5,7]. ## Bibliografia della fonte diff --git a/raw/fonti/07-grzybowski-2015.md b/raw/fonti/07-grzybowski-2015.md index d125d28..1494182 100644 --- a/raw/fonti/07-grzybowski-2015.md +++ b/raw/fonti/07-grzybowski-2015.md @@ -75,8 +75,8 @@ Il testo completo non è ad accesso aperto e non è stato consultato: sono dispo - **Sez. 1.1.2 Struttura e reattività** (`tesi.md` r. 247): Per quanto riguarda la reattività dei DPP, invece, questa risulta essere varia per via dei diversi centri reattivi e del grande numero di sostituenti che posso essere introdotti nell'anello aromatico[7]. - **Sez. 1.1.2 Struttura e reattività** (`tesi.md` r. 301): Il gruppo di ricerca di Gryko et al.[7] ha proposto un diverso esempio di sostituzione elettrofila aromatica: i DPP con sostituenti aromatici elettron-ricchi possono essere alchilati in DMF usando K2CO3 come base e tetrabutilammonio bisolfato (TBAHS) come catalizzatore a trasferimento di fase (Figura 22). - **Sez. 1.1.2 Struttura e reattività** (`tesi.md` r. 305): Figura 22 - reazione di ciclizzazione mediante sostituzione elettrofila aromatica sui DPP studiata da Gryko et al.[7] -- **Sez. 4.1 Dichetopirrolopirroli** (`tesi.md` r. 742): La sintesi del composto 1 è stata eseguita sulla base delle procedure sintetiche descritte in letteratura, seguendo un meccanismo di ciclizzazione di tipo pseudo-Stobbe[5,7]. -- **Sez. 4.1 Dichetopirrolopirroli** (`tesi.md` r. 748): In particolare, è stato scelto il diisopropil succinato per aumentare l'ingombro sterico intorno al carbonile e diminuire ulteriormente la possibilità dell'estere di subire autocondensazione di Claisen e successiva ciclizzazione, come riportato in letteratura.[7] +- **Sez. 4.1 Dichetopirrolopirroli** (`tesi.md` r. 739): La sintesi del composto 1 è stata eseguita sulla base delle procedure sintetiche descritte in letteratura, seguendo un meccanismo di ciclizzazione di tipo pseudo-Stobbe[5,7]. +- **Sez. 4.1 Dichetopirrolopirroli** (`tesi.md` r. 745): In particolare, è stato scelto il diisopropil succinato per aumentare l'ingombro sterico intorno al carbonile e diminuire ulteriormente la possibilità dell'estere di subire autocondensazione di Claisen e successiva ciclizzazione, come riportato in letteratura.[7] ## Bibliografia della fonte diff --git a/raw/fonti/50-cardona-2011.md b/raw/fonti/50-cardona-2011.md index dc6224a..3eeca61 100644 --- a/raw/fonti/50-cardona-2011.md +++ b/raw/fonti/50-cardona-2011.md @@ -76,7 +76,7 @@ Il testo completo non è ad accesso aperto e non è stato consultato: sono dispo ## Come è citata nella tesi -- **Sez. 3.4 Procedure sperimentali delle analisi voltammetriche** (`tesi.md` r. 714): Sfruttando il comportamento reversibile e il potenziale noto della coppia redox Fc/Fc+, è stato possibile calibrare l'asse dei potenziali e riferire i valori di onset sperimentali alla scala assoluta delle energie nel vuoto, passaggio indispensabile per un calcolo rigoroso dei livelli energetici HOMO e LUMO dei materiali.[50] +- **Sez. 3.4 Procedure sperimentali delle analisi voltammetriche** (`tesi.md` r. 711): Sfruttando il comportamento reversibile e il potenziale noto della coppia redox Fc/Fc+, è stato possibile calibrare l'asse dei potenziali e riferire i valori di onset sperimentali alla scala assoluta delle energie nel vuoto, passaggio indispensabile per un calcolo rigoroso dei livelli energetici HOMO e LUMO dei materiali.[50] ## Bibliografia della fonte diff --git a/raw/fonti/51-scurti-2026.md b/raw/fonti/51-scurti-2026.md new file mode 100644 index 0000000..16ec45c --- /dev/null +++ b/raw/fonti/51-scurti-2026.md @@ -0,0 +1,47 @@ +--- +id: 51 +anchor: ref-51 +stato: parziale +doi: 10.1016/j.dyepig.2025.113288 +url: https://doi.org/10.1016/j.dyepig.2025.113288 +anno: 2026 +rivista: "Dyes and Pigments" +volume: "245" +pagine: "113288" +tipo: journal-article +autori: ["S. Scurti", "O. Racchi", "V. Spinoso", "A. Bussolari", "G. D'Altri", "I. Gualandi", "F. Di Maiolo", "C. Sissa", "D. Caretti"] +contenuto_letto: abstract +tags: [fonte, bibliografia] +cited_in_sections: [4.1] +--- + +# [51] Scurti (2026) - Symmetric azobenzene-substituted diketopyrrolopyrroles dyes as acid-base switchable molecular-probe for colorimetric paper-based sensors + +## Come è scritta nella tesi + +Scurti, S. *et al.* Symmetric azobenzene-substituted diketopyrrolopyrroles dyes as acid-base switchable molecular-probe for colorimetric paper-based sensors. *Dyes Pigments* **245**, 113288 (2026). + +## Scheda bibliografica + +**Citazione completa:** Scurti, S.; Racchi, O.; Spinoso, V.; Bussolari, A.; D'Altri, G.; Gualandi, I.; Di Maiolo, F.; Sissa, C.; Caretti, D. Symmetric azobenzene-substituted diketopyrrolopyrroles dyes as acid-base switchable molecular-probe for colorimetric paper-based sensors. *Dyes and Pigments* **2026**, 245, 113288. https://doi.org/10.1016/j.dyepig.2025.113288 + +- **Pubblicato in:** Dyes and Pigments (ISSN 0143-7208), vol. 245, art. 113288 (2026; data di pubblicazione indicata dal repository: 2026-01-01) + +## Stato della verifica + +**Parziale**: dati bibliografici letti dalla scheda del repository dell'Università di Parma (https://air.unipr.it/handle/11381/3044494) e da una ricerca web; scheda non generata da Crossref/OpenAlex come le altre e testo integrale non letto. + +## Dove trovarla + +- **DOI:** https://doi.org/10.1016/j.dyepig.2025.113288 +- **Repository (IRIS):** https://hdl.handle.net/11381/3044494 + +## Contenuto in sintesi + +*Riassunto in italiano dall'abstract (non dal testo integrale).* Sintesi di DPP simmetrici sostituiti con azobenzene mediante condensazione pseudo-Stobbe di benzonitrili seguita da accoppiamento azoico; i gruppi elettron-donatori (es. ammino) favoriscono un isomero strutturale del DPP (isoDPP) per effetto degli equilibri acido-base. I coloranti cambiano colore con il pH in modo prevedibile dai sostituenti; il derivato fenolico (2a) dà lo spostamento maggiore (90 nm). Il meccanismo è supportato da NMR e calcoli TD-DFT; sensori su carta rivestiti per immersione mostrano cambi di colore reversibili con HCl e NH3 in fase liquida e gassosa. + +## Come è citata nella tesi + +- **Sez. 4.1 Dichetopirrolopirroli** (`tesi.md` r. 727): al termine del paragrafo sull'isomero iso-DPP, dove la fluorescenza nel visibile è inibita per l'attivazione di processi di rilassamento non radiativo[51]. Questo riferimento è presente solo nella nuova versione della tesi. + +[Torna alla bibliografia della tesi](../tesi.md#ref-51) · Scheda scritta a mano (non generata dal catalogo). diff --git a/raw/fonti/51-wang-2022.md b/raw/fonti/52-wang-2022.md similarity index 97% rename from raw/fonti/51-wang-2022.md rename to raw/fonti/52-wang-2022.md index b1e550c..e86ae95 100644 --- a/raw/fonti/51-wang-2022.md +++ b/raw/fonti/52-wang-2022.md @@ -1,6 +1,6 @@ --- -id: 51 -anchor: ref-51 +id: 52 +anchor: ref-52 stato: verificata doi: 10.1039/d2sc05580e url: https://doi.org/10.1039/d2sc05580e @@ -22,7 +22,7 @@ tags: [fonte, bibliografia] cited_in_sections: [4.1] --- -# [51] Wang (2022) - Robust singlet fission process in strong absorption π-expanded diketopyrrolopyrroles +# [52] Wang (2022) - Robust singlet fission process in strong absorption π-expanded diketopyrrolopyrroles ## Come è scritta nella tesi @@ -118,13 +118,13 @@ Gli Ex-DPP combinano forte assorbimento, rigidità (alta resa di fluorescenza, s - Nessuna tabella; dati nel testo e nelle figure; ESI con XRD/GIWAXS e calcolo delle rese. ### Collegamento con la tesi -È citata (rif. 51) nella tabella delle proprietà ottiche (sez. 4.1, riga 814) in corrispondenza del coefficiente di estinzione molare 28000 M^-1 cm^-1 del prodotto 1: la tesi la usa come riferimento di letteratura per i valori di ε e le proprietà spettrali di cromofori DPP. Attenzione: il valore 28000 non coincide con quelli letti nel testo (7,0 x 10^4 per Ex-DPP; i riferimenti TDPP/PhDPP sono dedotti solo come rapporti), quindi conviene verificarlo nell'articolo (Fig. 3c e ESI) o negli SI. Parti utili: Fig. 3 (assorbimento, ε, emissione DPP in soluzione e film) e il confronto soluzione/film per la perdita di fluorescenza in stato solido. +È citata (rif. 52) nella tabella delle proprietà ottiche (sez. 4.1, riga 811) in corrispondenza del coefficiente di estinzione molare 28000 M^-1 cm^-1 del prodotto 1: la tesi la usa come riferimento di letteratura per i valori di ε e le proprietà spettrali di cromofori DPP. Attenzione: il valore 28000 non coincide con quelli letti nel testo (7,0 x 10^4 per Ex-DPP; i riferimenti TDPP/PhDPP sono dedotti solo come rapporti), quindi conviene verificarlo nell'articolo (Fig. 3c e ESI) o negli SI. Parti utili: Fig. 3 (assorbimento, ε, emissione DPP in soluzione e film) e il confronto soluzione/film per la perdita di fluorescenza in stato solido. > **Note del revisore:** Letto via pagina PMC (il PDF RSC ha dato 403). Riassunto del testo reso dallo strumento; il significato del valore 28000 citato in tesi non è chiaro dal testo (probabile confronto). ## Come è citata nella tesi -- **Sez. 4.1 Dichetopirrolopirroli** (`tesi.md` r. 814): 1 | 531 | 542 | 11 | 28000[51] +- **Sez. 4.1 Dichetopirrolopirroli** (`tesi.md` r. 811): 1 | 531 | 542 | 11 | 28000[52] ## Bibliografia della fonte @@ -186,4 +186,4 @@ La fonte cita 50 riferimenti (mostrati i primi 40; elenco completo: https://api. - Citata **26** volte (OpenAlex); riferimenti nella fonte: 51 - Citazioni per anno: 2026: 5, 2025: 11, 2024: 2, 2023: 8 -[Torna alla bibliografia della tesi](../tesi.md#ref-51) · Generata dal catalogo `bibliografia.json` e da Crossref, OpenAlex, Europe PMC. +[Torna alla bibliografia della tesi](../tesi.md#ref-52) · Generata dal catalogo `bibliografia.json` e da Crossref, OpenAlex, Europe PMC. diff --git a/raw/fonti/52-abdel-aziz-2025.md b/raw/fonti/53-abdel-aziz-2025.md similarity index 97% rename from raw/fonti/52-abdel-aziz-2025.md rename to raw/fonti/53-abdel-aziz-2025.md index 5862e5d..0d8447d 100644 --- a/raw/fonti/52-abdel-aziz-2025.md +++ b/raw/fonti/53-abdel-aziz-2025.md @@ -1,6 +1,6 @@ --- -id: 52 -anchor: ref-52 +id: 53 +anchor: ref-53 stato: verificata doi: 10.1039/d5mh00096c url: https://doi.org/10.1039/d5mh00096c @@ -22,7 +22,7 @@ tags: [fonte, bibliografia] cited_in_sections: [4.2] --- -# [52] Abdel Aziz (2025) - Poly(3-hexylthiophene) as a versatile semiconducting polymer for cutting-edge bioelectronics +# [53] Abdel Aziz (2025) - Poly(3-hexylthiophene) as a versatile semiconducting polymer for cutting-edge bioelectronics ## Come è scritta nella tesi @@ -99,13 +99,13 @@ Il P3HT è biocompatibile con buone proprietà ottiche e conduttive; le applicaz Fig. 1-8 (struttura/proprietà del P3HT, forme del materiale, stimolazione cellulare in Fig. 7, drug delivery in Fig. 8E-G); Fig. 9 (trimeri di tiofene e polimerizzazione in vivo); Tabella 1 (riepilogo condizioni di illuminazione e modelli biologici: lunghezze d'onda 410-623 nm, intensità 0,0126-344 mW/mm2). ### Collegamento con la tesi -Citata (rif. 52) alla sez. 4.2, dove la scelta del 3HT come comonomero è motivata dal fatto che i politiofeni sono tra i polimeri semiconduttori organici più efficienti, con la catena esilica per la solubilità e l'anello tiofenico per l'estensione della coniugazione e la modulazione del band gap. Parti utili per approfondire: sezione 2 (sintesi, struttura, livelli energetici HOMO/LUMO, ruolo della regioregolarità, in particolare la polimerizzazione ossidativa con FeCl3) e le conclusioni. Le applicazioni biomediche sono solo contesto. +Citata (rif. 53) alla sez. 4.2, dove la scelta del 3HT come comonomero è motivata dal fatto che i politiofeni sono tra i polimeri semiconduttori organici più efficienti, con la catena esilica per la solubilità e l'anello tiofenico per l'estensione della coniugazione e la modulazione del band gap. Parti utili per approfondire: sezione 2 (sintesi, struttura, livelli energetici HOMO/LUMO, ruolo della regioregolarità, in particolare la polimerizzazione ossidativa con FeCl3) e le conclusioni. Le applicazioni biomediche sono solo contesto. > **Note del revisore:** Letto tramite PMC in due passaggi (caratteri 0-100000 e 100000-fine). Primo passaggio troncato nella sez. 4.3; il secondo ha coperto il resto. Nota dello strumento: unità del coefficiente di assorbimento sospetta, non riportata qui. ## Come è citata nella tesi -- **Sez. 4.2 Copolimeri coniugati** (`tesi.md` r. 832): Sotto il profilo strutturale e funzionale, la selezione del 3HT è motivata dalle note proprietà elettroniche dei politiofeni, classificati in letteratura tra i più efficienti polimeri semiconduttori organici.[52] +- **Sez. 4.2 Copolimeri coniugati** (`tesi.md` r. 847): Sotto il profilo strutturale e funzionale, la selezione del 3HT è motivata dalle note proprietà elettroniche dei politiofeni, classificati in letteratura tra i più efficienti polimeri semiconduttori organici.[53] ## Bibliografia della fonte @@ -167,4 +167,4 @@ La fonte cita 131 riferimenti (mostrati i primi 40; elenco completo: https://api - Citata **29** volte (OpenAlex); riferimenti nella fonte: 131 - Citazioni per anno: 2026: 20, 2025: 9 -[Torna alla bibliografia della tesi](../tesi.md#ref-52) · Generata dal catalogo `bibliografia.json` e da Crossref, OpenAlex, Europe PMC. +[Torna alla bibliografia della tesi](../tesi.md#ref-53) · Generata dal catalogo `bibliografia.json` e da Crossref, OpenAlex, Europe PMC. diff --git a/raw/fonti/53-paganin-nd.md b/raw/fonti/54-paganin-nd.md similarity index 90% rename from raw/fonti/53-paganin-nd.md rename to raw/fonti/54-paganin-nd.md index b7d2b25..2737a24 100644 --- a/raw/fonti/53-paganin-nd.md +++ b/raw/fonti/54-paganin-nd.md @@ -1,6 +1,6 @@ --- -id: 53 -anchor: ref-53 +id: 54 +anchor: ref-54 stato: non_risolta doi: null url: null @@ -22,7 +22,7 @@ tags: [fonte, bibliografia] cited_in_sections: [4.2] --- -# [53] Paganin (s.d.) - Sintesi e proprietà di nuovi polimeri tiofenici per applicazioni optoelettroniche +# [54] Paganin (s.d.) - Sintesi e proprietà di nuovi polimeri tiofenici per applicazioni optoelettroniche ## Come è scritta nella tesi @@ -60,10 +60,10 @@ Il testo completo non è ad accesso aperto e non è stato consultato: sono dispo ## Come è citata nella tesi -- **Sez. 4.2 Copolimeri coniugati** (`tesi.md` r. 840): Il centro metallico Fe3+ promuove l'attivazione dei monomeri attraverso un processo di trasferimento mono-elettronico (Single Electron Transfer, SET)[53]. +- **Sez. 4.2 Copolimeri coniugati** (`tesi.md` r. 855): Il centro metallico Fe3+ promuove l'attivazione dei monomeri attraverso un processo di trasferimento mono-elettronico (Single Electron Transfer, SET)[53]. ## Bibliografia della fonte Non applicabile. -[Torna alla bibliografia della tesi](../tesi.md#ref-53) · Generata dal catalogo `bibliografia.json` e da Crossref, OpenAlex, Europe PMC. +[Torna alla bibliografia della tesi](../tesi.md#ref-54) · Generata dal catalogo `bibliografia.json` e da Crossref, OpenAlex, Europe PMC. diff --git a/raw/fonti/54-odian-2004.md b/raw/fonti/55-odian-2004.md similarity index 97% rename from raw/fonti/54-odian-2004.md rename to raw/fonti/55-odian-2004.md index 3b0134b..b7cb1cb 100644 --- a/raw/fonti/54-odian-2004.md +++ b/raw/fonti/55-odian-2004.md @@ -1,6 +1,6 @@ --- -id: 54 -anchor: ref-54 +id: 55 +anchor: ref-55 stato: identificata_manualmente doi: 10.1002/047147875x url: https://doi.org/10.1002/047147875x @@ -22,7 +22,7 @@ tags: [fonte, bibliografia] cited_in_sections: [4.2] --- -# [54] Odian (2004) - +# [55] Odian (2004) - ## Come è scritta nella tesi @@ -73,7 +73,7 @@ Il testo completo non è ad accesso aperto e non è stato consultato: sono dispo ## Come è citata nella tesi -- **Sez. 4.2 Copolimeri coniugati** (`tesi.md` r. 942): Nei processi convenzionali, infatti, l'assenza di un rigoroso controllo sulla cinetica di crescita e sulle reazioni di terminazione o trasferimento di catena porta a distribuzioni dei pesi molecolari ampie, con valori teorici e sperimentali di PD che si assestano tipicamente attorno a 2 (distribuzione più probabile di Flory) o superiori.[54] +- **Sez. 4.2 Copolimeri coniugati** (`tesi.md` r. 959): Nei processi convenzionali, infatti, l'assenza di un rigoroso controllo sulla cinetica di crescita e sulle reazioni di terminazione o trasferimento di catena porta a distribuzioni dei pesi molecolari ampie, con valori teorici e sperimentali di PD che si assestano tipicamente attorno a 2 (distribuzione più probabile di Flory) o superiori.[55] ## Bibliografia della fonte @@ -95,4 +95,4 @@ Elenco dei riferimenti non depositato dall'editore su Crossref. - Citata **7144** volte (OpenAlex) - Citazioni per anno: 2026: 132, 2025: 187, 2024: 203, 2023: 212, 2022: 210, 2021: 284 -[Torna alla bibliografia della tesi](../tesi.md#ref-54) · Generata dal catalogo `bibliografia.json` e da Crossref, OpenAlex, Europe PMC. +[Torna alla bibliografia della tesi](../tesi.md#ref-55) · Generata dal catalogo `bibliografia.json` e da Crossref, OpenAlex, Europe PMC. diff --git a/raw/fonti/55-woodruff-2010.md b/raw/fonti/56-woodruff-2010.md similarity index 98% rename from raw/fonti/55-woodruff-2010.md rename to raw/fonti/56-woodruff-2010.md index bf22b6d..c7ab4cf 100644 --- a/raw/fonti/55-woodruff-2010.md +++ b/raw/fonti/56-woodruff-2010.md @@ -1,6 +1,6 @@ --- -id: 55 -anchor: ref-55 +id: 56 +anchor: ref-56 stato: verificata doi: 10.1016/j.progpolymsci.2010.04.002 url: https://doi.org/10.1016/j.progpolymsci.2010.04.002 @@ -22,7 +22,7 @@ tags: [fonte, bibliografia] cited_in_sections: [4.3] --- -# [55] Woodruff (2010) - The return of a forgotten polymer—Polycaprolactone in the 21st century +# [56] Woodruff (2010) - The return of a forgotten polymer—Polycaprolactone in the 21st century ## Come è scritta nella tesi @@ -90,13 +90,13 @@ Le proprietà reologiche e viscoelastiche, il costo contenuto, l'approvazione FD Fig. 1 (trend delle pubblicazioni), Fig. 2 (scaffold), Fig. 3-5 (meccanismi e cinetiche di degradazione), Fig. 6-16 (applicazioni e scaffold); Tabella 1 (proprietà dei polimeri: Tg, Tm, proprietà meccaniche) e Tabella 2 (definizioni di biodegradabile, bioriassorbibile, ecc.). ### Collegamento con la tesi -Citata (rif. 55) alla sez. 4.3 per giustificare la scelta del PCL come catena laterale: ROP lineare ed efficiente dal -OH terminale dell'unità DPP (grafting from), bassa Tg e buona solubilità nei solventi organici. Utili a questo fine la sezione 2 (sintesi, Tg, Tm, solubilità, miscibilità, Tabella 1); le parti biomediche sono marginali per la tesi. +Citata (rif. 56) alla sez. 4.3 per giustificare la scelta del PCL come catena laterale: ROP lineare ed efficiente dal -OH terminale dell'unità DPP (grafting from), bassa Tg e buona solubilità nei solventi organici. Utili a questo fine la sezione 2 (sintesi, Tg, Tm, solubilità, miscibilità, Tabella 1); le parti biomediche sono marginali per la tesi. > **Note del revisore:** Il PDF non è passato da WebFetch; testo estratto con pdftotext dal PDF scaricato (autore, versione accettata, circa 30000 parole). Letti per intero introduzione, sez. 2-3, parti di 5 e le sez. 10-11; le sezioni su scaffold, sterilizzazione e applicazioni solo per titoli. ## Come è citata nella tesi -- **Sez. 4.3 Polimeri bottle brush** (`tesi.md` r. 967): Per quanto riguarda le proprietà chimico-fisiche, invece, il PCL è caratterizzato da una bassa temperatura di transizione vetrosa (Tg) e da una buona solubilità nei comuni solventi organici[55]. +- **Sez. 4.3 Polimeri bottle brush** (`tesi.md` r. 986): Per quanto riguarda le proprietà chimico-fisiche, invece, il PCL è caratterizzato da una bassa temperatura di transizione vetrosa (Tg) e da una buona solubilità nei comuni solventi organici[55]. ## Bibliografia della fonte @@ -158,4 +158,4 @@ La fonte cita 217 riferimenti (mostrati i primi 40; elenco completo: https://api - Citata **4012** volte (OpenAlex); riferimenti nella fonte: 207 - Citazioni per anno: 2026: 233, 2025: 295, 2024: 256, 2023: 250, 2022: 313, 2021: 327 -[Torna alla bibliografia della tesi](../tesi.md#ref-55) · Generata dal catalogo `bibliografia.json` e da Crossref, OpenAlex, Europe PMC. +[Torna alla bibliografia della tesi](../tesi.md#ref-56) · Generata dal catalogo `bibliografia.json` e da Crossref, OpenAlex, Europe PMC. diff --git a/raw/fonti/56-labet-2009.md b/raw/fonti/57-labet-2009.md similarity index 97% rename from raw/fonti/56-labet-2009.md rename to raw/fonti/57-labet-2009.md index e2cc618..d2b0679 100644 --- a/raw/fonti/56-labet-2009.md +++ b/raw/fonti/57-labet-2009.md @@ -1,6 +1,6 @@ --- -id: 56 -anchor: ref-56 +id: 57 +anchor: ref-57 stato: verificata doi: 10.1039/b820162p url: https://doi.org/10.1039/b820162p @@ -22,7 +22,7 @@ tags: [fonte, bibliografia] cited_in_sections: [4.3] --- -# [56] Labet (2009) - Synthesis of polycaprolactone: a review +# [57] Labet (2009) - Synthesis of polycaprolactone: a review ## Come è scritta nella tesi @@ -73,8 +73,8 @@ Il testo completo non è ad accesso aperto e non è stato consultato: sono dispo ## Come è citata nella tesi -- **Sez. 4.3 Polimeri bottle brush** (`tesi.md` r. 969): La reazione di polimerizzazione ROP presenta diversi possibili meccanismi[56], uno dei più sfruttati è quello di coordinazione-inserzione del monomero sul centro attivo dell'iniziatore. In particolare, la reazione di apertura dell'anello catalizzata da stagno ottanoato (Sn(Oct)2) richiede generalmente l'aggiunta di co-iniziatori nucleofili come alcol[56]. -- **Sez. 4.3 Polimeri bottle brush** (`tesi.md` r. 969): La reazione di polimerizzazione ROP presenta diversi possibili meccanismi[56], uno dei più sfruttati è quello di coordinazione-inserzione del monomero sul centro attivo dell'iniziatore. In particolare, la reazione di apertura dell'anello catalizzata da stagno ottanoato (Sn(Oct)2) richiede generalmente l'aggiunta di co-iniziatori nucleofili come alcol[56]. +- **Sez. 4.3 Polimeri bottle brush** (`tesi.md` r. 988): La reazione di polimerizzazione ROP presenta diversi possibili meccanismi[56], uno dei più sfruttati è quello di coordinazione-inserzione del monomero sul centro attivo dell'iniziatore. In particolare, la reazione di apertura dell'anello catalizzata da stagno ottanoato (Sn(Oct)2) richiede generalmente l'aggiunta di co-iniziatori nucleofili come alcol[56]. +- **Sez. 4.3 Polimeri bottle brush** (`tesi.md` r. 988): La reazione di polimerizzazione ROP presenta diversi possibili meccanismi[56], uno dei più sfruttati è quello di coordinazione-inserzione del monomero sul centro attivo dell'iniziatore. In particolare, la reazione di apertura dell'anello catalizzata da stagno ottanoato (Sn(Oct)2) richiede generalmente l'aggiunta di co-iniziatori nucleofili come alcol[56]. ## Bibliografia della fonte @@ -137,4 +137,4 @@ La fonte cita 130 riferimenti (mostrati i primi 40; elenco completo: https://api - Citata **1667** volte (OpenAlex); riferimenti nella fonte: 131 - Citazioni per anno: 2026: 69, 2025: 144, 2024: 130, 2023: 139, 2022: 153, 2021: 151 -[Torna alla bibliografia della tesi](../tesi.md#ref-56) · Generata dal catalogo `bibliografia.json` e da Crossref, OpenAlex, Europe PMC. +[Torna alla bibliografia della tesi](../tesi.md#ref-57) · Generata dal catalogo `bibliografia.json` e da Crossref, OpenAlex, Europe PMC. diff --git a/raw/fonti/57-floyd-2021.md b/raw/fonti/58-floyd-2021.md similarity index 97% rename from raw/fonti/57-floyd-2021.md rename to raw/fonti/58-floyd-2021.md index 3d12b03..d8116f2 100644 --- a/raw/fonti/57-floyd-2021.md +++ b/raw/fonti/58-floyd-2021.md @@ -1,6 +1,6 @@ --- -id: 57 -anchor: ref-57 +id: 58 +anchor: ref-58 stato: verificata doi: 10.1021/acs.macromol.1c01458 url: https://doi.org/10.1021/acs.macromol.1c01458 @@ -22,7 +22,7 @@ tags: [fonte, bibliografia] cited_in_sections: [4.3] --- -# [57] Floyd (2021) - Cationic Bottlebrush Copolymers from Partially Hydrolyzed Poly(oxazoline)s +# [58] Floyd (2021) - Cationic Bottlebrush Copolymers from Partially Hydrolyzed Poly(oxazoline)s ## Come è scritta nella tesi @@ -77,7 +77,7 @@ Il testo completo non è ad accesso aperto e non è stato consultato: sono dispo ## Come è citata nella tesi -- **Sez. 4.3 Polimeri bottle brush** (`tesi.md` r. 1060): Al contrario, aumentando il peso molecolare dei segmenti laterali (ad esempio stimando tre catene per lato, per un peso teorico atteso di circa 62000 Da), la drastica compattazione strutturale porta a una sottostima del peso reale che si aggira intorno al 70%.[57] +- **Sez. 4.3 Polimeri bottle brush** (`tesi.md` r. 1079): Al contrario, aumentando il peso molecolare dei segmenti laterali (ad esempio stimando tre catene per lato, per un peso teorico atteso di circa 62000 Da), la drastica compattazione strutturale porta a una sottostima del peso reale che si aggira intorno al 70%.[58] ## Bibliografia della fonte @@ -140,4 +140,4 @@ La fonte cita 67 riferimenti (mostrati i primi 40; elenco completo: https://api. - Citata **14** volte (OpenAlex); riferimenti nella fonte: 66 - Citazioni per anno: 2025: 2, 2024: 4, 2023: 1, 2022: 6, 2021: 1 -[Torna alla bibliografia della tesi](../tesi.md#ref-57) · Generata dal catalogo `bibliografia.json` e da Crossref, OpenAlex, Europe PMC. +[Torna alla bibliografia della tesi](../tesi.md#ref-58) · Generata dal catalogo `bibliografia.json` e da Crossref, OpenAlex, Europe PMC. diff --git a/raw/fonti/58-kasha-1965.md b/raw/fonti/59-kasha-1965.md similarity index 97% rename from raw/fonti/58-kasha-1965.md rename to raw/fonti/59-kasha-1965.md index 3c96551..6f8babb 100644 --- a/raw/fonti/58-kasha-1965.md +++ b/raw/fonti/59-kasha-1965.md @@ -1,6 +1,6 @@ --- -id: 58 -anchor: ref-58 +id: 59 +anchor: ref-59 stato: verificata doi: 10.1351/pac196511030371 url: https://doi.org/10.1351/pac196511030371 @@ -22,7 +22,7 @@ tags: [fonte, bibliografia] cited_in_sections: [4.5] --- -# [58] Kasha (1965) - The exciton model in molecular spectroscopy +# [59] Kasha (1965) - The exciton model in molecular spectroscopy ## Come è scritta nella tesi @@ -87,13 +87,13 @@ Non verificabili senza il testo. È il riferimento storico da cui nascono i conc Non disponibili (testo non letto). ### Collegamento con la tesi -Citata (rif. 58) alla sez. 4.5 (riga 1260): la tesi usa la teoria dell'accoppiamento eccitonico di Kasha per distinguere aggregati H (face-to-face) e J (head-to-tail) e afferma che gli aggregati H presentano una transizione permessa verso lo stato eccitonico a più alta energia, quindi uno spostamento ipsocromico e una emissione ridotta. Per approfondire occorre la parte sul dimero eccitonico (splitting degli stati, regole di selezione in funzione della geometria). +Citata (rif. 59) alla sez. 4.5 (riga 1279): la tesi usa la teoria dell'accoppiamento eccitonico di Kasha per distinguere aggregati H (face-to-face) e J (head-to-tail) e afferma che gli aggregati H presentano una transizione permessa verso lo stato eccitonico a più alta energia, quindi uno spostamento ipsocromico e una emissione ridotta. Per approfondire occorre la parte sul dimero eccitonico (splitting degli stati, regole di selezione in funzione della geometria). > **Note del revisore:** Testo completo non ottenuto: de Gruyter 405/403 da WebFetch, IUPAC dietro Cloudflare. Il riassunto non va considerato una lettura dell'articolo. ## Come è citata nella tesi -- **Sez. 4.5 Caratterizzazione spettroscopica allo stato solido** (`tesi.md` r. 1260): Nei polimeri coniugati, le forti interazioni π-π favoriscono frequentemente la formazione di aggregati H, i quali presentano una transizione otticamente permessa verso lo stato eccitonico a maggiore energia.[58] +- **Sez. 4.5 Caratterizzazione spettroscopica allo stato solido** (`tesi.md` r. 1279): Nei polimeri coniugati, le forti interazioni π-π favoriscono frequentemente la formazione di aggregati H, i quali presentano una transizione otticamente permessa verso lo stato eccitonico a maggiore energia.[59] ## Bibliografia della fonte @@ -156,4 +156,4 @@ La fonte cita 1098 riferimenti (mostrati i primi 40; elenco completo: https://ap - Citata **4255** volte (OpenAlex); riferimenti nella fonte: 1079 - Citazioni per anno: 2026: 124, 2025: 169, 2024: 166, 2023: 161, 2022: 193, 2021: 180 -[Torna alla bibliografia della tesi](../tesi.md#ref-58) · Generata dal catalogo `bibliografia.json` e da Crossref, OpenAlex, Europe PMC. +[Torna alla bibliografia della tesi](../tesi.md#ref-59) · Generata dal catalogo `bibliografia.json` e da Crossref, OpenAlex, Europe PMC. diff --git a/raw/fonti/59-spano-2014.md b/raw/fonti/60-spano-2014.md similarity index 96% rename from raw/fonti/59-spano-2014.md rename to raw/fonti/60-spano-2014.md index d76672c..aa63d5e 100644 --- a/raw/fonti/59-spano-2014.md +++ b/raw/fonti/60-spano-2014.md @@ -1,6 +1,6 @@ --- -id: 59 -anchor: ref-59 +id: 60 +anchor: ref-60 stato: verificata doi: 10.1146/annurev-physchem-040513-103639 url: https://doi.org/10.1146/annurev-physchem-040513-103639 @@ -22,7 +22,7 @@ tags: [fonte, bibliografia] cited_in_sections: [4.5] --- -# [59] Spano (2014) - H- and J-Aggregate Behavior in Polymeric Semiconductors +# [60] Spano (2014) - H- and J-Aggregate Behavior in Polymeric Semiconductors ## Come è scritta nella tesi @@ -88,13 +88,13 @@ Non verificabili oltre l'abstract. Non disponibili. ### Collegamento con la tesi -Citata (rif. 59) alla sez. 4.5 (riga 1262), dove la tesi collega la formazione di aggregati H nei polimeri coniugati planari alla riduzione della resa quantica allo stato solido (ACQ) tramite rilassamento non radiativo. È coerente con l'abstract (interazioni interchain = comportamento H). Utili in particolare le sezioni sui politiofeni regioregolari (P3HT) e sul legame fra spettro vibronico (rapporto 0-0/0-1) e tipo di aggregazione. +Citata (rif. 60) alla sez. 4.5 (riga 1281), dove la tesi collega la formazione di aggregati H nei polimeri coniugati planari alla riduzione della resa quantica allo stato solido (ACQ) tramite rilassamento non radiativo. È coerente con l'abstract (interazioni interchain = comportamento H). Utili in particolare le sezioni sui politiofeni regioregolari (P3HT) e sul legame fra spettro vibronico (rapporto 0-0/0-1) e tipo di aggregazione. > **Note del revisore:** Testo completo non ottenuto (403). Riassunto basato solo sull'abstract; l'indicazione sul rapporto 0-0/0-1 è un suggerimento di lettura, non un contenuto verificato. ## Come è citata nella tesi -- **Sez. 4.5 Caratterizzazione spettroscopica allo stato solido** (`tesi.md` r. 1262): Di conseguenza, le rese quantiche di fluorescenza allo stato solido subiscono un drastico abbattimento rispetto a quelle misurate in soluzione.[59] +- **Sez. 4.5 Caratterizzazione spettroscopica allo stato solido** (`tesi.md` r. 1281): Di conseguenza, le rese quantiche di fluorescenza allo stato solido subiscono un drastico abbattimento rispetto a quelle misurate in soluzione.[60] ## Bibliografia della fonte @@ -157,4 +157,4 @@ La fonte cita 120 riferimenti (mostrati i primi 40; elenco completo: https://api - Citata **1121** volte (OpenAlex); riferimenti nella fonte: 124 - Citazioni per anno: 2026: 66, 2025: 105, 2024: 101, 2023: 93, 2022: 90, 2021: 117 -[Torna alla bibliografia della tesi](../tesi.md#ref-59) · Generata dal catalogo `bibliografia.json` e da Crossref, OpenAlex, Europe PMC. +[Torna alla bibliografia della tesi](../tesi.md#ref-60) · Generata dal catalogo `bibliografia.json` e da Crossref, OpenAlex, Europe PMC. diff --git a/raw/immagini.json b/raw/immagini.json index 2c627ba..67e783d 100644 --- a/raw/immagini.json +++ b/raw/immagini.json @@ -16,8 +16,8 @@ "quality": "confidence + flags + review_notes (discrepanze da verificare sul PDF/docx) + verification (esito della revisione indipendente: verdict ok/fix e issues trovate)" }, "stats": { - "figures": 78, - "image_files": 79 + "figures": 79, + "image_files": 80 }, "sections": [ { @@ -172,14 +172,14 @@ "number": "3.3", "title": "Principi teorici della ciclovoltammetria", "level": 2, - "md_line": 666, + "md_line": 663, "figure_ids": [] }, { "number": "3.4", "title": "Procedure sperimentali delle analisi voltammetriche", "level": 2, - "md_line": 702, + "md_line": 699, "figure_ids": [ "fig-039" ] @@ -188,14 +188,14 @@ "number": "4", "title": "Discussione dei risultati", "level": 1, - "md_line": 717, + "md_line": 714, "figure_ids": [] }, { "number": "4.1", "title": "Dichetopirrolopirroli", "level": 2, - "md_line": 722, + "md_line": 719, "figure_ids": [ "fig-040", "fig-041", @@ -208,16 +208,16 @@ "fig-048", "fig-049", "fig-050", - "fig-051" + "fig-051", + "fig-052" ] }, { "number": "4.2", "title": "Copolimeri coniugati", "level": 2, - "md_line": 826, + "md_line": 841, "figure_ids": [ - "fig-052", "fig-053", "fig-054", "fig-055", @@ -226,80 +226,81 @@ "fig-058", "fig-059", "fig-060", - "fig-061" + "fig-061", + "fig-062" ] }, { "number": "4.3", "title": "Polimeri bottle brush", "level": 2, - "md_line": 957, + "md_line": 976, "figure_ids": [ - "fig-062", "fig-063", "fig-064", "fig-065", "fig-066", "fig-067", - "fig-068" + "fig-068", + "fig-069" ] }, { "number": "4.4", "title": "Ciclovoltammetrie", "level": 2, - "md_line": 1100, + "md_line": 1119, "figure_ids": [] }, { "number": "4.4.1", "title": "Ciclovoltammetrie su polimeri elettroattivi", "level": 3, - "md_line": 1107, + "md_line": 1126, "figure_ids": [] }, { "number": "4.4.2", "title": "Metodologie di analisi voltammetrica", "level": 3, - "md_line": 1118, + "md_line": 1137, "figure_ids": [ - "fig-069", - "fig-070" + "fig-070", + "fig-071" ] }, { "number": "4.4.3", "title": "Proprietà elettrochimiche dei copolimeri lienari", "level": 3, - "md_line": 1175, + "md_line": 1194, "figure_ids": [ - "fig-071", "fig-072", - "fig-073" + "fig-073", + "fig-074" ] }, { "number": "4.4.4", "title": "Effetto del design bottle brush", "level": 3, - "md_line": 1230, + "md_line": 1249, "figure_ids": [] }, { "number": "4.5", "title": "Caratterizzazione spettroscopica allo stato solido", "level": 2, - "md_line": 1254, + "md_line": 1273, "figure_ids": [ - "fig-074" + "fig-075" ] }, { "number": "5", "title": "Conclusioni", "level": 1, - "md_line": 1279, + "md_line": 1298, "figure_ids": [] } ], @@ -898,10 +899,10 @@ "number": 9, "label": "Figura 9", "type": "reaction_scheme", - "title": "sintesi del DPP3 proposta da Closs e Gompper", + "title": "sintesi del DPP3 proposta da Gloss e Gompper", "caption": "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.", "alt_text": "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.", - "caption_printed": "Figura 9 - sintesi del DPP3 proposta da Closs e Gompper", + "caption_printed": "Figura 9 - sintesi del DPP3 proposta da Gloss e Gompper", "location": { "chapter": "1", "section": "1.1.1", @@ -965,7 +966,7 @@ "issues": [] } }, - "search_text": "Figura 9 | sintesi del DPP3 proposta da Closs e Gompper | 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. | 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. | composti: DPP3 | Closs-Gompper, succindiammide, t-BuOK, amidina" + "search_text": "Figura 9 | sintesi del DPP3 proposta da Gloss e Gompper | 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. | 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. | composti: DPP3 | Closs-Gompper, succindiammide, t-BuOK, amidina" }, { "id": "fig-010", @@ -2839,10 +2840,10 @@ "number": 33, "label": "Figura 33", "type": "diagram", - "title": "stati elettronici per molecole rigide e flessibili", + "title": "Stati elettronici per molecole rigide e flessibili", "caption": "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.", "alt_text": "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.", - "caption_printed": "Figura 33 - stati elettronici per molecole rigide e flessibili", + "caption_printed": "Figura 33 - Stati elettronici per molecole rigide e flessibili", "location": { "chapter": "1", "section": "1.2", @@ -2931,7 +2932,7 @@ ] } }, - "search_text": "Figura 33 | stati elettronici per molecole rigide e flessibili | 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. | 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. | 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. | fluorescenza, rigidità molecolare, rilassamento non radiativo, curve di energia potenziale, rilassamento radiativo" + "search_text": "Figura 33 | Stati elettronici per molecole rigide e flessibili | 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. | 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. | 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. | fluorescenza, rigidità molecolare, rilassamento non radiativo, curve di energia potenziale, rilassamento radiativo" }, { "id": "fig-034", @@ -3015,10 +3016,10 @@ "number": 35, "label": "Figura 35", "type": "diagram", - "title": "sistemi polimerici con inserimento di fluorofori, in verde il polimero e in rosso le unità di fluoroforo", + "title": "sistemi polimerici con inserimento di fluorofori, in verde il polimero e in rosso le unità di fluoroforo,", "caption": "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.", "alt_text": "Quattro schemi a)-d) di fluorofori in polimeri: dispersi, in catena principale, pendenti, reticolanti.", - "caption_printed": "Figura 35 - sistemi polimerici con inserimento di fluorofori, in verde il polimero e in rosso le unità di fluoroforo", + "caption_printed": "Figura 35 - sistemi polimerici con inserimento di fluorofori, in verde il polimero e in rosso le unità di fluoroforo,", "location": { "chapter": "1", "section": "1.3", @@ -3078,7 +3079,7 @@ ] } }, - "search_text": "Figura 35 | sistemi polimerici con inserimento di fluorofori, in verde il polimero e in rosso le unità di fluoroforo | 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. | 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). | polimeri fluorescenti, host-guest, matrice polimerica, fluoroforo in catena principale (main-chain), fluoroforo pendente (side-chain), fluoroforo come reticolante (cross-linked)" + "search_text": "Figura 35 | sistemi polimerici con inserimento di fluorofori, in verde il polimero e in rosso le unità di fluoroforo, | 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. | 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). | polimeri fluorescenti, host-guest, matrice polimerica, fluoroforo in catena principale (main-chain), fluoroforo pendente (side-chain), fluoroforo come reticolante (cross-linked)" }, { "id": "fig-036", @@ -3548,7 +3549,7 @@ "section": "3.2", "section_title": "Sintesi e procedure", "md_line": 648, - "caption_md_line": 661 + "caption_md_line": 658 }, "panels": [ { @@ -3626,8 +3627,8 @@ "chapter": "3", "section": "3.4", "section_title": "Procedure sperimentali delle analisi voltammetriche", - "md_line": 708, - "caption_md_line": 710 + "md_line": 705, + "caption_md_line": 707 }, "panels": [ { @@ -3635,7 +3636,7 @@ "file": "7454f0793d62db92121d98aa27815bc85d5aae9f16807d3f188d7feb1ee83463.jpg", "path": "immagini/7454f0793d62db92121d98aa27815bc85d5aae9f16807d3f188d7feb1ee83463.jpg", "embed": "![[immagini/7454f0793d62db92121d98aa27815bc85d5aae9f16807d3f188d7feb1ee83463.jpg]]", - "md_line": 708, + "md_line": 705, "width": 550, "height": 615, "description": "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.", @@ -3692,8 +3693,8 @@ "chapter": "4", "section": "4.1", "section_title": "Dichetopirrolopirroli", - "md_line": 726, - "caption_md_line": 728 + "md_line": 723, + "caption_md_line": 725 }, "panels": [ { @@ -3701,7 +3702,7 @@ "file": "b6398852c7419861eb44da7657cb2af96b59c5953a54007fb0df70f12a4c2cf9.jpg", "path": "immagini/b6398852c7419861eb44da7657cb2af96b59c5953a54007fb0df70f12a4c2cf9.jpg", "embed": "![[immagini/b6398852c7419861eb44da7657cb2af96b59c5953a54007fb0df70f12a4c2cf9.jpg]]", - "md_line": 726, + "md_line": 723, "width": 898, "height": 321, "description": "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.", @@ -3739,7 +3740,7 @@ ], "text_context": "EWG in para danno sistemi molto emissivi; EDG portano all'iso-DPP con fluorescenza inibita.", "cited_in_md_lines": [ - 724 + 721 ], "quality": { "confidence": "high", @@ -3765,8 +3766,8 @@ "chapter": "4", "section": "4.1", "section_title": "Dichetopirrolopirroli", - "md_line": 738, - "caption_md_line": 740 + "md_line": 735, + "caption_md_line": 737 }, "panels": [ { @@ -3774,7 +3775,7 @@ "file": "0238be4920f26782b3892465ff26009313f91823b3eaabb46aada5c489d49fd9.jpg", "path": "immagini/0238be4920f26782b3892465ff26009313f91823b3eaabb46aada5c489d49fd9.jpg", "embed": "![[immagini/0238be4920f26782b3892465ff26009313f91823b3eaabb46aada5c489d49fd9.jpg]]", - "md_line": 738, + "md_line": 735, "width": 1215, "height": 337, "description": "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.", @@ -3810,7 +3811,7 @@ ], "text_context": "Mostra la sintesi del fluoroforo 2 poi usato nelle polimerizzazioni.", "cited_in_md_lines": [ - 736 + 733 ], "quality": { "confidence": "high", @@ -3836,8 +3837,8 @@ "chapter": "4", "section": "4.1", "section_title": "Dichetopirrolopirroli", - "md_line": 744, - "caption_md_line": 746 + "md_line": 741, + "caption_md_line": 743 }, "panels": [ { @@ -3845,7 +3846,7 @@ "file": "b8095b77f46fe9daaa5430cabef072a05c35605430fd6ff6af09c38553a33d1c.jpg", "path": "immagini/b8095b77f46fe9daaa5430cabef072a05c35605430fd6ff6af09c38553a33d1c.jpg", "embed": "![[immagini/b8095b77f46fe9daaa5430cabef072a05c35605430fd6ff6af09c38553a33d1c.jpg]]", - "md_line": 744, + "md_line": 741, "width": 1134, "height": 600, "description": "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.", @@ -3882,7 +3883,7 @@ ], "text_context": "Il tiofene è introdotto dopo la formazione dell'alcolato, il succinato è gocciolato lentamente per evitare reazioni parassite.", "cited_in_md_lines": [ - 742 + 739 ], "quality": { "confidence": "high", @@ -3908,8 +3909,8 @@ "chapter": "4", "section": "4.1", "section_title": "Dichetopirrolopirroli", - "md_line": 750, - "caption_md_line": 752 + "md_line": 747, + "caption_md_line": 749 }, "panels": [ { @@ -3917,7 +3918,7 @@ "file": "9cb4d6705cae60dc0e20d74685b5217ff70680872a3714cd00103f3561ad251b.jpg", "path": "immagini/9cb4d6705cae60dc0e20d74685b5217ff70680872a3714cd00103f3561ad251b.jpg", "embed": "![[immagini/9cb4d6705cae60dc0e20d74685b5217ff70680872a3714cd00103f3561ad251b.jpg]]", - "md_line": 750, + "md_line": 747, "width": 1126, "height": 407, "description": "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).", @@ -3948,7 +3949,7 @@ ], "text_context": "Spiega la reazione parassita dovuta a eccessiva concentrazione locale di succinato in condizioni basiche.", "cited_in_md_lines": [ - 748 + 745 ], "quality": { "confidence": "high", @@ -3976,8 +3977,8 @@ "chapter": "4", "section": "4.1", "section_title": "Dichetopirrolopirroli", - "md_line": 758, - "caption_md_line": 760 + "md_line": 755, + "caption_md_line": 757 }, "panels": [ { @@ -3985,7 +3986,7 @@ "file": "5b9c36eb3db1dae7d33d24a159eb75cd575f40a33dad1110ef83da17bffaa3d9.jpg", "path": "immagini/5b9c36eb3db1dae7d33d24a159eb75cd575f40a33dad1110ef83da17bffaa3d9.jpg", "embed": "![[immagini/5b9c36eb3db1dae7d33d24a159eb75cd575f40a33dad1110ef83da17bffaa3d9.jpg]]", - "md_line": 758, + "md_line": 755, "width": 1223, "height": 829, "description": "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.", @@ -4031,7 +4032,7 @@ ], "text_context": "La simmetria rende equivalenti diversi protoni, riducendo il numero di segnali rispetto agli idrogeni totali.", "cited_in_md_lines": [ - 762 + 759 ], "quality": { "confidence": "medium", @@ -4051,16 +4052,16 @@ "number": 45, "label": "Figura 45", "type": "spectrum_uv_vis", - "title": "spettro UV-Visibile e di emissione del prodotto 1 in THF", + "title": "spettro UV-Visibile e di emissione del prodotto 1 in THF (λex:490 nm)", "caption": "Spettro di assorbimento UV-Visibile (linea continua) e di emissione (tratteggiata) normalizzati del prodotto 1 (DPP di partenza) in THF.", "alt_text": "Spettro di assorbimento UV-Visibile (linea continua) e di emissione (tratteggiata) normalizzati del prodotto 1 (DPP di partenza) in THF.", - "caption_printed": "Figura 45 - spettro UV-Visibile e di emissione del prodotto 1 in THF", + "caption_printed": "Figura 45 - spettro UV-Visibile e di emissione del prodotto 1 in THF (λex:490 nm)", "location": { "chapter": "4", "section": "4.1", "section_title": "Dichetopirrolopirroli", - "md_line": 766, - "caption_md_line": 768 + "md_line": 763, + "caption_md_line": 765 }, "panels": [ { @@ -4068,7 +4069,7 @@ "file": "ba9fb099eb33d86ffd10e40efffc19c6100dc56af328b2442f186b51e09433be.jpg", "path": "immagini/ba9fb099eb33d86ffd10e40efffc19c6100dc56af328b2442f186b51e09433be.jpg", "embed": "![[immagini/ba9fb099eb33d86ffd10e40efffc19c6100dc56af328b2442f186b51e09433be.jpg]]", - "md_line": 766, + "md_line": 763, "width": 1162, "height": 706, "description": "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.", @@ -4120,7 +4121,7 @@ "issues": [] } }, - "search_text": "Figura 45 | spettro UV-Visibile e di emissione del prodotto 1 in THF | Spettro di assorbimento UV-Visibile (linea continua) e di emissione (tratteggiata) normalizzati del prodotto 1 (DPP di partenza) in THF. | 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. | composti: 1 | UV-Vis, fluorescenza, emissione, DPP, THF, spettro normalizzato" + "search_text": "Figura 45 | spettro UV-Visibile e di emissione del prodotto 1 in THF (λex:490 nm) | Spettro di assorbimento UV-Visibile (linea continua) e di emissione (tratteggiata) normalizzati del prodotto 1 (DPP di partenza) in THF. | 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. | composti: 1 | UV-Vis, fluorescenza, emissione, DPP, THF, spettro normalizzato" }, { "id": "fig-046", @@ -4135,8 +4136,8 @@ "chapter": "4", "section": "4.1", "section_title": "Dichetopirrolopirroli", - "md_line": 778, - "caption_md_line": 780 + "md_line": 775, + "caption_md_line": 777 }, "panels": [ { @@ -4144,7 +4145,7 @@ "file": "9b67a0c4119927bb79c04800ab73ca66e034387467484976be81ef31499a5cfb.jpg", "path": "immagini/9b67a0c4119927bb79c04800ab73ca66e034387467484976be81ef31499a5cfb.jpg", "embed": "![[immagini/9b67a0c4119927bb79c04800ab73ca66e034387467484976be81ef31499a5cfb.jpg]]", - "md_line": 778, + "md_line": 775, "width": 1034, "height": 281, "description": "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.", @@ -4186,7 +4187,7 @@ ], "text_context": "Il testo spiega che l'azoto ammidico, deprotonato da t-BuOK, attacca il carbonio adiacente al bromo.", "cited_in_md_lines": [ - 776 + 773 ], "quality": { "confidence": "high", @@ -4214,8 +4215,8 @@ "chapter": "4", "section": "4.1", "section_title": "Dichetopirrolopirroli", - "md_line": 784, - "caption_md_line": 786 + "md_line": 781, + "caption_md_line": 783 }, "panels": [ { @@ -4223,7 +4224,7 @@ "file": "de181218223f66cd046706d8723e5010aa9d7a8779b172c877562b47a100738d.jpg", "path": "immagini/de181218223f66cd046706d8723e5010aa9d7a8779b172c877562b47a100738d.jpg", "embed": "![[immagini/de181218223f66cd046706d8723e5010aa9d7a8779b172c877562b47a100738d.jpg]]", - "md_line": 784, + "md_line": 781, "width": 1081, "height": 134, "description": "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).", @@ -4258,7 +4259,7 @@ ], "text_context": "Il testo avverte che un eccesso di base favorisce la ciclizzazione indesiderata del 6-bromo-1-esanolo.", "cited_in_md_lines": [ - 782 + 779 ], "quality": { "confidence": "high", @@ -4286,8 +4287,8 @@ "chapter": "4", "section": "4.1", "section_title": "Dichetopirrolopirroli", - "md_line": 792, - "caption_md_line": 794 + "md_line": 789, + "caption_md_line": 791 }, "panels": [ { @@ -4295,7 +4296,7 @@ "file": "d22ce85e035853dee124b1608b0cb176c370dc95ec3ab560926836261887394e.jpg", "path": "immagini/d22ce85e035853dee124b1608b0cb176c370dc95ec3ab560926836261887394e.jpg", "embed": "![[immagini/d22ce85e035853dee124b1608b0cb176c370dc95ec3ab560926836261887394e.jpg]]", - "md_line": 792, + "md_line": 789, "width": 1240, "height": 865, "description": "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.", @@ -4341,7 +4342,7 @@ ], "text_context": "Il testo commenta la regione aromatica con tre segnali dei protoni tiofenici e il doppietto a circa 8.9 ppm.", "cited_in_md_lines": [ - 796 + 793 ], "quality": { "confidence": "high", @@ -4367,8 +4368,8 @@ "chapter": "4", "section": "4.1", "section_title": "Dichetopirrolopirroli", - "md_line": 798, - "caption_md_line": 800 + "md_line": 795, + "caption_md_line": 797 }, "panels": [ { @@ -4376,7 +4377,7 @@ "file": "f890cc2c6264ef44ec1b471578277dc04114da1baa30e1f6aa17bb7f674615e8.jpg", "path": "immagini/f890cc2c6264ef44ec1b471578277dc04114da1baa30e1f6aa17bb7f674615e8.jpg", "embed": "![[immagini/f890cc2c6264ef44ec1b471578277dc04114da1baa30e1f6aa17bb7f674615e8.jpg]]", - "md_line": 798, + "md_line": 795, "width": 1256, "height": 862, "description": "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.", @@ -4426,7 +4427,7 @@ ], "text_context": "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.", "cited_in_md_lines": [ - 802 + 799 ], "quality": { "confidence": "high", @@ -4446,16 +4447,16 @@ "number": 50, "label": "Figura 50", "type": "spectrum_uv_vis", - "title": "spettro UV-Visibile e di emissione del prodotto2 in THF", + "title": "spettro UV-Visibile e di emissione del prodotto2 in THF (λex:540 nm)", "caption": "Spettro UV-Visibile e di emissione normalizzati del prodotto 2 in THF.", "alt_text": "Spettro UV-Visibile e di emissione normalizzati del prodotto 2 in THF.", - "caption_printed": "Figura 50 - spettro UV-Visibile e di emissione del prodotto2 in THF", + "caption_printed": "Figura 50 - spettro UV-Visibile e di emissione del prodotto2 in THF (λex:540 nm)", "location": { "chapter": "4", "section": "4.1", "section_title": "Dichetopirrolopirroli", - "md_line": 806, - "caption_md_line": 808 + "md_line": 803, + "caption_md_line": 805 }, "panels": [ { @@ -4463,7 +4464,7 @@ "file": "75c7d0cf12baae0fe259352e5495ea053607717f5a57233f468098343f6693c7.jpg", "path": "immagini/75c7d0cf12baae0fe259352e5495ea053607717f5a57233f468098343f6693c7.jpg", "embed": "![[immagini/75c7d0cf12baae0fe259352e5495ea053607717f5a57233f468098343f6693c7.jpg]]", - "md_line": 806, + "md_line": 803, "width": 1190, "height": 707, "description": "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.", @@ -4502,7 +4503,7 @@ ], "text_context": "Il testo confronta il prodotto 2 con il 1, riportando spostamento batocromico del massimo da 531 a 541 nm dopo alchilazione.", "cited_in_md_lines": [ - 804 + 801 ], "quality": { "confidence": "high", @@ -4513,23 +4514,23 @@ "issues": [] } }, - "search_text": "Figura 50 | spettro UV-Visibile e di emissione del prodotto2 in THF | Spettro UV-Visibile e di emissione normalizzati del prodotto 2 in THF. | 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. | composti: 2 | UV-Vis, fluorescenza, spostamento batocromico, DPP alchilato, THF" + "search_text": "Figura 50 | spettro UV-Visibile e di emissione del prodotto2 in THF (λex:540 nm) | Spettro UV-Visibile e di emissione normalizzati del prodotto 2 in THF. | 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. | composti: 2 | UV-Vis, fluorescenza, spostamento batocromico, DPP alchilato, THF" }, { "id": "fig-051", "number": 51, "label": "Figura 51", "type": "plot", - "title": "retta di calibrazione del fluoroforo 2 per il calcolo di ε", + "title": "retta di calibrazione del fluoroforo 2 in CHCl3 per il calcolo di ε", "caption": "Retta di calibrazione assorbanza-concentrazione del fluoroforo 2 per il calcolo del coefficiente di estinzione molare ε.", "alt_text": "Retta di calibrazione assorbanza-concentrazione del fluoroforo 2 per il calcolo del coefficiente di estinzione molare ε.", - "caption_printed": "Figura 51 - retta di calibrazione del fluoroforo 2 per il calcolo di ε", + "caption_printed": "Figura 51 - retta di calibrazione del fluoroforo 2 in CHCl3 per il calcolo di ε", "location": { "chapter": "4", "section": "4.1", "section_title": "Dichetopirrolopirroli", - "md_line": 821, - "caption_md_line": 823 + "md_line": 818, + "caption_md_line": 820 }, "panels": [ { @@ -4537,7 +4538,7 @@ "file": "336837d03a78ea923cf3fa1ae976385b52eefe8ab91dccfdff63f3bb33ecfc6b.jpg", "path": "immagini/336837d03a78ea923cf3fa1ae976385b52eefe8ab91dccfdff63f3bb33ecfc6b.jpg", "embed": "![[immagini/336837d03a78ea923cf3fa1ae976385b52eefe8ab91dccfdff63f3bb33ecfc6b.jpg]]", - "md_line": 821, + "md_line": 818, "width": 901, "height": 559, "description": "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.", @@ -4574,7 +4575,7 @@ ], "text_context": "Il testo spiega che ε è calcolato dalla pendenza della retta ottenuta con soluzioni di concentrazione nota in CHCl3.", "cited_in_md_lines": [ - 819 + 816 ], "quality": { "confidence": "high", @@ -4585,23 +4586,109 @@ "issues": [] } }, - "search_text": "Figura 51 | retta di calibrazione del fluoroforo 2 per il calcolo di ε | Retta di calibrazione assorbanza-concentrazione del fluoroforo 2 per il calcolo del coefficiente di estinzione molare ε. | 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. | composti: 2 | legge di Lambert-Beer, calibrazione, coefficiente di estinzione molare, CHCl3" + "search_text": "Figura 51 | retta di calibrazione del fluoroforo 2 in CHCl3 per il calcolo di ε | Retta di calibrazione assorbanza-concentrazione del fluoroforo 2 per il calcolo del coefficiente di estinzione molare ε. | 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. | composti: 2 | legge di Lambert-Beer, calibrazione, coefficiente di estinzione molare, CHCl3" }, { "id": "fig-052", "number": 52, "label": "Figura 52", + "type": "cv_voltammogram", + "title": "voltammogramma ciclico del prodotto 2 in soluzione di THF", + "caption": "Voltammogramma ciclico del prodotto 2 in THF: onda anodica ampia e irreversibile verso +0,8 V, picco di riduzione catodico definito a circa -1,6 V con picco di ritorno.", + "alt_text": "Voltammogramma ciclico del prodotto 2 in THF: onda anodica ampia e irreversibile verso +0,8 V, picco di riduzione catodico definito a circa -1,6 V con picco di ritorno.", + "caption_printed": "Figura 52 - voltammogramma ciclico del prodotto 2 in soluzione di THF", + "location": { + "chapter": "4", + "section": "4.1", + "section_title": "Dichetopirrolopirroli", + "md_line": 828, + "caption_md_line": 830 + }, + "panels": [ + { + "panel": null, + "file": "c43b5f5dac544853f6c17aff18ad43408c4b39ab24ba521cc098fbda40f50699.jpg", + "path": "immagini/c43b5f5dac544853f6c17aff18ad43408c4b39ab24ba521cc098fbda40f50699.jpg", + "embed": "![[immagini/c43b5f5dac544853f6c17aff18ad43408c4b39ab24ba521cc098fbda40f50699.jpg]]", + "md_line": 828, + "width": 647, + "height": 407, + "description": "Curva blu corrente (A, da -2E-03 a 3E-03) vs potenziale (V, da -2 a 1). Verso potenziali positivi la corrente cresce rapidamente oltre circa +0,5 V fino a circa 2,5E-03 A a circa +0,83 V, senza picco di ritorno simmetrico. Verso potenziali negativi: picco di riduzione intorno a -1,6 V (circa -1,1E-03 A), picco di ritorno intorno a -1,45 V (circa 2E-04 A), piccola pre-onda intorno a -0,65 V.", + "visible_text": [ + "Corrente (A)", + "Potenziale (V)", + "3E-03", + "2E-03", + "2E-03", + "1E-03", + "5E-04", + "0E+00", + "-5E-04", + "-1E-03", + "-2E-03", + "-2", + "-1,5", + "-1", + "-0,5", + "0", + "0,5", + "1" + ], + "quality_flags": [], + "confidence": "medium" + } + ], + "compounds": [ + "2" + ], + "keywords": [ + "ciclovoltammetria", + "irreversibilità", + "meccanismo EC", + "drogaggio di tipo p", + "drogaggio di tipo n", + "THF" + ], + "concepts": [ + "ciclovoltammetria", + "irreversibilita", + "meccanismo-ec", + "drogaggio-di-tipo-p", + "drogaggio-di-tipo-n", + "thf" + ], + "text_context": "Il testo descrive l'ossidazione irreversibile (meccanismo EC) e la riduzione con picco di ritorno del monomero 2.", + "cited_in_md_lines": [ + 824 + ], + "quality": { + "confidence": "medium", + "flags": [], + "review_notes": "Voce aggiunta dopo la nuova versione della tesi (tesi_new.docx, dove la figura è un grafico Word nativo); descrizione e valori letti dall'immagine, non verificati.", + "verification": { + "verdict": "n/d", + "issues": [ + "non revisionata" + ] + } + }, + "search_text": "Figura 52 | voltammogramma ciclico del prodotto 2 in soluzione di THF | Voltammogramma ciclico del prodotto 2 in THF: onda anodica ampia e irreversibile verso +0,8 V, picco di riduzione catodico definito a circa -1,6 V con picco di ritorno. | Curva blu corrente (A, da -2E-03 a 3E-03) vs potenziale (V, da -2 a 1). Verso potenziali positivi la corrente cresce rapidamente oltre circa +0,5 V fino a circa 2,5E-03 A a circa +0,83 V, senza picco di ritorno simmetrico. Verso potenziali negativi: picco di riduzione intorno a -1,6 V (circa -1,1E-03 A), picco di ritorno intorno a -1,45 V (circa 2E-04 A), piccola pre-onda intorno a -0,65 V. | composti: 2 | ciclovoltammetria, irreversibilità, meccanismo EC, drogaggio di tipo p, drogaggio di tipo n, THF" + }, + { + "id": "fig-053", + "number": 53, + "label": "Figura 53", "type": "reaction_scheme", "title": "schema di reazione dei copolimeri coniugati", "caption": "Schema di reazione di polimerizzazione ossidativa del fluoroforo 2 con 3-esiltiofene (3HT) con FeCl3 catalitico, che porta al copolimero 3.", "alt_text": "Schema di reazione di polimerizzazione ossidativa del fluoroforo 2 con 3-esiltiofene (3HT) con FeCl3 catalitico, che porta al copolimero 3.", - "caption_printed": "Figura 52 - schema di reazione dei copolimeri coniugati", + "caption_printed": "Figura 53 - schema di reazione dei copolimeri coniugati", "location": { "chapter": "4", "section": "4.2", "section_title": "Copolimeri coniugati", - "md_line": 836, - "caption_md_line": 838 + "md_line": 851, + "caption_md_line": 853 }, "panels": [ { @@ -4609,7 +4696,7 @@ "file": "0cc72ddb7b8a730785dfaeb2abb381f6ef486e86e068d50b5d0b0ac0e8bc220d.jpg", "path": "immagini/0cc72ddb7b8a730785dfaeb2abb381f6ef486e86e068d50b5d0b0ac0e8bc220d.jpg", "embed": "![[immagini/0cc72ddb7b8a730785dfaeb2abb381f6ef486e86e068d50b5d0b0ac0e8bc220d.jpg]]", - "md_line": 836, + "md_line": 851, "width": 1226, "height": 248, "description": "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.", @@ -4654,7 +4741,7 @@ ], "text_context": "Il testo introduce la polimerizzazione ossidativa del fluoroforo 2 con 3HT secondo lo schema di Figura 52.", "cited_in_md_lines": [ - 834 + 849 ], "quality": { "confidence": "high", @@ -4665,23 +4752,23 @@ "issues": [] } }, - "search_text": "Figura 52 | schema di reazione dei copolimeri coniugati | Schema di reazione di polimerizzazione ossidativa del fluoroforo 2 con 3-esiltiofene (3HT) con FeCl3 catalitico, che porta al copolimero 3. | 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. | composti: 2, 3, 3HT | polimerizzazione ossidativa, FeCl3, 3-esiltiofene, copolimero, DPP, nitrometano" + "search_text": "Figura 53 | schema di reazione dei copolimeri coniugati | Schema di reazione di polimerizzazione ossidativa del fluoroforo 2 con 3-esiltiofene (3HT) con FeCl3 catalitico, che porta al copolimero 3. | 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. | composti: 2, 3, 3HT | polimerizzazione ossidativa, FeCl3, 3-esiltiofene, copolimero, DPP, nitrometano" }, { - "id": "fig-053", - "number": 53, - "label": "Figura 53", + "id": "fig-054", + "number": 54, + "label": "Figura 54", "type": "mechanism", "title": "meccanismo di polimerizzazione ossidativa mediante tricloruro ferrico", "caption": "Meccanismo di polimerizzazione ossidativa mediante FeCl3: ossidazione del DPP-tiofene a radicale, attacco del 3-esiltiofene e propagazione al copolimero 3.", "alt_text": "Meccanismo di polimerizzazione ossidativa mediante FeCl3: ossidazione del DPP-tiofene a radicale, attacco del 3-esiltiofene e propagazione al copolimero 3.", - "caption_printed": "Figura 53 - meccanismo di polimerizzazione ossidativa mediante tricloruro ferrico", + "caption_printed": "Figura 54 - meccanismo di polimerizzazione ossidativa mediante tricloruro ferrico", "location": { "chapter": "4", "section": "4.2", "section_title": "Copolimeri coniugati", - "md_line": 842, - "caption_md_line": 844 + "md_line": 857, + "caption_md_line": 859 }, "panels": [ { @@ -4689,7 +4776,7 @@ "file": "34cdcf9d6836a55ee2dd35ac99f5e80cd9dffb87cbfaf818b5257c5ccfed2b51.jpg", "path": "immagini/34cdcf9d6836a55ee2dd35ac99f5e80cd9dffb87cbfaf818b5257c5ccfed2b51.jpg", "embed": "![[immagini/34cdcf9d6836a55ee2dd35ac99f5e80cd9dffb87cbfaf818b5257c5ccfed2b51.jpg]]", - "md_line": 842, + "md_line": 857, "width": 1256, "height": 312, "description": "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.", @@ -4729,7 +4816,7 @@ ], "text_context": "Il testo descrive il primo stadio governato dalla reattività di FeCl3 come ossidante in eccesso e il ruolo del nitrometano.", "cited_in_md_lines": [ - 840 + 855 ], "quality": { "confidence": "high", @@ -4742,23 +4829,23 @@ ] } }, - "search_text": "Figura 53 | meccanismo di polimerizzazione ossidativa mediante tricloruro ferrico | Meccanismo di polimerizzazione ossidativa mediante FeCl3: ossidazione del DPP-tiofene a radicale, attacco del 3-esiltiofene e propagazione al copolimero 3. | 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. | composti: 2, 3, 3HT | polimerizzazione ossidativa, FeCl3, radicale, accoppiamento ossidativo, 3-esiltiofene" + "search_text": "Figura 54 | meccanismo di polimerizzazione ossidativa mediante tricloruro ferrico | Meccanismo di polimerizzazione ossidativa mediante FeCl3: ossidazione del DPP-tiofene a radicale, attacco del 3-esiltiofene e propagazione al copolimero 3. | 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. | composti: 2, 3, 3HT | polimerizzazione ossidativa, FeCl3, radicale, accoppiamento ossidativo, 3-esiltiofene" }, { - "id": "fig-054", - "number": 54, - "label": "Figura 54", + "id": "fig-055", + "number": 55, + "label": "Figura 55", "type": "spectrum_nmr", - "title": "spettro 1H-NMR del copolimero 3a in CDCl3", + "title": "Spettro 1H-NMR del copolimero 3a in CDCl3", "caption": "Spettro 1H-NMR del copolimero 3a in CDCl3, con integrali usati per stimare la composizione DPP/3HT.", "alt_text": "Spettro 1H-NMR del copolimero 3a in CDCl3, con integrali usati per stimare la composizione DPP/3HT.", - "caption_printed": "Figura 54 - spettro 1H-NMR del copolimero 3a in CDCl3", + "caption_printed": "Figura 55 - Spettro 1H-NMR del copolimero 3a in CDCl3", "location": { "chapter": "4", "section": "4.2", "section_title": "Copolimeri coniugati", - "md_line": 886, - "caption_md_line": 888 + "md_line": 903, + "caption_md_line": 905 }, "panels": [ { @@ -4766,7 +4853,7 @@ "file": "a182a55cad5ef042b39852288ff9f6ae3b5f9c0fd758fd0815f0366e77b09a8e.jpg", "path": "immagini/a182a55cad5ef042b39852288ff9f6ae3b5f9c0fd758fd0815f0366e77b09a8e.jpg", "embed": "![[immagini/a182a55cad5ef042b39852288ff9f6ae3b5f9c0fd758fd0815f0366e77b09a8e.jpg]]", - "md_line": 886, + "md_line": 903, "width": 1073, "height": 851, "description": "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.", @@ -4811,7 +4898,7 @@ ], "text_context": "Il testo spiega il calcolo della percentuale reale di DPP dai rapporti di aree integrate; i risultati sono in Tabella 6.", "cited_in_md_lines": [ - 872 + 887 ], "quality": { "confidence": "high", @@ -4822,23 +4909,23 @@ "issues": [] } }, - "search_text": "Figura 54 | spettro 1H-NMR del copolimero 3a in CDCl3 | Spettro 1H-NMR del copolimero 3a in CDCl3, con integrali usati per stimare la composizione DPP/3HT. | 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. | composti: 3a | 1H-NMR, CDCl3, composizione copolimero, integrazione, 3HT, DPP" + "search_text": "Figura 55 | Spettro 1H-NMR del copolimero 3a in CDCl3 | Spettro 1H-NMR del copolimero 3a in CDCl3, con integrali usati per stimare la composizione DPP/3HT. | 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. | composti: 3a | 1H-NMR, CDCl3, composizione copolimero, integrazione, 3HT, DPP" }, { - "id": "fig-055", - "number": 55, - "label": "Figura 55", + "id": "fig-056", + "number": 56, + "label": "Figura 56", "type": "spectrum_nmr", - "title": "spettro 1H-NMR del copolimero 3b in CDCl3", + "title": "Spettro 1H-NMR del copolimero 3b in CDCl3", "caption": "Spettro 1H-NMR del copolimero 3b in CDCl3, con integrali per il calcolo della composizione.", "alt_text": "Spettro 1H-NMR del copolimero 3b in CDCl3, con integrali per il calcolo della composizione.", - "caption_printed": "Figura 55 - spettro 1H-NMR del copolimero 3b in CDCl3", + "caption_printed": "Figura 56 - Spettro 1H-NMR del copolimero 3b in CDCl3", "location": { "chapter": "4", "section": "4.2", "section_title": "Copolimeri coniugati", - "md_line": 890, - "caption_md_line": 892 + "md_line": 907, + "caption_md_line": 909 }, "panels": [ { @@ -4846,7 +4933,7 @@ "file": "5ab89fc3cc83f82abb39c0bfd40b1f0da53a8f88a4ca771e00621a476cf8901d.jpg", "path": "immagini/5ab89fc3cc83f82abb39c0bfd40b1f0da53a8f88a4ca771e00621a476cf8901d.jpg", "embed": "![[immagini/5ab89fc3cc83f82abb39c0bfd40b1f0da53a8f88a4ca771e00621a476cf8901d.jpg]]", - "md_line": 890, + "md_line": 907, "width": 1121, "height": 837, "description": "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.", @@ -4887,7 +4974,7 @@ ], "text_context": "Il testo riporta gli spettri NMR dei tre copolimeri per determinare la percentuale reale di DPP.", "cited_in_md_lines": [ - 872 + 887 ], "quality": { "confidence": "high", @@ -4898,23 +4985,23 @@ "issues": [] } }, - "search_text": "Figura 55 | spettro 1H-NMR del copolimero 3b in CDCl3 | Spettro 1H-NMR del copolimero 3b in CDCl3, con integrali per il calcolo della composizione. | 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. | composti: 3b | 1H-NMR, CDCl3, composizione copolimero, integrazione" + "search_text": "Figura 56 | Spettro 1H-NMR del copolimero 3b in CDCl3 | Spettro 1H-NMR del copolimero 3b in CDCl3, con integrali per il calcolo della composizione. | 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. | composti: 3b | 1H-NMR, CDCl3, composizione copolimero, integrazione" }, { - "id": "fig-056", - "number": 56, - "label": "Figura 56", + "id": "fig-057", + "number": 57, + "label": "Figura 57", "type": "spectrum_nmr", - "title": "spettro 1H-NMR del copolimero 3c in CDCl3", + "title": "Spettro 1H-NMR del copolimero 3c in CDCl3", "caption": "Spettro 1H-NMR del copolimero 3c in CDCl3, con integrali per il calcolo della composizione.", "alt_text": "Spettro 1H-NMR del copolimero 3c in CDCl3, con integrali per il calcolo della composizione.", - "caption_printed": "Figura 56 - spettro 1H-NMR del copolimero 3c in CDCl3", + "caption_printed": "Figura 57 - Spettro 1H-NMR del copolimero 3c in CDCl3", "location": { "chapter": "4", "section": "4.2", "section_title": "Copolimeri coniugati", - "md_line": 894, - "caption_md_line": 896 + "md_line": 911, + "caption_md_line": 913 }, "panels": [ { @@ -4922,7 +5009,7 @@ "file": "f078dd5e0992c244123ad8fcbd08d2f2235bffb15f21adcee16bef8ed40a1f4e.jpg", "path": "immagini/f078dd5e0992c244123ad8fcbd08d2f2235bffb15f21adcee16bef8ed40a1f4e.jpg", "embed": "![[immagini/f078dd5e0992c244123ad8fcbd08d2f2235bffb15f21adcee16bef8ed40a1f4e.jpg]]", - "md_line": 894, + "md_line": 911, "width": 1090, "height": 809, "description": "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).", @@ -4963,7 +5050,7 @@ ], "text_context": "Ultimo dei tre spettri NMR dei copolimeri; il testo successivo passa a FT-IR, UV-Vis, GPC e DSC.", "cited_in_md_lines": [ - 872 + 887 ], "quality": { "confidence": "high", @@ -4974,23 +5061,23 @@ "issues": [] } }, - "search_text": "Figura 56 | spettro 1H-NMR del copolimero 3c in CDCl3 | Spettro 1H-NMR del copolimero 3c in CDCl3, con integrali per il calcolo della composizione. | 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). | composti: 3c | 1H-NMR, CDCl3, composizione copolimero, integrazione" + "search_text": "Figura 57 | Spettro 1H-NMR del copolimero 3c in CDCl3 | Spettro 1H-NMR del copolimero 3c in CDCl3, con integrali per il calcolo della composizione. | 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). | composti: 3c | 1H-NMR, CDCl3, composizione copolimero, integrazione" }, { - "id": "fig-057", - "number": 57, - "label": "Figura 57", + "id": "fig-058", + "number": 58, + "label": "Figura 58", "type": "spectrum_ir", "title": "spettro FT-IR dei copolimeri 3a (blu), 3b (verde), 3c (rosso)", "caption": "Spettri FT-IR sovrapposti dei copolimeri 3a, 3b e 3c.", "alt_text": "Spettri FT-IR sovrapposti dei copolimeri 3a, 3b e 3c.", - "caption_printed": "Figura 57 - spettro FT-IR dei copolimeri 3a (blu), 3b (verde), 3c (rosso)", + "caption_printed": "Figura 58 - spettro FT-IR dei copolimeri 3a (blu), 3b (verde), 3c (rosso)", "location": { "chapter": "4", "section": "4.2", "section_title": "Copolimeri coniugati", - "md_line": 900, - "caption_md_line": 902 + "md_line": 917, + "caption_md_line": 919 }, "panels": [ { @@ -4998,7 +5085,7 @@ "file": "4b81d4490846b8b0f24cd7ae9e1ed776036c588345475c519334bef4eb76a684.jpg", "path": "immagini/4b81d4490846b8b0f24cd7ae9e1ed776036c588345475c519334bef4eb76a684.jpg", "embed": "![[immagini/4b81d4490846b8b0f24cd7ae9e1ed776036c588345475c519334bef4eb76a684.jpg]]", - "md_line": 900, + "md_line": 917, "width": 1229, "height": 848, "description": "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).", @@ -5051,7 +5138,7 @@ ], "text_context": "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.", "cited_in_md_lines": [ - 904 + 921 ], "quality": { "confidence": "medium", @@ -5068,23 +5155,23 @@ ] } }, - "search_text": "Figura 57 | spettro FT-IR dei copolimeri 3a (blu), 3b (verde), 3c (rosso) | Spettri FT-IR sovrapposti dei copolimeri 3a, 3b e 3c. | 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). | composti: 3a, 3b, 3c | FT-IR, copolimeri, C-H alifatici, 3-esiltiofene, C=O" + "search_text": "Figura 58 | spettro FT-IR dei copolimeri 3a (blu), 3b (verde), 3c (rosso) | Spettri FT-IR sovrapposti dei copolimeri 3a, 3b e 3c. | 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). | composti: 3a, 3b, 3c | FT-IR, copolimeri, C-H alifatici, 3-esiltiofene, C=O" }, { - "id": "fig-058", - "number": 58, - "label": "Figura 58", + "id": "fig-059", + "number": 59, + "label": "Figura 59", "type": "spectrum_uv_vis", "title": "spettro UV-Visibile e di emissione del copolimero 3a in THF", "caption": "Spettro UV-Visibile e di emissione normalizzati del copolimero 3a in THF.", "alt_text": "Spettro UV-Visibile e di emissione normalizzati del copolimero 3a in THF.", - "caption_printed": "Figura 58 - spettro UV-Visibile e di emissione del copolimero 3a in THF", + "caption_printed": "Figura 59 - spettro UV-Visibile e di emissione del copolimero 3a in THF", "location": { "chapter": "4", "section": "4.2", "section_title": "Copolimeri coniugati", - "md_line": 908, - "caption_md_line": 910 + "md_line": 925, + "caption_md_line": 927 }, "panels": [ { @@ -5092,7 +5179,7 @@ "file": "585dc7627f409d974b2dda6d2db2fc8d1febafb609faba20d707f941b23f851c.jpg", "path": "immagini/585dc7627f409d974b2dda6d2db2fc8d1febafb609faba20d707f941b23f851c.jpg", "embed": "![[immagini/585dc7627f409d974b2dda6d2db2fc8d1febafb609faba20d707f941b23f851c.jpg]]", - "md_line": 908, + "md_line": 925, "width": 1193, "height": 693, "description": "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.", @@ -5131,8 +5218,8 @@ ], "text_context": "Il testo afferma che i tre copolimeri hanno profili quasi identici, con λmax 540-545 nm.", "cited_in_md_lines": [ - 906, - 920 + 923, + 937 ], "quality": { "confidence": "high", @@ -5143,23 +5230,23 @@ "issues": [] } }, - "search_text": "Figura 58 | spettro UV-Visibile e di emissione del copolimero 3a in THF | Spettro UV-Visibile e di emissione normalizzati del copolimero 3a in THF. | 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. | composti: 3a | UV-Vis, fluorescenza, copolimero, THF" + "search_text": "Figura 59 | spettro UV-Visibile e di emissione del copolimero 3a in THF | Spettro UV-Visibile e di emissione normalizzati del copolimero 3a in THF. | 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. | composti: 3a | UV-Vis, fluorescenza, copolimero, THF" }, { - "id": "fig-059", - "number": 59, - "label": "Figura 59", + "id": "fig-060", + "number": 60, + "label": "Figura 60", "type": "spectrum_uv_vis", "title": "spettro UV-Visibile e di emissione del copolimero 3b in THF", "caption": "Spettro UV-Visibile e di emissione normalizzati del copolimero 3b in THF.", "alt_text": "Spettro UV-Visibile e di emissione normalizzati del copolimero 3b in THF.", - "caption_printed": "Figura 59 - spettro UV-Visibile e di emissione del copolimero 3b in THF", + "caption_printed": "Figura 60 - spettro UV-Visibile e di emissione del copolimero 3b in THF", "location": { "chapter": "4", "section": "4.2", "section_title": "Copolimeri coniugati", - "md_line": 912, - "caption_md_line": 914 + "md_line": 929, + "caption_md_line": 931 }, "panels": [ { @@ -5167,7 +5254,7 @@ "file": "f8b0852a6a485472cb2438e024374bb56e26d87d86831f40903fd0be201d0771.jpg", "path": "immagini/f8b0852a6a485472cb2438e024374bb56e26d87d86831f40903fd0be201d0771.jpg", "embed": "![[immagini/f8b0852a6a485472cb2438e024374bb56e26d87d86831f40903fd0be201d0771.jpg]]", - "md_line": 912, + "md_line": 929, "width": 1196, "height": 831, "description": "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.", @@ -5206,8 +5293,8 @@ ], "text_context": "Insieme a Figure 58 e 60 mostra profili fotofisici simili al DPP di partenza.", "cited_in_md_lines": [ - 906, - 920 + 923, + 937 ], "quality": { "confidence": "high", @@ -5218,23 +5305,23 @@ "issues": [] } }, - "search_text": "Figura 59 | spettro UV-Visibile e di emissione del copolimero 3b in THF | Spettro UV-Visibile e di emissione normalizzati del copolimero 3b in THF. | 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. | composti: 3b | UV-Vis, fluorescenza, copolimero, THF" + "search_text": "Figura 60 | spettro UV-Visibile e di emissione del copolimero 3b in THF | Spettro UV-Visibile e di emissione normalizzati del copolimero 3b in THF. | 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. | composti: 3b | UV-Vis, fluorescenza, copolimero, THF" }, { - "id": "fig-060", - "number": 60, - "label": "Figura 60", + "id": "fig-061", + "number": 61, + "label": "Figura 61", "type": "spectrum_uv_vis", "title": "spettro UV-Visibile e di emissione del copolimero 3c in THF", "caption": "Spettro UV-Visibile e di emissione normalizzati del copolimero 3c in THF.", "alt_text": "Spettro UV-Visibile e di emissione normalizzati del copolimero 3c in THF.", - "caption_printed": "Figura 60 - spettro UV-Visibile e di emissione del copolimero 3c in THF", + "caption_printed": "Figura 61 - spettro UV-Visibile e di emissione del copolimero 3c in THF", "location": { "chapter": "4", "section": "4.2", "section_title": "Copolimeri coniugati", - "md_line": 916, - "caption_md_line": 918 + "md_line": 933, + "caption_md_line": 935 }, "panels": [ { @@ -5242,7 +5329,7 @@ "file": "2b34f5439b53ddcf7aeff01949aba8f61aa554f29849c81d7c3922f06dd3bba9.jpg", "path": "immagini/2b34f5439b53ddcf7aeff01949aba8f61aa554f29849c81d7c3922f06dd3bba9.jpg", "embed": "![[immagini/2b34f5439b53ddcf7aeff01949aba8f61aa554f29849c81d7c3922f06dd3bba9.jpg]]", - "md_line": 916, + "md_line": 933, "width": 1196, "height": 837, "description": "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.", @@ -5281,8 +5368,8 @@ ], "text_context": "Il testo osserva che 3a, 3b e 3c in THF mostrano profili quasi identici con λmax 540-545 nm.", "cited_in_md_lines": [ - 906, - 920 + 923, + 937 ], "quality": { "confidence": "high", @@ -5293,23 +5380,23 @@ "issues": [] } }, - "search_text": "Figura 60 | spettro UV-Visibile e di emissione del copolimero 3c in THF | Spettro UV-Visibile e di emissione normalizzati del copolimero 3c in THF. | 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. | composti: 3c | UV-Vis, fluorescenza, copolimero, THF" + "search_text": "Figura 61 | spettro UV-Visibile e di emissione del copolimero 3c in THF | Spettro UV-Visibile e di emissione normalizzati del copolimero 3c in THF. | 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. | composti: 3c | UV-Vis, fluorescenza, copolimero, THF" }, { - "id": "fig-061", - "number": 61, - "label": "Figura 61", + "id": "fig-062", + "number": 62, + "label": "Figura 62", "type": "photo", "title": "film solidi dei copolimeri sotto lampada UV, in ordine copolimero 3a, 3b, 3c", "caption": "Film solidi dei copolimeri 3a, 3b e 3c sotto lampada UV: l'emissione risulta praticamente assente (quenching da aggregazione).", "alt_text": "Film solidi dei copolimeri 3a, 3b e 3c sotto lampada UV: l'emissione risulta praticamente assente (quenching da aggregazione).", - "caption_printed": "Figura 61 - film solidi dei copolimeri sotto lampada UV, in ordine copolimero 3a, 3b, 3c", + "caption_printed": "Figura 62 - film solidi dei copolimeri sotto lampada UV, in ordine copolimero 3a, 3b, 3c", "location": { "chapter": "4", "section": "4.2", "section_title": "Copolimeri coniugati", - "md_line": 932, - "caption_md_line": 934 + "md_line": 949, + "caption_md_line": 951 }, "panels": [ { @@ -5317,7 +5404,7 @@ "file": "efcc22eae8c7e8ff910d35fa7c018b13417126c67a70da70eed1784a889d6d32.jpg", "path": "immagini/efcc22eae8c7e8ff910d35fa7c018b13417126c67a70da70eed1784a889d6d32.jpg", "embed": "![[immagini/efcc22eae8c7e8ff910d35fa7c018b13417126c67a70da70eed1784a889d6d32.jpg]]", - "md_line": 932, + "md_line": 949, "width": 1020, "height": 343, "description": "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).", @@ -5353,7 +5440,7 @@ ], "text_context": "Il testo spiega che allo stato solido l'aggregazione porta a quenching emissivo, criticità per i sistemi lineari.", "cited_in_md_lines": [ - 930 + 947 ], "quality": { "confidence": "high", @@ -5366,23 +5453,23 @@ "issues": [] } }, - "search_text": "Figura 61 | film solidi dei copolimeri sotto lampada UV, in ordine copolimero 3a, 3b, 3c | Film solidi dei copolimeri 3a, 3b e 3c sotto lampada UV: l'emissione risulta praticamente assente (quenching da aggregazione). | 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). | composti: 3a, 3b, 3c | film solidi, lampada UV, quenching, aggregazione, fluorescenza stato solido" + "search_text": "Figura 62 | film solidi dei copolimeri sotto lampada UV, in ordine copolimero 3a, 3b, 3c | Film solidi dei copolimeri 3a, 3b e 3c sotto lampada UV: l'emissione risulta praticamente assente (quenching da aggregazione). | 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). | composti: 3a, 3b, 3c | film solidi, lampada UV, quenching, aggregazione, fluorescenza stato solido" }, { - "id": "fig-062", - "number": 62, - "label": "Figura 62", + "id": "fig-063", + "number": 63, + "label": "Figura 63", "type": "diagram", - "title": "effetto dell'intensità dello stacking π-π sull'emissione luminosa", + "title": "Effetto dell'intensità dello stacking π-π sull'emissione luminosa", "caption": "Schema dell'effetto dell'intensità dello stacking π-π sull'emissione luminosa.", "alt_text": "Schema dell'effetto dell'intensità dello stacking π-π sull'emissione luminosa.", - "caption_printed": "Figura 62 - effetto dell'intensità dello stacking π-π sull'emissione luminosa", + "caption_printed": "Figura 63 - Effetto dell'intensità dello stacking π-π sull'emissione luminosa", "location": { "chapter": "4", "section": "4.3", "section_title": "Polimeri bottle brush", - "md_line": 961, - "caption_md_line": 963 + "md_line": 980, + "caption_md_line": 982 }, "panels": [ { @@ -5390,7 +5477,7 @@ "file": "a3ecc2457962649d36b1824710784bec90b0e52d32275fc154743f9bf9f62339.jpg", "path": "immagini/a3ecc2457962649d36b1824710784bec90b0e52d32275fc154743f9bf9f62339.jpg", "embed": "![[immagini/a3ecc2457962649d36b1824710784bec90b0e52d32275fc154743f9bf9f62339.jpg]]", - "md_line": 961, + "md_line": 980, "width": 1021, "height": 471, "description": "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'.", @@ -5434,23 +5521,23 @@ ] } }, - "search_text": "Figura 62 | effetto dell'intensità dello stacking π-π sull'emissione luminosa | Schema dell'effetto dell'intensità dello stacking π-π sull'emissione luminosa. | 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'. | π-π stacking, bottle brush, quenching, emissione, catene laterali" + "search_text": "Figura 63 | Effetto dell'intensità dello stacking π-π sull'emissione luminosa | Schema dell'effetto dell'intensità dello stacking π-π sull'emissione luminosa. | 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'. | π-π stacking, bottle brush, quenching, emissione, catene laterali" }, { - "id": "fig-063", - "number": 63, - "label": "Figura 63", + "id": "fig-064", + "number": 64, + "label": "Figura 64", "type": "mechanism", "title": "meccanismo di reazione della ROP con gruppo alcolico come iniziatore", "caption": "Meccanismo di polimerizzazione per apertura d'anello (ROP) dell'ε-caprolattone con iniziatore alcolico e Sn(Oct)2 (coordinazione-inserzione).", "alt_text": "Meccanismo di polimerizzazione per apertura d'anello (ROP) dell'ε-caprolattone con iniziatore alcolico e Sn(Oct)2 (coordinazione-inserzione): scambio di leganti con R-OH, coordinazione e attacco nucleofilo sul carbonile, apertura dell'anello e propagazione della catena.", - "caption_printed": "Figura 63 - meccanismo di reazione della ROP con gruppo alcolico come iniziatore", + "caption_printed": "Figura 64 - meccanismo di reazione della ROP con gruppo alcolico come iniziatore", "location": { "chapter": "4", "section": "4.3", "section_title": "Polimeri bottle brush", - "md_line": 971, - "caption_md_line": 973 + "md_line": 990, + "caption_md_line": 992 }, "panels": [ { @@ -5458,7 +5545,7 @@ "file": "86add528de15d390b0a228d524bbd008d318d4ae0e85530a063f2df5ddf904ee.jpg", "path": "immagini/86add528de15d390b0a228d524bbd008d318d4ae0e85530a063f2df5ddf904ee.jpg", "embed": "![[immagini/86add528de15d390b0a228d524bbd008d318d4ae0e85530a063f2df5ddf904ee.jpg]]", - "md_line": 971, + "md_line": 990, "width": 1254, "height": 387, "description": "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.", @@ -5501,7 +5588,7 @@ ], "text_context": "Il testo descrive il meccanismo di coordinazione-inserzione catalizzato da stagno ottanoato.", "cited_in_md_lines": [ - 969 + 988 ], "quality": { "confidence": "high", @@ -5516,23 +5603,23 @@ ] } }, - "search_text": "Figura 63 | meccanismo di reazione della ROP con gruppo alcolico come iniziatore | Meccanismo di polimerizzazione per apertura d'anello (ROP) dell'ε-caprolattone con iniziatore alcolico e Sn(Oct)2 (coordinazione-inserzione). | 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. | composti: PCL, Sn(Oct)2, ε-caprolattone | ROP, coordinazione-inserzione, Sn(Oct)2, PCL, caprolattone, iniziatore alcolico" + "search_text": "Figura 64 | meccanismo di reazione della ROP con gruppo alcolico come iniziatore | Meccanismo di polimerizzazione per apertura d'anello (ROP) dell'ε-caprolattone con iniziatore alcolico e Sn(Oct)2 (coordinazione-inserzione). | 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. | composti: PCL, Sn(Oct)2, ε-caprolattone | ROP, coordinazione-inserzione, Sn(Oct)2, PCL, caprolattone, iniziatore alcolico" }, { - "id": "fig-064", - "number": 64, - "label": "Figura 64", + "id": "fig-065", + "number": 65, + "label": "Figura 65", "type": "spectrum_nmr", "title": "spettro 1H-NMR del polimero 3.1b in CDCl3", "caption": "Spettro 1H-NMR del polimero bottle brush 3.1b in CDCl3, con i segnali caratteristici del PCL assegnati sulla struttura.", "alt_text": "Spettro 1H-NMR del polimero bottle brush 3.1b in CDCl3, con i segnali caratteristici del PCL assegnati sulla struttura.", - "caption_printed": "Figura 64 - spettro 1H-NMR del polimero 3.1b in CDCl3", + "caption_printed": "Figura 65 - spettro 1H-NMR del polimero 3.1b in CDCl3", "location": { "chapter": "4", "section": "4.3", "section_title": "Polimeri bottle brush", - "md_line": 1002, - "caption_md_line": 1004 + "md_line": 1021, + "caption_md_line": 1023 }, "panels": [ { @@ -5540,7 +5627,7 @@ "file": "aae4bec55b3a0f29e1dfa6231c86c1d0295d5d38f2f2e9f0af6a69eba8aa0231.jpg", "path": "immagini/aae4bec55b3a0f29e1dfa6231c86c1d0295d5d38f2f2e9f0af6a69eba8aa0231.jpg", "embed": "![[immagini/aae4bec55b3a0f29e1dfa6231c86c1d0295d5d38f2f2e9f0af6a69eba8aa0231.jpg]]", - "md_line": 1002, + "md_line": 1021, "width": 1092, "height": 721, "description": "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.", @@ -5591,7 +5678,7 @@ ], "text_context": "Il testo verifica la polimerizzazione del caprolattone dalla comparsa dei segnali caratteristici del PCL.", "cited_in_md_lines": [ - 1000 + 1019 ], "quality": { "confidence": "high", @@ -5605,23 +5692,23 @@ ] } }, - "search_text": "Figura 64 | spettro 1H-NMR del polimero 3.1b in CDCl3 | Spettro 1H-NMR del polimero bottle brush 3.1b in CDCl3, con i segnali caratteristici del PCL assegnati sulla struttura. | 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. | composti: 3.1b, PCL | 1H-NMR, CDCl3, PCL, bottle brush, ROP" + "search_text": "Figura 65 | spettro 1H-NMR del polimero 3.1b in CDCl3 | Spettro 1H-NMR del polimero bottle brush 3.1b in CDCl3, con i segnali caratteristici del PCL assegnati sulla struttura. | 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. | composti: 3.1b, PCL | 1H-NMR, CDCl3, PCL, bottle brush, ROP" }, { - "id": "fig-065", - "number": 65, - "label": "Figura 65", + "id": "fig-066", + "number": 66, + "label": "Figura 66", "type": "spectrum_ir", - "title": "spettri FT-IR dei polimeri bottle brush ottenuti a partire dal copolimero 3b (verde)", + "title": "spettri FT-IR dei polimeri bottle brush ottenuti a partire dal copolimero 3b (verde):", "caption": "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).", "alt_text": "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).", - "caption_printed": "Figura 65 - spettri FT-IR dei polimeri bottle brush ottenuti a partire dal copolimero 3b (verde)", + "caption_printed": "Figura 66 - spettri FT-IR dei polimeri bottle brush ottenuti a partire dal copolimero 3b (verde):", "location": { "chapter": "4", "section": "4.3", "section_title": "Polimeri bottle brush", - "md_line": 1012, - "caption_md_line": 1014 + "md_line": 1031, + "caption_md_line": 1033 }, "panels": [ { @@ -5629,7 +5716,7 @@ "file": "4cd08436660a2e3a6f913e54d196a0d183b780c3f5f915be6d22a563771d3e43.jpg", "path": "immagini/4cd08436660a2e3a6f913e54d196a0d183b780c3f5f915be6d22a563771d3e43.jpg", "embed": "![[immagini/4cd08436660a2e3a6f913e54d196a0d183b780c3f5f915be6d22a563771d3e43.jpg]]", - "md_line": 1012, + "md_line": 1031, "width": 1174, "height": 829, "description": "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.", @@ -5690,7 +5777,7 @@ ], "text_context": "Il testo evidenzia la scomparsa dell'OH e la crescita dei segnali PCL con l'aumentare delle catene laterali.", "cited_in_md_lines": [ - 1006 + 1025 ], "quality": { "confidence": "medium", @@ -5706,23 +5793,23 @@ ] } }, - "search_text": "Figura 65 | spettri FT-IR dei polimeri bottle brush ottenuti a partire dal copolimero 3b (verde) | 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). | 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. | composti: 3b, 3.1b, 3.2b, 3.3b, PCL | FT-IR, PCL, C=O estere, bottle brush, OH" + "search_text": "Figura 66 | spettri FT-IR dei polimeri bottle brush ottenuti a partire dal copolimero 3b (verde): | 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). | 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. | composti: 3b, 3.1b, 3.2b, 3.3b, PCL | FT-IR, PCL, C=O estere, bottle brush, OH" }, { - "id": "fig-066", - "number": 66, - "label": "Figura 66", + "id": "fig-067", + "number": 67, + "label": "Figura 67", "type": "spectrum_ir", - "title": "spettri FT-IR dei polimeri bottle brush ottenuti a partire dal copolimero 3c (verde)", + "title": "spettri FT-IR dei polimeri bottle brush ottenuti a partire dal copolimero 3c (verde):", "caption": "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).", "alt_text": "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).", - "caption_printed": "Figura 66 - spettri FT-IR dei polimeri bottle brush ottenuti a partire dal copolimero 3c (verde)", + "caption_printed": "Figura 67 - spettri FT-IR dei polimeri bottle brush ottenuti a partire dal copolimero 3c (verde):", "location": { "chapter": "4", "section": "4.3", "section_title": "Polimeri bottle brush", - "md_line": 1018, - "caption_md_line": 1020 + "md_line": 1037, + "caption_md_line": 1039 }, "panels": [ { @@ -5730,10 +5817,10 @@ "file": "d5559d2ff37ffb2861c2ac8eecbade7c09f8fc905c8363be4f48c06a0afae72e.jpg", "path": "immagini/d5559d2ff37ffb2861c2ac8eecbade7c09f8fc905c8363be4f48c06a0afae72e.jpg", "embed": "![[immagini/d5559d2ff37ffb2861c2ac8eecbade7c09f8fc905c8363be4f48c06a0afae72e.jpg]]", - "md_line": 1018, + "md_line": 1037, "width": 1176, "height": 873, - "description": "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.", + "description": "Quattro tracce come in Figura 66 (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.", "visible_text": [ "Trasmittanza", "Lunghezza d'onda [cm-1]", @@ -5785,7 +5872,7 @@ ], "text_context": "Seconda serie di polimeri bottle brush a confronto con il precursore.", "cited_in_md_lines": [ - 1006 + 1025 ], "quality": { "confidence": "medium", @@ -5801,23 +5888,23 @@ ] } }, - "search_text": "Figura 66 | spettri FT-IR dei polimeri bottle brush ottenuti a partire dal copolimero 3c (verde) | 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). | 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. | composti: 3c, 3.1c, 3.2c, 3.3c, PCL | FT-IR, PCL, bottle brush, C=O estere" + "search_text": "Figura 67 | spettri FT-IR dei polimeri bottle brush ottenuti a partire dal copolimero 3c (verde): | 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). | 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. | composti: 3c, 3.1c, 3.2c, 3.3c, PCL | FT-IR, PCL, bottle brush, C=O estere" }, { - "id": "fig-067", - "number": 67, - "label": "Figura 67", + "id": "fig-068", + "number": 68, + "label": "Figura 68", "type": "spectrum_fluorescence", - "title": "spettri UV-Visibile (linea continua) e di emissione (linea tratteggiata) dei polimeri bottle brush in THF", + "title": "spettri UV-Visibile (linea continua) e di emissione (linea tratteggiata) dei polimeri bottle brush in THF (λecc=490 nm)", "caption": "Spettri UV-Visibile (continua) ed emissione (tratteggiata) normalizzati dei sei polimeri bottle brush 3.1b-3.3b e 3.1c-3.3c in THF.", "alt_text": "Spettri UV-Visibile (continua) ed emissione (tratteggiata) normalizzati dei sei polimeri bottle brush 3.1b-3.3b e 3.1c-3.3c in THF.", - "caption_printed": "Figura 67 - spettri UV-Visibile (linea continua) e di emissione (linea tratteggiata) dei polimeri bottle brush in THF", + "caption_printed": "Figura 68 - spettri UV-Visibile (linea continua) e di emissione (linea tratteggiata) dei polimeri bottle brush in THF (λecc=490 nm)", "location": { "chapter": "4", "section": "4.3", "section_title": "Polimeri bottle brush", - "md_line": 1026, - "caption_md_line": 1028 + "md_line": 1045, + "caption_md_line": 1047 }, "panels": [ { @@ -5825,7 +5912,7 @@ "file": "be53b102694fafa8036962962c8c0a3735cc1ec95cf721f163b7d25bdd7099fb.png", "path": "immagini/be53b102694fafa8036962962c8c0a3735cc1ec95cf721f163b7d25bdd7099fb.png", "embed": "![[immagini/be53b102694fafa8036962962c8c0a3735cc1ec95cf721f163b7d25bdd7099fb.png]]", - "md_line": 1026, + "md_line": 1045, "width": 1005, "height": 1235, "description": "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.", @@ -5866,7 +5953,7 @@ ], "text_context": "Il testo riporta massimi di assorbimento 544-554 nm ed emissione 557-564 nm (Tabella 10).", "cited_in_md_lines": [ - 1024 + 1043 ], "quality": { "confidence": "high", @@ -5877,23 +5964,23 @@ "issues": [] } }, - "search_text": "Figura 67 | spettri UV-Visibile (linea continua) e di emissione (linea tratteggiata) dei polimeri bottle brush in THF | Spettri UV-Visibile (continua) ed emissione (tratteggiata) normalizzati dei sei polimeri bottle brush 3.1b-3.3b e 3.1c-3.3c in THF. | 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. | composti: 3.1b, 3.2b, 3.3b, 3.1c, 3.2c, 3.3c | UV-Vis, fluorescenza, bottle brush, THF" + "search_text": "Figura 68 | spettri UV-Visibile (linea continua) e di emissione (linea tratteggiata) dei polimeri bottle brush in THF (λecc=490 nm) | Spettri UV-Visibile (continua) ed emissione (tratteggiata) normalizzati dei sei polimeri bottle brush 3.1b-3.3b e 3.1c-3.3c in THF. | 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. | composti: 3.1b, 3.2b, 3.3b, 3.1c, 3.2c, 3.3c | UV-Vis, fluorescenza, bottle brush, THF" }, { - "id": "fig-068", - "number": 68, - "label": "Figura 68", + "id": "fig-069", + "number": 69, + "label": "Figura 69", "type": "plot", "title": "esempio di termogramma dei polimeri bottle brush realizzati (in figura l'analisi del campione 3.1c)", "caption": "Termogramma DSC del polimero bottle brush 3.1c, con picco di fusione e picco di cristallizzazione del PCL.", "alt_text": "Termogramma DSC del polimero bottle brush 3.1c, con picco di fusione e picco di cristallizzazione del PCL.", - "caption_printed": "Figura 68 - esempio di termogramma dei polimeri bottle brush realizzati (in figura l'analisi del campione 3.1c)", + "caption_printed": "Figura 69 - esempio di termogramma dei polimeri bottle brush realizzati (in figura l'analisi del campione 3.1c)", "location": { "chapter": "4", "section": "4.3", "section_title": "Polimeri bottle brush", - "md_line": 1095, - "caption_md_line": 1097 + "md_line": 1114, + "caption_md_line": 1116 }, "panels": [ { @@ -5901,7 +5988,7 @@ "file": "d2ed44d32060aa9ee04e73304940b111e53bf65cf115a93ace696933048e308b.jpg", "path": "immagini/d2ed44d32060aa9ee04e73304940b111e53bf65cf115a93ace696933048e308b.jpg", "embed": "![[immagini/d2ed44d32060aa9ee04e73304940b111e53bf65cf115a93ace696933048e308b.jpg]]", - "md_line": 1095, + "md_line": 1114, "width": 1210, "height": 554, "description": "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'.", @@ -5961,23 +6048,23 @@ ] } }, - "search_text": "Figura 68 | esempio di termogramma dei polimeri bottle brush realizzati (in figura l'analisi del campione 3.1c) | Termogramma DSC del polimero bottle brush 3.1c, con picco di fusione e picco di cristallizzazione del PCL. | 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'. | composti: 3.1c, PCL | DSC, fusione, cristallizzazione, PCL, bottle brush, termogramma" + "search_text": "Figura 69 | esempio di termogramma dei polimeri bottle brush realizzati (in figura l'analisi del campione 3.1c) | Termogramma DSC del polimero bottle brush 3.1c, con picco di fusione e picco di cristallizzazione del PCL. | 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'. | composti: 3.1c, PCL | DSC, fusione, cristallizzazione, PCL, bottle brush, termogramma" }, { - "id": "fig-069", - "number": 69, - "label": "Figura 69", + "id": "fig-070", + "number": 70, + "label": "Figura 70", "type": "cv_voltammogram", - "title": "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", + "title": "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.", "caption": "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.", "alt_text": "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.", - "caption_printed": "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", + "caption_printed": "Figura 70 - 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.", "location": { "chapter": "4", "section": "4.4.2", "section_title": "Metodologie di analisi voltammetrica", - "md_line": 1128, - "caption_md_line": 1130 + "md_line": 1147, + "caption_md_line": 1149 }, "panels": [ { @@ -5985,7 +6072,7 @@ "file": "6afc0d601841f25b1c02e27bc6b1616abc101c5f1ceaa0ba9d30ed0f965ebed2.jpg", "path": "immagini/6afc0d601841f25b1c02e27bc6b1616abc101c5f1ceaa0ba9d30ed0f965ebed2.jpg", "embed": "![[immagini/6afc0d601841f25b1c02e27bc6b1616abc101c5f1ceaa0ba9d30ed0f965ebed2.jpg]]", - "md_line": 1128, + "md_line": 1147, "width": 1190, "height": 754, "description": "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).", @@ -6035,8 +6122,8 @@ ], "text_context": "Esempio della procedura di determinazione dei potenziali di onset applicata a tutti i materiali.", "cited_in_md_lines": [ - 1126, - 1148 + 1145, + 1167 ], "quality": { "confidence": "high", @@ -6047,23 +6134,23 @@ "issues": [] } }, - "search_text": "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 | 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. | 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). | composti: 3.2c | ciclovoltammetria, potenziale di onset, THF, TBAPF6, HOMO-LUMO, 0.05 V/s" + "search_text": "Figura 70 | 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. | 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. | 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). | composti: 3.2c | ciclovoltammetria, potenziale di onset, THF, TBAPF6, HOMO-LUMO, 0.05 V/s" }, { - "id": "fig-070", - "number": 70, - "label": "Figura 70", + "id": "fig-071", + "number": 71, + "label": "Figura 71", "type": "cv_voltammogram", - "title": "voltammogramma ciclico del polimero 3.2.c registrato a diverse velocità di scansione", + "title": "Voltammogramma ciclico del polimero 3.2.c registrato a diverse velocità di scansione", "caption": "Voltammogrammi ciclici del polimero 3.2c a diverse velocità di scansione (0.05, 0.1, 0.5, 1 V/s).", "alt_text": "Voltammogrammi ciclici del polimero 3.2c a diverse velocità di scansione (0.05, 0.1, 0.5, 1 V/s).", - "caption_printed": "Figura 70 - voltammogramma ciclico del polimero 3.2.c registrato a diverse velocità di scansione", + "caption_printed": "Figura 71 - Voltammogramma ciclico del polimero 3.2.c registrato a diverse velocità di scansione", "location": { "chapter": "4", "section": "4.4.2", "section_title": "Metodologie di analisi voltammetrica", - "md_line": 1136, - "caption_md_line": 1138 + "md_line": 1155, + "caption_md_line": 1157 }, "panels": [ { @@ -6071,7 +6158,7 @@ "file": "5491a0651d00b47f168b335586b4f144e1b25834ff74113ff26b1d3a2c8cc991.jpg", "path": "immagini/5491a0651d00b47f168b335586b4f144e1b25834ff74113ff26b1d3a2c8cc991.jpg", "embed": "![[immagini/5491a0651d00b47f168b335586b4f144e1b25834ff74113ff26b1d3a2c8cc991.jpg]]", - "md_line": 1136, + "md_line": 1155, "width": 1076, "height": 704, "description": "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).", @@ -6108,7 +6195,7 @@ ], "text_context": "Il testo osserva l'assenza di onde di scarica simmetriche al ritorno e la progressiva diminuzione delle correnti con la velocità.", "cited_in_md_lines": [ - 1140 + 1159 ], "quality": { "confidence": "high", @@ -6119,23 +6206,23 @@ "issues": [] } }, - "search_text": "Figura 70 | voltammogramma ciclico del polimero 3.2.c registrato a diverse velocità di scansione | Voltammogrammi ciclici del polimero 3.2c a diverse velocità di scansione (0.05, 0.1, 0.5, 1 V/s). | 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). | composti: 3.2c | ciclovoltammetria, velocità di scansione, reversibilità, THF" + "search_text": "Figura 71 | Voltammogramma ciclico del polimero 3.2.c registrato a diverse velocità di scansione | Voltammogrammi ciclici del polimero 3.2c a diverse velocità di scansione (0.05, 0.1, 0.5, 1 V/s). | 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). | composti: 3.2c | ciclovoltammetria, velocità di scansione, reversibilità, THF" }, { - "id": "fig-071", - "number": 71, - "label": "Figura 71", + "id": "fig-072", + "number": 72, + "label": "Figura 72", "type": "plot", "title": "correlazione tra bandgap elettrochimico e frazione reale di DPP nei copolimeri sintetizzati", "caption": "Correlazione tra bandgap elettrochimico (eV) e frazione reale di DPP nei copolimeri sintetizzati: il bandgap cresce con il contenuto di DPP.", "alt_text": "Correlazione tra bandgap elettrochimico (eV) e frazione reale di DPP nei copolimeri sintetizzati: il bandgap cresce con il contenuto di DPP.", - "caption_printed": "Figura 71 - correlazione tra bandgap elettrochimico e frazione reale di DPP nei copolimeri sintetizzati", + "caption_printed": "Figura 72 - correlazione tra bandgap elettrochimico e frazione reale di DPP nei copolimeri sintetizzati", "location": { "chapter": "4", "section": "4.4.3", "section_title": "Proprietà elettrochimiche dei copolimeri lienari", - "md_line": 1193, - "caption_md_line": 1195 + "md_line": 1212, + "caption_md_line": 1214 }, "panels": [ { @@ -6143,7 +6230,7 @@ "file": "6c7bd8393eb8c1a329f65b7fc74e5f338a866e514455c0122a43d13ca340ded5.jpg", "path": "immagini/6c7bd8393eb8c1a329f65b7fc74e5f338a866e514455c0122a43d13ca340ded5.jpg", "embed": "![[immagini/6c7bd8393eb8c1a329f65b7fc74e5f338a866e514455c0122a43d13ca340ded5.jpg]]", - "md_line": 1193, + "md_line": 1212, "width": 940, "height": 570, "description": "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.", @@ -6187,7 +6274,7 @@ ], "text_context": "Il testo illustra la correlazione sperimentale tra ampiezza del bandgap e frazione reale di DPP: all'aumentare del DPP il bandgap si allarga.", "cited_in_md_lines": [ - 1191 + 1210 ], "quality": { "confidence": "high", @@ -6198,23 +6285,23 @@ "issues": [] } }, - "search_text": "Figura 71 | correlazione tra bandgap elettrochimico e frazione reale di DPP nei copolimeri sintetizzati | Correlazione tra bandgap elettrochimico (eV) e frazione reale di DPP nei copolimeri sintetizzati: il bandgap cresce con il contenuto di DPP. | 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. | composti: DPP | ciclovoltammetria, bandgap elettrochimico, frazione reale DPP, copolimeri lineari" + "search_text": "Figura 72 | correlazione tra bandgap elettrochimico e frazione reale di DPP nei copolimeri sintetizzati | Correlazione tra bandgap elettrochimico (eV) e frazione reale di DPP nei copolimeri sintetizzati: il bandgap cresce con il contenuto di DPP. | 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. | composti: DPP | ciclovoltammetria, bandgap elettrochimico, frazione reale DPP, copolimeri lineari" }, { - "id": "fig-072", - "number": 72, - "label": "Figura 72", + "id": "fig-073", + "number": 73, + "label": "Figura 73", "type": "plot", "title": "correlazione tra Epicco e frazione reale di DPP nei copolimeri sintetizzati", "caption": "Potenziali di picco anodico e catodico in funzione della frazione reale di DPP nei copolimeri sintetizzati.", "alt_text": "Potenziali di picco anodico e catodico in funzione della frazione reale di DPP nei copolimeri sintetizzati.", - "caption_printed": "Figura 72 - correlazione tra Epicco e frazione reale di DPP nei copolimeri sintetizzati", + "caption_printed": "Figura 73 - correlazione tra Epicco e frazione reale di DPP nei copolimeri sintetizzati", "location": { "chapter": "4", "section": "4.4.3", "section_title": "Proprietà elettrochimiche dei copolimeri lienari", - "md_line": 1205, - "caption_md_line": 1207 + "md_line": 1224, + "caption_md_line": 1226 }, "panels": [ { @@ -6222,7 +6309,7 @@ "file": "d7a3694f2d97dcaa84465aeed07d8d26adca6a8f8ed64f7ea2bf86943b918b66.jpg", "path": "immagini/d7a3694f2d97dcaa84465aeed07d8d26adca6a8f8ed64f7ea2bf86943b918b66.jpg", "embed": "![[immagini/d7a3694f2d97dcaa84465aeed07d8d26adca6a8f8ed64f7ea2bf86943b918b66.jpg]]", - "md_line": 1205, + "md_line": 1224, "width": 937, "height": 584, "description": "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.", @@ -6270,23 +6357,23 @@ "issues": [] } }, - "search_text": "Figura 72 | correlazione tra Epicco e frazione reale di DPP nei copolimeri sintetizzati | Potenziali di picco anodico e catodico in funzione della frazione reale di DPP nei copolimeri sintetizzati. | 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. | composti: DPP | ciclovoltammetria, potenziale di picco, drogaggio n, ossidazione/riduzione" + "search_text": "Figura 73 | correlazione tra Epicco e frazione reale di DPP nei copolimeri sintetizzati | Potenziali di picco anodico e catodico in funzione della frazione reale di DPP nei copolimeri sintetizzati. | 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. | composti: DPP | ciclovoltammetria, potenziale di picco, drogaggio n, ossidazione/riduzione" }, { - "id": "fig-073", - "number": 73, - "label": "Figura 73", + "id": "fig-074", + "number": 74, + "label": "Figura 74", "type": "plot", "title": "correlazione tra Eonset e frazione reale di DPP nei copolimeri sintetizzati", "caption": "Potenziali di onset anodico e catodico in funzione della frazione reale di DPP nei copolimeri sintetizzati.", "alt_text": "Potenziali di onset anodico e catodico in funzione della frazione reale di DPP nei copolimeri sintetizzati.", - "caption_printed": "Figura 73 - correlazione tra Eonset e frazione reale di DPP nei copolimeri sintetizzati", + "caption_printed": "Figura 74 - correlazione tra Eonset e frazione reale di DPP nei copolimeri sintetizzati", "location": { "chapter": "4", "section": "4.4.3", "section_title": "Proprietà elettrochimiche dei copolimeri lienari", - "md_line": 1217, - "caption_md_line": 1219 + "md_line": 1236, + "caption_md_line": 1238 }, "panels": [ { @@ -6294,7 +6381,7 @@ "file": "b2931ebedd31df7df3b344c25fcbb4a64aceb7b356181adecf39363e49dcb0fe.jpg", "path": "immagini/b2931ebedd31df7df3b344c25fcbb4a64aceb7b356181adecf39363e49dcb0fe.jpg", "embed": "![[immagini/b2931ebedd31df7df3b344c25fcbb4a64aceb7b356181adecf39363e49dcb0fe.jpg]]", - "md_line": 1217, + "md_line": 1236, "width": 945, "height": 587, "description": "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.", @@ -6330,7 +6417,7 @@ ], "text_context": "Il testo indica che l'onset catodico (LUMO) si sposta fortemente verso valori negativi, in linea con i potenziali di picco.", "cited_in_md_lines": [ - 1221 + 1240 ], "quality": { "confidence": "high", @@ -6341,23 +6428,23 @@ "issues": [] } }, - "search_text": "Figura 73 | correlazione tra Eonset e frazione reale di DPP nei copolimeri sintetizzati | Potenziali di onset anodico e catodico in funzione della frazione reale di DPP nei copolimeri sintetizzati. | 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. | composti: DPP | ciclovoltammetria, potenziale di onset, HOMO/LUMO" + "search_text": "Figura 74 | correlazione tra Eonset e frazione reale di DPP nei copolimeri sintetizzati | Potenziali di onset anodico e catodico in funzione della frazione reale di DPP nei copolimeri sintetizzati. | 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. | composti: DPP | ciclovoltammetria, potenziale di onset, HOMO/LUMO" }, { - "id": "fig-074", - "number": 74, - "label": "Figura 74", + "id": "fig-075", + "number": 75, + "label": "Figura 75", "type": "spectrum_uv_vis", "title": "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)", "caption": "Spettri UV-Vis (nero) ed emissione (rosso) del polimero 3.2b in soluzione (linea continua) e allo stato solido (tratteggio).", "alt_text": "Spettri UV-Vis (nero) ed emissione (rosso) del polimero 3.2b in soluzione (linea continua) e allo stato solido (tratteggio).", - "caption_printed": "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)", + "caption_printed": "Figura 75 - 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)", "location": { "chapter": "4", "section": "4.5", "section_title": "Caratterizzazione spettroscopica allo stato solido", - "md_line": 1268, - "caption_md_line": 1270 + "md_line": 1287, + "caption_md_line": 1289 }, "panels": [ { @@ -6365,7 +6452,7 @@ "file": "04f625a8b25744bf2d07d569e55558174b59a5cb564c8bdd0a53c704dfbde545.jpg", "path": "immagini/04f625a8b25744bf2d07d569e55558174b59a5cb564c8bdd0a53c704dfbde545.jpg", "embed": "![[immagini/04f625a8b25744bf2d07d569e55558174b59a5cb564c8bdd0a53c704dfbde545.jpg]]", - "md_line": 1268, + "md_line": 1287, "width": 965, "height": 648, "description": "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).", @@ -6407,7 +6494,7 @@ ], "text_context": "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.", "cited_in_md_lines": [ - 1266 + 1285 ], "quality": { "confidence": "high", @@ -6422,7 +6509,7 @@ ] } }, - "search_text": "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) | Spettri UV-Vis (nero) ed emissione (rosso) del polimero 3.2b in soluzione (linea continua) e allo stato solido (tratteggio). | 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). | composti: 3.2b | UV-Vis, fluorescenza, stato solido, soluzione, bottle brush, red shift" + "search_text": "Figura 75 | 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) | Spettri UV-Vis (nero) ed emissione (rosso) del polimero 3.2b in soluzione (linea continua) e allo stato solido (tratteggio). | 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). | composti: 3.2b | UV-Vis, fluorescenza, stato solido, soluzione, bottle brush, red shift" } ], "indexes": { @@ -6435,8 +6522,9 @@ "fig-040" ], "cv_voltammogram": [ - "fig-069", - "fig-070" + "fig-052", + "fig-070", + "fig-071" ], "diagram": [ "fig-017", @@ -6449,7 +6537,7 @@ "fig-037", "fig-038", "fig-039", - "fig-062" + "fig-063" ], "mechanism": [ "fig-005", @@ -6458,18 +6546,18 @@ "fig-042", "fig-043", "fig-046", - "fig-053", - "fig-063" + "fig-054", + "fig-064" ], "photo": [ - "fig-061" + "fig-062" ], "plot": [ "fig-051", - "fig-068", - "fig-071", + "fig-069", "fig-072", - "fig-073" + "fig-073", + "fig-074" ], "reaction_scheme": [ "fig-002", @@ -6499,33 +6587,33 @@ "fig-x-136800", "fig-041", "fig-047", - "fig-052" + "fig-053" ], "spectrum_fluorescence": [ - "fig-067" + "fig-068" ], "spectrum_ir": [ "fig-049", - "fig-057", - "fig-065", - "fig-066" + "fig-058", + "fig-066", + "fig-067" ], "spectrum_nmr": [ "fig-044", "fig-048", - "fig-054", "fig-055", "fig-056", - "fig-064" + "fig-057", + "fig-065" ], "spectrum_uv_vis": [ "fig-015", "fig-045", "fig-050", - "fig-058", "fig-059", "fig-060", - "fig-074" + "fig-061", + "fig-075" ] }, "by_section": { @@ -6602,10 +6690,10 @@ "fig-048", "fig-049", "fig-050", - "fig-051" + "fig-051", + "fig-052" ], "4.2": [ - "fig-052", "fig-053", "fig-054", "fig-055", @@ -6614,28 +6702,29 @@ "fig-058", "fig-059", "fig-060", - "fig-061" + "fig-061", + "fig-062" ], "4.3": [ - "fig-062", "fig-063", "fig-064", "fig-065", "fig-066", "fig-067", - "fig-068" + "fig-068", + "fig-069" ], "4.4.2": [ - "fig-069", - "fig-070" + "fig-070", + "fig-071" ], "4.4.3": [ - "fig-071", "fig-072", - "fig-073" + "fig-073", + "fig-074" ], "4.5": [ - "fig-074" + "fig-075" ] }, "by_compound": { @@ -6686,7 +6775,8 @@ "fig-050", "fig-051", "fig-052", - "fig-053" + "fig-053", + "fig-054" ], "20": [ "fig-013" @@ -6727,37 +6817,37 @@ "fig-003", "fig-019", "fig-020", - "fig-052", - "fig-053" + "fig-053", + "fig-054" ], "3.1b": [ - "fig-064", "fig-065", - "fig-067" - ], - "3.1c": [ "fig-066", - "fig-067", "fig-068" ], - "3.2b": [ - "fig-065", + "3.1c": [ "fig-067", - "fig-074" + "fig-068", + "fig-069" + ], + "3.2b": [ + "fig-066", + "fig-068", + "fig-075" ], "3.2c": [ - "fig-066", "fig-067", - "fig-069", - "fig-070" + "fig-068", + "fig-070", + "fig-071" ], "3.3b": [ - "fig-065", - "fig-067" + "fig-066", + "fig-068" ], "3.3c": [ - "fig-066", - "fig-067" + "fig-067", + "fig-068" ], "30": [ "fig-021" @@ -6800,33 +6890,33 @@ ], "3HT": [ "fig-x-cc3f54", - "fig-052", - "fig-053" + "fig-053", + "fig-054" ], "3a": [ "fig-x-cc3f54", - "fig-054", - "fig-057", + "fig-055", "fig-058", - "fig-061" + "fig-059", + "fig-062" ], "3b": [ "fig-x-cc3f54", "fig-x-136800", - "fig-055", - "fig-057", - "fig-059", - "fig-061", - "fig-065" + "fig-056", + "fig-058", + "fig-060", + "fig-062", + "fig-066" ], "3c": [ "fig-x-cc3f54", "fig-x-136800", - "fig-056", "fig-057", - "fig-060", + "fig-058", "fig-061", - "fig-066" + "fig-062", + "fig-067" ], "4": [ "fig-003" @@ -6912,9 +7002,9 @@ "fig-018", "fig-022", "fig-046", - "fig-071", "fig-072", - "fig-073" + "fig-073", + "fig-074" ], "DPP3": [ "fig-005", @@ -6924,41 +7014,41 @@ ], "PCL": [ "fig-x-136800", - "fig-063", "fig-064", "fig-065", "fig-066", - "fig-068" + "fig-067", + "fig-069" ], "Sn(Oct)2": [ - "fig-063" + "fig-064" ], "caprolattone": [ "fig-x-136800" ], "ε-caprolattone": [ - "fig-063" + "fig-064" ] }, "by_concept": { "0-05-v-s": [ - "fig-069" + "fig-070" ], "1h-nmr": [ "fig-044", "fig-048", - "fig-054", "fig-055", "fig-056", - "fig-064" + "fig-057", + "fig-065" ], "3-esiltiofene": [ - "fig-052", "fig-053", - "fig-057" + "fig-054", + "fig-058" ], "3ht": [ - "fig-054" + "fig-055" ], "6-bromo-1-esanolo": [ "fig-046" @@ -6969,10 +7059,10 @@ "accoppiamento-ossidativo": [ "fig-012", "fig-028", - "fig-053" + "fig-054" ], "aggregazione": [ - "fig-061" + "fig-062" ], "amidina": [ "fig-009" @@ -7014,7 +7104,7 @@ "fig-038" ], "bandgap-elettrochimico": [ - "fig-071" + "fig-072" ], "base": [ "fig-007", @@ -7038,13 +7128,13 @@ ], "bottle-brush": [ "fig-x-136800", - "fig-062", - "fig-064", + "fig-063", "fig-065", "fig-066", "fig-067", "fig-068", - "fig-074" + "fig-069", + "fig-075" ], "bromurazione": [ "fig-020", @@ -7058,14 +7148,14 @@ ], "c-h-alifatici": [ "fig-049", - "fig-057" + "fig-058" ], "c-o": [ - "fig-057" + "fig-058" ], "c-o-estere": [ - "fig-065", - "fig-066" + "fig-066", + "fig-067" ], "c-o-lattame": [ "fig-049" @@ -7074,20 +7164,20 @@ "fig-051" ], "caprolattone": [ - "fig-063" + "fig-064" ], "carbazolo": [ "fig-024" ], "catene-laterali": [ - "fig-062" + "fig-063" ], "cdcl3": [ "fig-048", - "fig-054", "fig-055", "fig-056", - "fig-064" + "fig-057", + "fig-065" ], "cella-a-tre-elettrodi": [ "fig-039" @@ -7116,11 +7206,12 @@ ], "ciclovoltammetria": [ "fig-039", - "fig-069", + "fig-052", "fig-070", "fig-071", "fig-072", - "fig-073" + "fig-073", + "fig-074" ], "clorurazione": [ "fig-020" @@ -7133,9 +7224,9 @@ "fig-051" ], "composizione-copolimero": [ - "fig-054", "fig-055", - "fig-056" + "fig-056", + "fig-057" ], "condensazione-di-claisen": [ "fig-043" @@ -7147,25 +7238,25 @@ "fig-031" ], "coordinazione-inserzione": [ - "fig-063" + "fig-064" ], "copolimeri": [ - "fig-057" + "fig-058" ], "copolimeri-lineari": [ - "fig-071" + "fig-072" ], "copolimero": [ - "fig-052", - "fig-058", + "fig-053", "fig-059", - "fig-060" + "fig-060", + "fig-061" ], "copolimero-dpp-3ht": [ "fig-x-cc3f54" ], "cristallizzazione": [ - "fig-068" + "fig-069" ], "cross-coupling": [ "fig-017", @@ -7235,8 +7326,8 @@ "fig-045", "fig-046", "fig-049", - "fig-052", - "fig-054" + "fig-053", + "fig-055" ], "dpp-alchilato": [ "fig-048", @@ -7248,11 +7339,17 @@ "dpp-bromurato": [ "fig-026" ], + "drogaggio-di-tipo-n": [ + "fig-052" + ], + "drogaggio-di-tipo-p": [ + "fig-052" + ], "drogaggio-n": [ - "fig-072" + "fig-073" ], "dsc": [ - "fig-068" + "fig-069" ], "eccitone": [ "fig-038" @@ -7271,7 +7368,7 @@ ], "emissione": [ "fig-045", - "fig-062" + "fig-063" ], "eml": [ "fig-037" @@ -7295,11 +7392,11 @@ "fig-028", "fig-x-185efd", "fig-x-cc3f54", - "fig-052", - "fig-053" + "fig-053", + "fig-054" ], "film-solidi": [ - "fig-061" + "fig-062" ], "fluorene": [ "fig-024" @@ -7311,14 +7408,14 @@ "fig-040", "fig-045", "fig-050", - "fig-058", "fig-059", "fig-060", - "fig-067", - "fig-074" + "fig-061", + "fig-068", + "fig-075" ], "fluorescenza-stato-solido": [ - "fig-061" + "fig-062" ], "fluoroareni": [ "fig-027" @@ -7340,13 +7437,13 @@ "fig-034" ], "frazione-reale-dpp": [ - "fig-071" + "fig-072" ], "ft-ir": [ "fig-049", - "fig-057", - "fig-065", - "fig-066" + "fig-058", + "fig-066", + "fig-067" ], "furano": [ "fig-021" @@ -7355,7 +7452,7 @@ "fig-012" ], "fusione": [ - "fig-068" + "fig-069" ], "glassy-carbon": [ "fig-039" @@ -7371,8 +7468,8 @@ ], "homo-lumo": [ "fig-038", - "fig-069", - "fig-073" + "fig-070", + "fig-074" ], "host-guest": [ "fig-035" @@ -7384,12 +7481,12 @@ "fig-011" ], "iniziatore-alcolico": [ - "fig-063" + "fig-064" ], "integrazione": [ - "fig-054", "fig-055", - "fig-056" + "fig-056", + "fig-057" ], "interazioni-intermolecolari": [ "fig-015" @@ -7409,6 +7506,9 @@ "fig-007", "fig-014" ], + "irreversibilita": [ + "fig-052" + ], "iso-dpp": [ "fig-040" ], @@ -7416,7 +7516,7 @@ "fig-037" ], "lampada-uv": [ - "fig-061" + "fig-062" ], "langhals": [ "fig-012", @@ -7451,6 +7551,9 @@ "fig-042", "fig-043" ], + "meccanismo-ec": [ + "fig-052" + ], "n-alchilazione": [ "fig-022", "fig-x-f6eeb1", @@ -7464,7 +7567,7 @@ "fig-021" ], "nitrometano": [ - "fig-052" + "fig-053" ], "nucleofilo": [ "fig-017" @@ -7473,7 +7576,7 @@ "fig-049" ], "oh": [ - "fig-065" + "fig-066" ], "oled": [ "fig-036", @@ -7486,7 +7589,7 @@ "fig-047" ], "ossidazione-riduzione": [ - "fig-072" + "fig-073" ], "p3ht": [ "fig-x-cc3f54" @@ -7495,11 +7598,11 @@ "fig-023" ], "pcl": [ - "fig-063", "fig-064", "fig-065", "fig-066", - "fig-068" + "fig-067", + "fig-069" ], "pd-oac-2": [ "fig-025", @@ -7527,8 +7630,8 @@ "polimerizzazione-ossidativa": [ "fig-028", "fig-x-cc3f54", - "fig-052", - "fig-053" + "fig-053", + "fig-054" ], "polimero-coniugato": [ "fig-038" @@ -7537,11 +7640,11 @@ "fig-028" ], "potenziale-di-onset": [ - "fig-069", - "fig-073" + "fig-070", + "fig-074" ], "potenziale-di-picco": [ - "fig-072" + "fig-073" ], "protezione": [ "fig-019" @@ -7552,14 +7655,14 @@ "fig-042" ], "quenching": [ - "fig-061", - "fig-062" + "fig-062", + "fig-063" ], "radical-catione": [ "fig-028" ], "radicale": [ - "fig-053" + "fig-054" ], "reattivita": [ "fig-017" @@ -7569,7 +7672,7 @@ "fig-047" ], "red-shift": [ - "fig-074" + "fig-075" ], "reformatskij": [ "fig-002", @@ -7584,7 +7687,7 @@ "fig-006" ], "reversibilita": [ - "fig-070" + "fig-071" ], "riepilogo-sintesi-dpp": [ "fig-014" @@ -7603,8 +7706,8 @@ ], "rop": [ "fig-x-136800", - "fig-063", - "fig-064" + "fig-064", + "fig-065" ], "sale-di-zinco": [ "fig-004" @@ -7628,7 +7731,7 @@ ], "sn-oct-2": [ "fig-x-136800", - "fig-063" + "fig-064" ], "snar": [ "fig-030" @@ -7637,7 +7740,7 @@ "fig-020" ], "soluzione": [ - "fig-074" + "fig-075" ], "sonogashira": [ "fig-023" @@ -7662,13 +7765,13 @@ "fig-011" ], "stacking": [ - "fig-062" + "fig-063" ], "stannilazione": [ "fig-029" ], "stato-solido": [ - "fig-074" + "fig-075" ], "stato-solido-vs-soluzione": [ "fig-015" @@ -7707,10 +7810,10 @@ ], "tbapf6": [ "fig-039", - "fig-069" + "fig-070" ], "termogramma": [ - "fig-068" + "fig-069" ], "tetraidro-dpp": [ "fig-011" @@ -7725,12 +7828,13 @@ "fig-039", "fig-045", "fig-050", - "fig-058", + "fig-052", "fig-059", "fig-060", - "fig-067", - "fig-069", - "fig-070" + "fig-061", + "fig-068", + "fig-070", + "fig-071" ], "tiofene": [ "fig-021", @@ -7751,14 +7855,14 @@ "fig-015", "fig-045", "fig-050", - "fig-058", "fig-059", "fig-060", - "fig-067", - "fig-074" + "fig-061", + "fig-068", + "fig-075" ], "velocita-di-scansione": [ - "fig-070" + "fig-071" ], "williamson": [ "fig-047" @@ -7777,12 +7881,13 @@ "fig-x-136800", "fig-044", "fig-049", - "fig-057", - "fig-061", + "fig-052", + "fig-058", 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zQ50P`pU4P#%zc!xwixEsG;mmqo&fdR?aYYmQO#De#s^pyG~5NScDPft)pUl3$nZpP z@2sEgt#L6%B?T0rqx8qNczrs~X4@%LX;0b9Z$LU8y;`?R_ZCprbPz4Fq&F-Q{)<6_F^!;920)fv5KrKeomPZ4D{vIA@zQ zGl_rJe^m>?{L{};)KSR0af^3ZX;C5f>o17G_lgt_>>Hd3DZjq?YdXu5Ebw&YSd>|~ ziGD#AXcx_+NAsx-%TD-zVCm4`8916$Kz_@5xpTI5YjJUfvp}2l<`w^6Z?!l|MXDk^ zXwWtfF#v<@b$Rx`<#VJw;<&V~Emc_}-(fjhvyBj6w|7J%HmbvC$E|O)<6P^tzaBQ) z*@re!;wb+upEU`>2MjAhZ-$z9W2lX>v7`ialiM;U%w|5-0{pBu+2FLgJy0LY#l3hVPJ1S={Ra^|7 zvCPq?tT{VivAAi3I^qk*Slu<96jG<>#Qj$8g27nhmjLf+b0!8MDhrB|jZ#SH$7dl}n)P0#e?44!Tb;$OFSa z0o`U6hTD6uqxzzXST$(OJRqTc8UkhkSnsNQaE6vJ<)Y6KH-iygN0>x4BX&k97%-|F zt#FThE$Uc9CH!H3ZsJ^l1pOgpzc1;lmk;b~-CB&t zPV~1(`2c5*(@5#M#`d^(<5W0YGXP0{{R3 literal 0 HcmV?d00001 diff --git a/raw/tesi.md b/raw/tesi.md index 01adcfa..09ce787 100644 --- a/raw/tesi.md +++ b/raw/tesi.md @@ -106,7 +106,7 @@ Come è possibile osservare in **Tabella 1**, l'aggiunta progressiva di amminoci | A | B | Zn | 1 | 5 | 4 | 3 | | --- | --- | --- | --- | --- | --- | --- | | 1 | 1 | 1 | 0 | 100 | - | - | -| 1 | 1 | 1 | 0,2 | 60 | 35 | ⁓5 | +| 1 | 1 | 1 | 0.2 | 60 | 35 | ⁓5 | | 1 | 1 | 1 | 1 | ⁓5 | 85 | 10 | **Tabella 1** - *descrizione degli esperimenti di crossover e risultati espressi in rapporto molare* @@ -163,7 +163,7 @@ Un'attenta ottimizzazione del processo sintetico ha permesso di massimizzare la ![](immagini/d930a8d7b48446faf3acb4839a5330e3cf9dbf19e1ba59b5cdac9da94addf461.jpg) -**Figura 9** - *sintesi del DPP3 proposta da Closs e Gompper* +**Figura 9** - *sintesi del DPP3 proposta da Gloss e Gompper* Una variante metodologica all'approccio classico, anche questo descritto da Iqbal et al.[5](#ref-5), prevede il passaggio attraverso i tetraidrodichetopirrolopirroli, i quali vengono sottoposti a un processo di deidrogenazione per generare il nucleo DPP finale. Il reagente selezionato per promuovere quest'ultima fase è solitamente il DDQ (2,3-dicloro-5,6-dicianobenzochinone). @@ -298,7 +298,7 @@ Una delle reazioni più utili per le successive funzionalizzazioni è la bromura La sintesi dei DPP **32**, **33** e **34** è difficile da realizzare mediante il metodo che sfrutta gli esteri succinici combinati con i corrispondenti nitrili: questo è dovuto al fatto che, in condizioni fortemente basiche, gli atomi di bromo in questi nitrili subiscono facilmente sostituzione nucleofila, riducendo le rese e complicando il processo di purificazione dei prodotti desiderati. -Il gruppo di ricerca di Gryko et al.[7](#ref-7) ha proposto un diverso esempio di sostituzione elettrofila aromatica: i DPP con sostituenti aromatici elettron-ricchi possono essere alchilati in DMF usando K2CO3 come base e tetrabutilammonio bisolfato (TBAHS) come catalizzatore a trasferimento di fase (**Figura 22**). Questa reazione porta alla formazione di diacetali (**35**) che possono essere trasformati nei rispettivi derivati carbonilici mediante un acido forte di Brønsted, attivando quindi una reazione di ciclizzazione elettrofila da parte dell'anello aromatico elettron-ricco adiacente. In questo modo sono riusciti ad ottenere dei pigmenti composti da almeno sei anelli fusi π coniugati con particolari caratteristiche fotofisiche (**36**). +Il gruppo di ricerca di Gryko et al.[7](#ref-7) ha proposto un diverso esempio di sostituzione elettrofila aromatica: i DPP con sostituenti aromatici elettron-ricchi possono essere alchilati in DMF usando K2CO3 come base e tetrabutilammonio bisolfato (TBAHS) come catalizzatore a trasferimento di fase (**Figura 22**). Questa reazione porta alla formazione didiacetali (**35**) che possono essere trasformati nei rispettivi derivati carbonilici mediante un acido forte di Brønsted, attivando quindi una reazione di ciclizzazione elettrofila da parte dell'anello aromatico elettron-ricco adiacente. In questo modo sono riusciti ad ottenere dei pigmenti composti da almeno sei anelli fusi π coniugati con particolari caratteristiche fotofisiche (**36**). ![](immagini/1d7d62195b9dfac2fc36ce6c359e0d5ed64e249c8967e57beb30b7fa6135e67c.jpg) @@ -408,7 +408,7 @@ L'efficienza dell'emissione fluorescente dipende dunque in gran parte dalla stru ![](immagini/ba021605d4b365536a686cb2f71f1c58ea2d5f5b9f962692d596f7a5a3d05ac7.jpg) ![](immagini/8047b55e3609435acd325d3602705c73a5308dc9b407322726ea6a1dde74af65.jpg) -**Figura 33** - *stati elettronici per molecole rigide e flessibili* +**Figura 33** - *Stati elettronici per molecole rigide e flessibili* Nelle molecole poco flessibili, infatti, la geometria dello stato fondamentale e quella dello stato eccitato non presentano distorsioni significative; questo riduce significativamente la probabilità che l'energia assorbita venga dissipata sotto forma di calore attraverso movimenti vibrazionali. Di conseguenza, l'energia dello stato eccitato viene rilasciata quasi interamente sotto forma di luce. Le strutture molecolari ideali per massimizzare questo effetto sono quelle che presentano pochi gradi di libertà, come i sistemi coniugati e i composti aromatici. I dichetopirrolopirroli rientrano perfettamente in questa categoria: grazie al loro scheletro molecolare planare e al vasto sistema di elettroni delocalizzati, il rilassamento vibrazionale è fortemente limitato[34](#ref-34). @@ -482,7 +482,7 @@ L'inserimento di fluorofori all'interno di un sistema macromolecolare richiede u ![](immagini/84a75adb472bc4fd46a5f6d27b0f8d6a3f709b8d073d033aeddaba16c2173b7e.png) -**Figura 35** - *sistemi polimerici con inserimento di fluorofori, in verde il polimero e in rosso le unità di fluoroforo* +**Figura 35** - *sistemi polimerici con inserimento di fluorofori, in verde il polimero e in rosso le unità di fluoroforo,* *a: sistema host-guest, b: sistema main-chain, c: sistema side-chain, d: sistema cross-linked* @@ -503,7 +503,7 @@ Per ovviare al problema della mobilità delle catene polimeriche, che nel tempo Negli ultimi anni, i derivati del dichetopirrolopirrolo (DPP) hanno ampiamente trasceso il loro impiego originario come pigmenti commerciali, affermandosi in una vasta gamma di campi tecnologici avanzati che spaziano dai transistor organici a effetto di campo (OFET), al fotovoltaico, fino alle sonde fluorescenti per il bioimaging. -Tra queste molteplici applicazioni, l'impiego del DPP ha assunto una rilevanza cruciale nel settore dell'optoelettronica organica; grazie all'elevata stabilità termica e fotochimica, unita a un nucleo fortemente elettron-deficiente, questo cromoforo è diventato un elemento chiave per la progettazione di semiconduttori innovativi e dispositivi a emissione di luce.[44](#ref-44) +Tra queste molteplici applicazioni, l'impiego del DPP ha assunto una rilevanza cruciale nel settore dell'optoelettronica organica; grazie all'elevata stabilità termica e fotochimica, unita a un nucleo fortemente elettron-povero, questo cromoforo è diventato un composto chiave per la progettazione di semiconduttori innovativi e dispositivi a emissione di luce.[44](#ref-44) L'optoelettronica comprende lo studio e lo sviluppo di dispositivi basati sull'interazione tra la radiazione elettromagnetica e i materiali semiconduttori, con lo scopo di ottenere la conversione di segnali elettrici in fotoni, come nei diodi a emissione di luce (OLED), o viceversa, come nel caso delle celle fotovoltaiche (OSC) e dei fotorivelatori (**Figura 36**). @@ -511,19 +511,19 @@ L'optoelettronica comprende lo studio e lo sviluppo di dispositivi basati sull'i **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)* -Storicamente, questo settore tecnologico è stato dominato dall'impiego di semiconduttori inorganici rigidi, caratterizzati da reticoli cristallini altamente ordinati quali il silicio.[45](#ref-45) +Storicamente, questo settore tecnologico è stato dominato dall'impiego di semiconduttori inorganici rigidi, caratterizzati da reticoli cristallini altamente ordinati come il silicio.[45](#ref-45) -Tuttavia, negli ultimi decenni, la ricerca si è orientata in modo significativo verso lo sviluppo dell'optoelettronica organica, che sfrutta le proprietà chimico-fisiche di piccole molecole e polimeri con estesi sistemi π-coniugati. L'impiego di materiali organici in sostituzione delle tradizionali controparti inorganiche offre una serie di vantaggi tecnologici. Tra i principali punti di forza spiccano la notevole leggerezza e la flessibilità meccanica, che consentono l'integrazione di tali semiconduttori in dispositivi deformabili o pieghevoli, spaziando dai display di nuova generazione fino all'elettronica indossabile (wearable electronics).[46](#ref-46) Inoltre, da un punto di vista chimico e ingegneristico, uno dei vantaggi più rilevanti risiede nella processabilità di questi materiali. A differenza del silicio, i polimeri coniugati possono essere depositati da soluzione a basse temperature impiegando tecniche ad alta resa e a basso costo, quali la deposizione per spin-coating o processi di stampa su larga scala. Questo approccio garantisce una drastica riduzione dei costi operativi rispetto ai complessi processi ad alta temperatura o in alto vuoto richiesti dalla tecnologia inorganica, promuovendo contestualmente un minor impatto ambientale e aprendo la strada a un'elettronica scalabile e sostenibile. +Tuttavia, negli ultimi decenni, la ricerca si è orientata in modo significativo verso lo sviluppo dell'optoelettronica organica, che sfrutta le proprietà chimico-fisiche di molecole a basso peso molecolare e polimeri con estesi sistemi π-coniugati. L'impiego di materiali organici in sostituzione delle tradizionali controparti inorganiche offre una serie di vantaggi tecnologici. Tra i principali punti di forza spiccano la notevole leggerezza e la flessibilità meccanica, che consentono l'integrazione di tali semiconduttori in dispositivi deformabili o pieghevoli, spaziando dai display di nuova generazione fino all'elettronica indossabile (wearable electronics).[46](#ref-46) Inoltre, da un punto di vista chimico e ingegneristico, uno dei vantaggi più rilevanti risiede nella processabilità di questi materiali. A differenza del silicio, i polimeri coniugati possono essere depositati da soluzione a basse temperature impiegando tecniche ad alta resa e a basso costo, quali la deposizione per spin-coating o processi di stampa su larga scala. Questo approccio garantisce una drastica riduzione dei costi operativi rispetto ai complessi processi ad alta temperatura o in alto vuoto richiesti dalla tecnologia inorganica, promuovendo contestualmente un minor impatto ambientale e aprendo la strada a un'elettronica scalabile e sostenibile. -Affinché tali materiali polimerici processabili possano essere impiegati efficacemente nei dispositivi optoelettronici, risulta indispensabile poter governare in modo preciso le loro proprietà ottiche ed elettroniche. Questo si traduce nella necessità di ingegnerizzare il band gap del materiale.[47](#ref-47) Negli attuali semiconduttori organici, la strategia sintetica d'elezione per ottenere un controllo accurato di tale parametro è l'approccio donatore-accettore (D-A). Questa architettura macromolecolare si basa sulla copolimerizzazione alternata di unità strutturali fortemente elettron-deficienti (accettori) e unità elettron-ricche (donatori) lungo lo scheletro $\pi$ -coniugato.[48](#ref-48) L'interazione tra questi due blocchi monomerici induce un'ibridazione dei rispettivi orbitali di frontiera: il livello HOMO del copolimero risultante è determinato principalmente dalla porzione elettron-donatrice, mentre il livello LUMO è governato dall'unità elettron-accettrice. Questo riposizionamento energetico intracatena promuove un marcato trasferimento di carica intramolecolare, il quale comporta una drastica riduzione del salto energetico e consente di centrare lo spettro di assorbimento e di emissione del polimero all'interno della regione visibile. [49](#ref-49) +Affinché tali materiali polimerici processabili possano essere impiegati efficacemente nei dispositivi optoelettronici, risulta indispensabile poter governare in modo preciso le loro proprietà ottiche ed elettroniche. Questo si traduce nella necessità di ingegnerizzare il band gap del materiale.[47](#ref-47) Negli attuali semiconduttori organici, la strategia sintetica d'elezione per ottenere un controllo accurato di tale parametro è l'approccio donatore-accettore (D-A). Questa architettura macromolecolare si basa sulla copolimerizzazione alternata di unità strutturali fortemente elettron-povere (accettori) e unità elettron-ricche (donatori) lungo lo scheletro $\pi$ -coniugato.[48](#ref-48) L'interazione tra questi due blocchi monomerici induce un'ibridazione dei rispettivi orbitali di frontiera: il livello HOMO del copolimero risultante è determinato principalmente dalla porzione elettron-donatrice, mentre il livello LUMO è governato dall'unità elettron-accettrice. Questo riposizionamento energetico intracatena promuove un marcato trasferimento di carica intramolecolare, il quale comporta una drastica riduzione del salto energetico e consente di centrare lo spettro di assorbimento e di emissione del polimero all'interno della regione visibile. [49](#ref-49) -Nel caso specifico delle architetture polimeriche sviluppate in questo progetto di tesi, il nucleo fortemente elettron-accettore del dichetopirrolopirrolo è stato combinato con unità di 3-esiltiofene (3HT), impiegate per il loro spiccato carattere elettron-donatore. L'introduzione del monomero tiofenico non solo funge da partner elettronico ideale per ibridare gli orbitali di frontiera del DPP, ma, grazie alla presenza della catena alchilica laterale esilica, garantisce anche l'adeguata solubilità della macromolecola finale, preservandone la processabilità.[49](#ref-49) +Nel caso specifico delle architetture polimeriche sviluppate in questo progetto di tesi, il nucleo fortemente elettron-accettore del dichetopirrolopirrolo è stato combinato con unità di 3-esiltiofene (3HT), impiegate per il loro spiccato carattere elettron-donatore. L'introduzione del monomero tiofenico non solo funge da partner elettronico ideale per ibridare gli orbitali di frontiera del DPP, ma, grazie alla presenza della catena alchilica laterale, garantisce anche l'adeguata solubilità della macromolecola finale, preservandone la processabilità.[49](#ref-49) -La sinergia donatore-accettore (D-A) instaurata tra il nucleo di DPP e l'unità di 3HT permette di sintonizzare la struttura a bande del materiale, conferendogli i requisiti optoelettronici ottimali per un potenziale impiego come strato elettro-luminescente nei dispositivi OLED. +La sinergia donatore-accettore (D-A) instaurata tra il nucleo di DPP e l'unità di 3HT permette di sintonizzare la struttura a bande del materiale, conferendogli i requisiti ottimali per un potenziale impiego come strato elettro-luminescente nei dispositivi OLED. Affinché le proprietà ottiche ed elettroniche dei polimeri D-A possano essere sfruttate tecnologicamente, è necessario implementare questi materiali all'interno di dispositivi a stato solido. Un diodo organico a emissione di luce (OLED) si basa su una complessa architettura multistrato, progettata con estrema precisione per ottimizzare l'iniezione, il trasporto e la ricombinazione delle cariche elettriche. Storicamente, i primi dispositivi organici a singolo strato presentavano efficienze estremamente ridotte a causa di un forte sbilanciamento tra la mobilità degli elettroni e quella delle lacune. Per ovviare a questo problema, i moderni OLED impiegano una struttura a sandwich comprendente molteplici film sottili specializzati. -Il cuore del dispositivo è costituito dallo strato emissivo (EML, Emissive Layer) interposto tra due elettrodi asimmetrici. Da un lato, il dispositivo è delimitato da un anodo trasparente, tipicamente costituito da ossido di indio-stagno (ITO), caratterizzato da un elevato lavoro di estrazione e trasparente alla luce visibile; dall'altro lato, è presente un catodo metallico a basso lavoro di estrazione, come leghe di alluminio, calcio o bario. +Il cuore del dispositivo è costituito dallo strato emissivo (EML, Emissive Layer) interposto tra due elettrodi asimmetrici. Da un lato, il dispositivo è delimitato da un anodo trasparente, tipicamente costituito da ossido di indio-stagno (ITO), caratterizzato da un elevato lavoro di estrazione, ovvero di un'alta quantità di energia per espellere un elettrone dalla sua superficie, e trasparente alla luce visibile; dall'altro lato, è presente un catodo metallico a basso lavoro di estrazione, come leghe di alluminio, calcio o bario, il quale permette invece di cedere facilmente elettroni verso lo strato emissivo. Per abbassare le barriere energetiche all'interfaccia tra gli elettrodi e il polimero luminescente, vengono frapposti degli strati ausiliari denominati HTL (Hole Transport Layer) ed ETL (Electron Transport Layer) (**Figura 37**). @@ -576,7 +576,7 @@ I prodotti sono stati caratterizzati per spettroscopia infrarossa a riflettanza I polimeri ottenuti sono stati caratterizzati per Gel Permeation Cromatography (GPC) in modo da determinare i loro pesi molecolari. Le analisi sono state effettuate impiegando una colonna del tipo 5MXL da 300 mm in grado di analizzare un range di Mw compreso tra 800-30000 Da. Lo strumento impiega un detector ad indice di rifrazione. I campioni sono stati solubilizzati in THF e l'analisi è stata eseguita con una velocità di flusso di 1 mL/min ad una temperatura di 20 °C. La calibrazione della colonna è stata effettuata mediante standard monodispersi di polistirene. -Le analisi UV-Vis sono state eseguite con uno spettrofotometro a doppio raggio "Agilent Cary 3500 UV-Vis" acquisendo uno spettro da 800 a 200 nm usando cuvette di quarzo con un cammino ottico di 1 cm. +Le analisi UV-VIS sono state eseguite con uno spettrofotometro a doppio raggio "Agilent Cary 3500 UV-Vis" acquisendo uno spettro da 800 a 200 nm usando cuvette di quarzo con un cammino ottico di 1 cm. Le misure di fluorescenza sono state svolte con uno spettrometro Agilent Cary Eclipse, avente come sorgente una lampada allo xenon (80 Hz) e come detector un fotomoltiplicatore PMT 900. @@ -599,11 +599,11 @@ Il prodotto **1** si presenta come un solido rosso scuro/violaceo. *Caratterizzazione del prodotto* **1** -**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) +**1H NMR** (400 MHz, d6-DMSO): δ = 11.23 – 11.18 (s, 2H), 8.28 – 8.22 (dd, *J* = 3.7, 1.3 Hz, 2H), 7.98 – 7.91 (dd, *J* = 5.0, 1.1 Hz, 2H), 7.36 – 7.22 (m, 2H) **UV-Vis** (in THF): 532 nm, 498 nm -**Fluorescenza** (in THF): 490 nm +**Fluorescenza** (in THF): λem = 543 nm; λecc = 490 nm ***Sintesi del 2,5-bis(6-idrossiesil)-3,6-di(tiofen-2-il)-2,5-diidropirrolo[3,4-c]pirrolo-1,4-dione (2)*** @@ -617,13 +617,13 @@ Il grezzo di reazione viene purificato mediante cristallizzazione in etanolo: il *Caratterizzazione del prodotto* **2** -**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) +**1H NMR** (400 MHz, CDCl3): δ 8.94 – 8.83 (m, 2H), 7.66 – 7.57 (m, 2H), 7.33 – 7.17 (m, 2H), 4.14 – 4.05 (m, 4H), 3.72 – 3.59 (td, *J* = 6.5, 2.3 Hz, 4H), 3.43 – 3.31 (t, *J* = 6.5 Hz, 2H), 1.85 – 1.71 (q, *J* = 7.3 Hz, 4H), 1.62 – 1.35 (t, *J* = 6.4 Hz, 12H). **IR** (ATR): 3350, 3070, 2920, 2850, 1645, 1555, 1495, 1440, 1390, 820, 730 cm⁻¹ **UV-Vis** (in THF): 541 nm -**Fluorescenza** (in THF): 540 nm +**Fluorescenza** (in THF): λem = 555 nm; λecc = 540 nm ***Sintesi dei copolimeri coniugati (3a, 3b, 3c)*** @@ -631,32 +631,29 @@ Il grezzo di reazione viene purificato mediante cristallizzazione in etanolo: il Sono stati sintetizzati tre copolimeri in base alla percentuale di DPP utilizzata (**Tabella 3**). -| 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 | +| Copolimero | Rapporto molare DPP:3HT | +| --- | --- | +| 3a | 20:80 | +| 3b | 50:50 | +| 3c | 80:20 | **Tabella 3** - *composizione dei copolimeri* -La procedura sperimentale risulta analoga per ognuno dei copolimeri sintetizzati. In un pallone a tre colli posto in atmosfera d'azoto, vengono aggiunti 40 mL di cloroformio anidro (CHCl3) ed i due monomeri nelle proporzioni corrette. La completa solubilizzazione del prodotto **2** viene favorita mediante sonicatore. In parallelo, si prepara una soluzione di 818 mg di tricloruro ferrico (FeCl3) (5,05 mmol, 5 eq) in 10 mL di nitrometano (CH3NO2), lasciandola anch'essa in sonicatore per alcuni minuti per agevolarne la dissoluzione. La soluzione ossidante viene sgocciolata nel pallone mantenendo il sistema in agitazione per 1 h. Al termine, si aggiungono 30 mL di THF sbiancato e si lascia nuovamente in agitazione per 30 min. +La procedura sperimentale risulta analoga per ognuno dei copolimeri sintetizzati. In un pallone a tre colli posto in atmosfera d'azoto, vengono aggiunti 40 mL di cloroformio anidro (CHCl3) ed i due monomeri nelle proporzioni corrette. La completa solubilizzazione del prodotto **2** viene favorita mediante sonicatore. In parallelo, si prepara una soluzione di 818 mg di tricloruro ferrico (FeCl3) (5.05 mmol, 5 eq) in 10 mL di nitrometano (CH3NO2), lasciandola anch'essa in sonicatore per alcuni minuti per agevolarne la dissoluzione. La soluzione ossidante viene sgocciolata nel pallone mantenendo il sistema in agitazione per 1 h. Al termine, si aggiungono 30 mL di THF sbiancato e si lascia nuovamente in agitazione per 30 min. -Successivamente, si trasferisce il grezzo di reazione in imbuto separatore e si lava con HCl 0,6 M finché la fase acquosa sottoposta al saggio con tiocianato non risulta trasparente (la persistenza del colore rosso indica la presenza di tracce residue di tricloruro ferrico; il test si esegue a partire dal terzo lavaggio). La fase organica viene estratta con una soluzione satura di NaCl in acqua, anidrificata e evaporata mediante rotavapor. Per separare il polimero dai possibili sottoprodotti (poli-3esiltiofene) e dalle molecole a basso peso molecolare viene effettuata una precipitazione in non-solvente. Il prodotto viene solubilizzato nella minima quantità di THF e si fa gocciolare in 150 mL di metanolo freddo. Il precipitato viene filtrato e la soluzione portata a secco mediante l'utilizzo del rotavapor. +Successivamente, si trasferisce il grezzo di reazione in imbuto separatore e si lava con HCl 0.6 M finché la fase acquosa sottoposta al saggio con tiocianato non risulta trasparente (la persistenza del colore rosso indica la presenza di tracce residue di tricloruro ferrico; il test si esegue a partire dal terzo lavaggio). La fase organica viene estratta con una soluzione satura di NaCl in acqua, anidrificata e evaporata mediante rotavapor. Per separare il polimero dai possibili sottoprodotti (poli-3esiltiofene) e dalle molecole a basso peso molecolare viene effettuata una precipitazione in non-solvente. Il prodotto viene solubilizzato nella minima quantità di THF e si fa gocciolare in 150 mL di metanolo freddo. Il precipitato viene filtrato e la soluzione portata a secco mediante l'utilizzo del rotavapor. ***Sintesi dei polimeri bottle brush*** ![](immagini/136800375cf0b441570672093e255d90a47c45a009bd254929fb74b1f17b382d.jpg) -A partire dai campioni **3b** e **3c** sono stati realizzati copolimeri con struttura bottle brush a diverso peso molecolare. La quantità di $\varepsilon$ -caprolattone necessaria per l'innesto dei blocchi di PCL è stata determinata impostando il rapporto stechiometrico in funzione degli equivalenti di gruppi -OH del derivato DPP, considerandoli come iniziatori attivi per la ROP. +A partire dai campioni **3b** e **3c** sono stati realizzati copolimeri con struttura bottle-brush a diverso peso molecolare. La quantità di $ε$-caprolattone necessaria per l'innesto dei blocchi di PCL è stata determinata impostando il rapporto stechiometrico in funzione degli equivalenti di gruppi -OH del derivato DPP, considerandoli come iniziatori attivi per la ROP. -| Copolimero | Mn teorico | Caprolattone V (ml) | Caprolattone mol | +| Mn teorico | Rapporto molare copolimero:PLC | Copolimero 3b | Copolimero 3c | | --- | --- | --- | --- | -| 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 | +| 1500 Da | 1:20 | **3.1b** | **3.1c** | +| 5000 Da | 1:88 | **3.2b** | **3.2c** | +| 10000 Da | 1:175 | **3.3b** | **3.3c** | **Tabella 4** - *composizione dei polimeri bottle brush* @@ -691,7 +688,7 @@ Invertendo poi il potenziale applicato, le specie generate all'elettrodo durante Per un sistema diffusivo ideale e reversibile, il valore della corrente di picco in funzione della velocità di scansione è descritto quantitativamente dall'equazione di Randles-Sevcik (**Equazione 8**): $$ -I_{p}=\left(2{,}69\times 10^{5}\right)\cdot n^{3/2}\cdot A\cdot D^{1/2}\cdot C\cdot v^{1/2} +I_{p}=\left(2.69\times 10^{5}\right)\cdot n^{3/2}\cdot A\cdot D^{1/2}\cdot C\cdot v^{1/2} $$ **Equazione 8** - *equazione di Randles-Sevcik* @@ -703,7 +700,7 @@ In questa equazione, $n$ rappresenta il numero di elettroni scambiati nella reaz Le caratterizzazioni elettrochimiche sono state condotte a temperatura ambiente impiegando un potenziostato CHI660C (CH Instruments), interfacciato con una cella elettrochimica standard a tre elettrodi. Il sistema era costituito da un elettrodo di lavoro in glassy carbon (carbonio vetroso), un elettrodo di riferimento ad Ag/AgCl e un controelettrodo costituito da un filo di platino. -Tutte le misurazioni sono state eseguite in fase omogenea, utilizzando tetraidrofurano (THF) come solvente. Come elettrolita di supporto è stato impiegato il tetrabutilammonio esafluorofosfato (TBAPF6) ad una concentrazione di 0,1 M. Prima di procedere all'analisi dei materiali sintetizzati, è stata registrata la ciclovoltammetria del bianco sulla sola soluzione elettrolitica, al fine di verificare la pulizia del sistema e l'assenza di specie elettroattive interferenti all'interno della finestra di potenziale indagata. Successivamente, la soluzione è stata utilizzata per la preparazione delle soluzioni polimeriche a una concentrazione fissa di 10 mg/mL. +Tutte le misurazioni sono state eseguite in fase omogenea, utilizzando tetraidrofurano (THF) come solvente. Come elettrolita di supporto è stato impiegato il tetrabutilammonio esafluorofosfato (TBAPF6) ad una concentrazione di 0.1 M. Prima di procedere all'analisi dei materiali sintetizzati, è stata registrata la ciclovoltammetria del bianco sulla sola soluzione elettrolitica, al fine di verificare la pulizia del sistema e l'assenza di specie elettroattive interferenti all'interno della finestra di potenziale indagata. Successivamente, la soluzione è stata utilizzata per la preparazione delle soluzioni polimeriche a una concentrazione fissa di 10 mg/mL. ![](immagini/7454f0793d62db92121d98aa27815bc85d5aae9f16807d3f188d7feb1ee83463.jpg) @@ -711,7 +708,7 @@ Tutte le misurazioni sono state eseguite in fase omogenea, utilizzando tetraidro Inizialmente la soluzione è stata sottoposta a degasaggio tramite gorgogliamento di azoto, per rimuovere tutto l'ossigeno disciolto che potrebbe interferire con le analisi riducendosi al catodo. Successivamente, il flusso di azoto dentro la soluzione è stato rimosso per evitare perturbazioni meccaniche all'interfaccia elettrodo/soluzione durante le misure, mantenendolo solo come battente per impedire l'ingresso di ossigeno nella cella. -Le scansioni voltammetriche di base per l'identificazione dei processi redox sono state registrate applicando una velocità di scansione di 0,05 V/s, variando in seguito le velocità di scansione (0.05, 0.1, 0.5 e 1.0 V/s) per investigare l'influenza della cinetica di trasferimento. Al termine delle misurazioni per ciascun campione, è stata aggiunta una piccola quantità di ferrocene direttamente nella cella elettrochimica per fungere da standard redox interno, in quanto i potenziali misurati sperimentalmente sono relativi e strettamente dipendenti dal particolare elettrodo di riferimento impiegato. Sfruttando il comportamento reversibile e il potenziale noto della coppia redox Fc/Fc+, è stato possibile calibrare l'asse dei potenziali e riferire i valori di onset sperimentali alla scala assoluta delle energie nel vuoto, passaggio indispensabile per un calcolo rigoroso dei livelli energetici HOMO e LUMO dei materiali.[50](#ref-50) +Le scansioni voltammetriche di base per l'identificazione dei processi redox sono state registrate applicando una velocità di scansione di 0.05 V/s, variando in seguito le velocità di scansione (0.05, 0.1, 0.5 e 1.0 V/s) per investigare l'influenza della cinetica di trasferimento. Al termine delle misurazioni per ciascun campione, è stata aggiunta una piccola quantità di ferrocene direttamente nella cella elettrochimica per fungere da standard redox interno, in quanto i potenziali misurati sperimentalmente sono relativi e strettamente dipendenti dal particolare elettrodo di riferimento impiegato. Sfruttando il comportamento reversibile e il potenziale noto della coppia redox Fc/Fc+, è stato possibile calibrare l'asse dei potenziali e riferire i valori di onset sperimentali alla scala assoluta delle energie nel vuoto, passaggio indispensabile per un calcolo rigoroso dei livelli energetici HOMO e LUMO dei materiali.[50](#ref-50) # 4 **Discussione dei risultati** @@ -727,7 +724,7 @@ Il gruppo di ricerca all'interno del quale è stato svolto il lavoro di tesi si **Figura 40** - *sostituenti del DPP precedentemente studiati dal gruppo di ricerca* -L'impiego di benzonitrili con sostituenti in *para* di tipo EWG porta alla formazione di sistemi altamente emissivi; al contrario, la presenza di gruppi EDG porta alla formazione di un isomero strutturale (iso-DPP) in cui la fluorescenza nel visibile risulta inibita principalmente a causa dell'attivazione di processi di rilassamento non radiativo. +L'impiego di benzonitrili con sostituenti in *para* di tipo EWG porta alla formazione di sistemi altamente emissivi; al contrario, la presenza di gruppi EDG porta alla formazione di un isomero strutturale (iso-DPP) in cui la fluorescenza nel visibile risulta inibita principalmente a causa dell'attivazione di processi di rilassamento non radiativo.[51](#ref-51) Questo studio iniziale ha garantito solide fondamenta riguardo i possibili fluorofori da utilizzare in successive reazioni di polimerizzazione, sulla base di fattori come proprietà emissive e loro reattività. @@ -765,7 +762,7 @@ Nella regione a circa 11 ppm si osserva un singoletto allargato attribuibile ai ![](immagini/ba9fb099eb33d86ffd10e40efffc19c6100dc56af328b2442f186b51e09433be.jpg) -**Figura 45** - *spettro UV-Visibile e di emissione del prodotto 1 in THF* +**Figura 45** - *spettro UV-Visibile e di emissione del prodotto 1 in THF (λex:490 nm)* Dall'analisi dello spettro UV-visibile del prodotto **1** è possibile osservare una banda di assorbimento ben definita, con due massimi a lunghezze d'onda pari a circa 532 nm e 498 nm, caratteristici del sistema coniugato e planare del core dichetopirrolopirrolico. Lo spettro di emissione risulta essere pressoché simmetrico con quello di assorbimento, presentando un massimo principale a 543 nm e una spalla secondaria a circa 585 nm. È inoltre interessante notare uno Stokes Shift di soli 11 nm, indice del fatto che l'elevata rigidità molecolare del sistema minimizza i riarrangiamenti strutturali tra stato fondamentale ed eccitato, limitando così i decadimenti non radiativi in seguito all'eccitazione. @@ -793,7 +790,7 @@ Il prodotto è stato purificato per cristallizzazione, una tecnica che sfrutta l **Figura 48** - *spettro 1H-NMR in CDCl3 del prodotto 2* -Nella regione aromatica dello spettro 1H-NMR, riportato in **Figura 48**, si osservano chiaramente tre distinti segnali assegnabili ai protoni degli anelli tiofenici. Il segnale più indicativo è rappresentato da un doppietto a campi particolarmente bassi (circa 8,9 ppm), attribuibile ai protoni fortemente deschermati per effetto dei gruppi carbonilici adiacenti del core DPP. Gli altri due protoni tiofenici completano il pattern generando gli altri due segnali separati a campi progressivamente più alti (7,6 ppm e 7,3 ppm). L'avvenuta reazione di N-alchilazione è comprovata, nella regione alifatica, dalla comparsa di due multipletti: il segnale più deschermato (4,1 ppm) è relativo ai gruppi metilenici legati direttamente all'azoto lattamico, mentre il secondo (3,6 ppm) corrisponde ai metileni adiacenti all'ossidrile terminale. Infine, i restanti protoni metilenici della catena alifatica sono chiaramente visibili sotto forma di multipletti nella regione compresa tra 1 e 2 ppm. +Nella regione aromatica dello spettro 1H-NMR, riportato in **Figura 48**, si osservano chiaramente tre distinti segnali assegnabili ai protoni degli anelli tiofenici. Il segnale più indicativo è rappresentato da un doppietto a campi particolarmente bassi (circa 8.9 ppm), attribuibile ai protoni fortemente deschermati per effetto dei gruppi carbonilici adiacenti del core DPP. Gli altri due protoni tiofenici completano il pattern generando gli altri due segnali separati a campi progressivamente più alti (7.6 ppm e 7.3 ppm). L'avvenuta reazione di N-alchilazione è comprovata, nella regione alifatica, dalla comparsa di due multipletti: il segnale più deschermato (4.1 ppm) è relativo ai gruppi metilenici legati direttamente all'azoto lattamico, mentre il secondo (3.6 ppm) corrisponde ai metileni adiacenti all'ossidrile terminale. Infine, i restanti protoni metilenici della catena alifatica sono chiaramente visibili sotto forma di multipletti nella regione compresa tra 1 e 2 ppm. ![](immagini/f890cc2c6264ef44ec1b471578277dc04114da1baa30e1f6aa17bb7f674615e8.jpg) @@ -805,13 +802,13 @@ Per completare la caratterizzazione, il fluoroforo è stato analizzato mediante ![](immagini/75c7d0cf12baae0fe259352e5495ea053607717f5a57233f468098343f6693c7.jpg) -**Figura 50** - *spettro UV-Visibile e di emissione del prodotto2 in THF* +**Figura 50** - *spettro UV-Visibile e di emissione del prodotto2 in THF (λex:540 nm)* In seguito all'alchilazione si osserva uno spostamento batocromico del massimo di assorbimento, passando da 531 nm nel caso del prodotto **1** a 541 nm del prodotto **2**. Tale fenomeno è riconducibile all'effetto induttivo elettron-donatore delle catene alifatiche, le quali arricchiscono la densità elettronica sugli atomi di azoto determinando una destabilizzazione energetica dell'orbitale HOMO e un conseguente restringimento del bandgap ottico. Lo Stokes shift, invece, è simile per entrambi i fluorofori e vale circa 14 nm. | Prodotto | λmax, abs (nm) | λmax, ex (nm) | Stokes shift (nm) | ε (M-1 cm-1) | | --- | --- | --- | --- | --- | -| 1 | 531 | 542 | 11 | 28000[51](#ref-51) | +| 1 | 531 | 542 | 11 | 28000[52](#ref-52) | | 2 | 541 | 555 | 14 | 13218 | **Tabella 5** - *dati spettroscopici dei fluorofori sintetizzati* @@ -820,38 +817,56 @@ Inoltre, è stato possibile calcolare il coefficiente di estinzione molare ε (M ![](immagini/336837d03a78ea923cf3fa1ae976385b52eefe8ab91dccfdff63f3bb33ecfc6b.jpg) -**Figura 51** - *retta di calibrazione del fluoroforo 2 per il calcolo di ε* +**Figura 51** - *retta di calibrazione del fluoroforo 2 in CHCl3 per il calcolo di ε* + +Successivamente alle analisi spettroscopiche, il monomero è stato sottoposto a voltammetria ciclica (CV) per studiarne il comportamento redox e stimare i livelli energetici di frontiera. + +L'analisi qualitativa del voltammogramma ciclico del prodotto **2** (**Figura 52**) evidenzia un comportamento diverso per i processi di estrazione ed iniezione di carica all'interfaccia elettrodica. + +Durante la scansione anodica, corrispondente al processo di drogaggio di tipo p, si osserva lo sviluppo di un'ampia onda faradica priva di un corrispondente picco di ritorno simmetrico nella scansione inversa, denotando la marcata irreversibilità dell'ossidazione. Tale asimmetria è riconducibile all'instaurarsi di un meccanismo di tipo elettrochimico-chimico (EC): i radicali cationi generati inizialmente risultano altamente instabili e vengono rapidamente consumati da reazioni chimiche secondarie di degradazione, impedendo al sistema di ripristinare il suo stato neutro originario. Al contrario, procedendo verso i potenziali catodici per indagare il drogaggio di tipo n, l'iniezione di elettroni genera un picco di riduzione principale ben definito, a cui fa seguito un'evidente onda di scarica anodica durante la scansione di ritorno. Sebbene si registri anche la presenza di un segnale pre-onda di minore intensità, la chiara comparsa del picco di ritorno indica che la specie radical-anionica transitoria possiede una stabilità chimica nettamente superiore rispetto a quella formata durante il processo ossidativo. + +![](immagini/c43b5f5dac544853f6c17aff18ad43408c4b39ab24ba521cc098fbda40f50699.jpg) + +**Figura 52** - *voltammogramma ciclico del prodotto 2 in soluzione di THF* + +A causa dell'irreversibilità descritta e delle concomitanti cinetiche di reazione che alterano i potenziali di picco, questi ultimi non rappresentano parametri termodinamici affidabili per una rigorosa valutazione energetica del materiale. Pertanto, l'elaborazione quantitativa si è basata sulla determinazione dei potenziali di onset, estratti mediante il metodo grafico dell'intersezione delle tangenti, in quanto approssimano con maggiore accuratezza la minima energia richiesta per innescare i trasferimenti elettronici. A partire dai valori riportati in **Tabella 6**, e dopo aver effettuato una opportuna calibrazione rispetto al potenziale di riferimento del ferrocene, l'applicazione delle equazioni empiriche (**Paragrafo 3.3**) ha consentito di ricavare i livelli energetici assoluti degli orbitali di frontiera. Nello specifico, per il monomero sintetizzato è stato stimato un livello energetico HOMO pari a -5,357 eV e un livello LUMO pari a -3,347 eV, parametri dai quali deriva un bandgap elettrochimico complessivo di 2,01 eV. + +| Prodotto | Eonsetox (V) | Eonsetrid (V) | HOMO (eV) | LUMO (eV) | Bandgap (eV) | +| --- | --- | --- | --- | --- | --- | +| 2 | 0,557 | -1,453 | -5,357 | -3,347 | 2,01 | + +**Tabella 6** - *dati voltammetrici del prodotto 2* ## 4.2 **Copolimeri coniugati** Successivamente alla sintesi e alla caratterizzazione fotofisica del fluoroforo dichetopirrolopirrolico **2**, l'attenzione è stata rivolta alla sua integrazione in sistemi polimerici coniugati. In tale ottica, si è proceduto alla sintesi di copolimeri statistici, facendo reagire questo monomero con il 3-esiltiofene (3HT). -La scelta del 3HT come comonomero è stata guidata dalla collaborazione con il gruppo di ricerca del Prof. Lanzi. L'esperienza pregressa di tale gruppo ha infatti ampiamente convalidato l'efficacia e la versatilità della polimerizzazione ossidativa applicata a questa classe di derivati tiofenici. La scelta di questa specifica via sintetica, inoltre, si giustifica alla luce di diversi vantaggi operativi: a differenza dei tradizionali e più complessi metodi di *cross-coupling* catalizzati da metalli di transizione, la polimerizzazione ossidativa diretta non richiede la pre-funzionalizzazione dei monomeri, diminuendo drasticamente gli step sintetici. Inoltre, richiedendo condizioni termodinamiche blande, temperatura ambiente e pressione atmosferica, il processo si distingue per una notevole semplicità esecutivo ed un basso costo energetico. Tali caratteristiche le conferiscono un grande potenziale di scale-up, aspetto di notevole rilevanza nell'ambito di ricerca di questa tesi. +La scelta del 3HT come comonomero è stata guidata dalla collaborazione con il gruppo di ricerca del Prof. Lanzi. L'esperienza pregressa di tale gruppo ha infatti ampiamente convalidato l'efficacia e la versatilità della polimerizzazione ossidativa applicata a questa classe di derivati tiofenici. La scelta di questa specifica via sintetica, inoltre, si giustifica alla luce di diversi vantaggi operativi: a differenza dei tradizionali e più complessi metodi di *cross-coupling* catalizzati da metalli di transizione, la polimerizzazione ossidativa diretta non richiede la pre-funzionalizzazione dei monomeri, diminuendo drasticamente gli step sintetici. Inoltre, richiedendo condizioni termodinamiche blande, temperatura ambiente e pressione atmosferica, il processo si distingue per una notevole semplicità esecutiva ed un basso costo energetico. Tali caratteristiche le conferiscono un grande potenziale di scale-up, aspetto di notevole rilevanza nell'ambito di ricerca di questa tesi. -Sotto il profilo strutturale e funzionale, la selezione del 3HT è motivata dalle note proprietà elettroniche dei politiofeni, classificati in letteratura tra i più efficienti polimeri semiconduttori organici.[52](#ref-52) L'inserimento di questa unità nella catena polimerica persegue quindi un duplice obiettivo: da un lato, la presenza della catena esilica assicura l'aumento di solubilità del materiale finale nei comuni solventi organici, requisito fondamentale per la successiva processabilità del polimero; dall'altro lato, l'anello tiofenico contribuisce attivamente all'estensione del sistema π-coniugato, agendo in sinergia con gli altri moduli strutturali della catena per modulare il band gap del materiale e ottimizzare le prestazioni di trasporto di carica del polimero semiconduttore. +Sotto il profilo strutturale e funzionale, la selezione del 3HT è motivata dalle note proprietà elettroniche dei politiofeni, classificati in letteratura tra i più efficienti polimeri semiconduttori organici.[53](#ref-53) L'inserimento di questa unità nella catena polimerica persegue quindi un duplice obiettivo: da un lato, la presenza della catena alchidica assicura l'aumento di solubilità del materiale finale nei comuni solventi organici, requisito fondamentale per la successiva processabilità del polimero. Invece, l'anello tiofenico contribuisce attivamente all'estensione del sistema π-coniugato, interagendo con le altre unità costituenti della catena permette di modulare il band gap del materiale e ottimizzare le prestazioni di trasporto di carica del polimero semiconduttore. La reazione di polimerizzazione ossidativa del fluoroforo **2** con il 3HT è stata effettuata secondo lo schema di reazione riportato in **Figura 52**. ![](immagini/0cc72ddb7b8a730785dfaeb2abb381f6ef486e86e068d50b5d0b0ac0e8bc220d.jpg) -**Figura 52** - *schema di reazione dei copolimeri coniugati* +**Figura 53** - *schema di reazione dei copolimeri coniugati* -Il primo stadio del meccanismo di polimerizzazione ossidativa è governato dalla reattività del tricloruro ferrico (FeCl3). In questo caso, il sale inorganico funge da agente ossidante ed è impiegato in eccesso stechiometrico rispetto ai reagenti. Il centro metallico Fe3+ promuove l'attivazione dei monomeri attraverso un processo di trasferimento mono-elettronico (Single Electron Transfer, SET)[53](#ref-53). Durante questa fase, il ferro estrae un elettrone dagli anelli tiofenici dei monomeri, elettron-ricchi di natura, riducendosi a Fe2+. Questa reazione redox porta alla generazione di cationi radicalici fortemente delocalizzati sul sistema π-coniugato dei dichetopirrolopirroli e dei derivati tiofenici. Questi intermedi, altamente reattivi, rappresentano i veri centri attivi della polimerizzazione, che tendono a legarsi per formare i nuovi legami carbonio-carbonio necessari all'accrescimento della catena (**Figura 53**). +Il primo stadio del meccanismo di polimerizzazione ossidativa è governato dalla reattività del tricloruro ferrico (FeCl3). In questo caso, il sale inorganico funge da agente ossidante ed è impiegato in eccesso stechiometrico rispetto ai reagenti. Il centro metallico Fe3+ promuove l'attivazione dei monomeri attraverso un processo di trasferimento mono-elettronico (Single Electron Transfer, SET)[54](#ref-54). Durante questa fase, il ferro estrae un elettrone dagli anelli tiofenici dei monomeri, elettron-ricchi di natura, riducendosi a Fe2+. Questa reazione redox porta alla generazione di cationi radicalici fortemente delocalizzati sul sistema π-coniugato dei dichetopirrolopirroli e dei derivati tiofenici. Questi intermedi, altamente reattivi, rappresentano i veri centri attivi della polimerizzazione, che tendono a legarsi per formare i nuovi legami carbonio-carbonio necessari all'accrescimento della catena (**Figura 53**). ![](immagini/34cdcf9d6836a55ee2dd35ac99f5e80cd9dffb87cbfaf818b5257c5ccfed2b51.jpg) -**Figura 53** - *meccanismo di polimerizzazione ossidativa mediante tricloruro ferrico* +**Figura 54** - *meccanismo di polimerizzazione ossidativa mediante tricloruro ferrico* -Per garantire l'efficienza e il controllo di questa propagazione radicalica, l'impiego del nitrometano (CH3NO2) all'interno della miscela di solventi risulta determinante. Allo stato solido e in solventi non coordinanti come il cloroformio, il FeCl3 tende a formare dimeri o aggregati, nei quali i siti attivi per l'ossidazione sono limitati alla superficie o ai difetti strutturali dei cluster. L'introduzione del nitrometano nella miscela di reazione risolve questa criticità: agendo come legante, esso rompe i ponti alogeno intermolecolari, spezzando i dimeri e solvatando il cloruro ferrico. La formazione di questi complessi di coordinazione con il nitrometano attiva di fatto il sistema, generando una soluzione omogenea di centri metallici discreti e stericamente accessibili per il trasferimento elettronico. Parallelamente, la coordinazione del ferro con il nitrometano ne modera sensibilmente sia la forte acidità di Lewis che il potenziale ossidante. Questa azione attenuatrice è essenziale per indirizzare la cinetica di reazione: controllando la forza dell'ossidante, si prevengono reazioni secondarie come l'iper-ossidazione della catena o l'insorgere di difetti di reticolazione (cross-linking). Di conseguenza si migliora la regioselettività della polimerizzazione, massimizzando la regolarità strutturale e l'estensione della π-coniugazione nel copolimero semiconduttore **3** sintetizzato. +Per garantire l'efficienza e il controllo della propagazione radicalica, l'impiego del nitrometano (CH3NO2) all'interno della miscela di solventi risulta determinante. Allo stato solido e in solventi non coordinanti come il cloroformio, il FeCl3 tende a formare dimeri o aggregati, nei quali i siti attivi per l'ossidazione sono limitati alla superficie o ai difetti strutturali dei cluster. L'introduzione del nitrometano nella miscela di reazione risolve questa criticità: agendo come legante, esso rompe i ponti alogeno intermolecolari, spezzando i dimeri e solvatando il cloruro ferrico. La formazione di questi complessi di coordinazione con il nitrometano attiva di fatto il sistema, generando una soluzione omogenea di centri metallici discreti e stericamente accessibili per il trasferimento elettronico. Parallelamente, la coordinazione del ferro con il nitrometano ne modera sensibilmente sia la forte acidità di Lewis che il potenziale ossidante. Questa azione attenuatrice è essenziale per indirizzare la cinetica di reazione: controllando la forza dell'ossidante, si prevengono reazioni secondarie come l'iper-ossidazione della catena o l'insorgere di difetti di reticolazione (cross-linking). Di conseguenza si migliora la regioselettività della polimerizzazione, massimizzando la regolarità strutturale e l'estensione della π-coniugazione nel copolimero semiconduttore **3** sintetizzato. Come solvente di reazione, invece, è stato scelto di utilizzare il cloroformio anidro, necessario per prevenire reazioni secondarie indotte dall'umidità. L'acqua, agendo come nucleofilo e base di Lewis, potrebbe interferire con il processo di polimerizzazione attraverso due meccanismi competitivi. In primo luogo, si potrebbe coordinare al FeCl3 formando specie idrate stabili; ciò saturerebbe la sfera di coordinazione del metallo, riducendone il potenziale ossidativo e inibendo l'innesco della reazione. In secondo luogo, l'acqua potrebbe causare il quenching degli intermedi cationico-radicalici in propagazione. Questo attacco nucleofilo porterebbe alla terminazione prematura della catena polimerica e all'introduzione di difetti strutturali, i quali interromperebbero la coniugazione della catena compromettendo le proprietà semiconduttrici del copolimero **3**. Una volta completato il tempo di reazione, l'isolamento del materiale polimerico ha richiesto un accurato work-up, mirato non solo al recupero del prodotto, ma soprattutto alla completa rimozione delle impurità inorganiche e delle frazioni a basso peso molecolare. -Inizialmente sono stati effettuati lavaggi con acido cloridrico, in questo modo si mantengono i sali di ferro disciolti nella fase acquosa, evitando che precipitino sotto forma di idrossidi insolubili all'interfaccia. La completa rimozione dell'ossidante inorganico è un requisito fondamentale per mantenere l'elettronica del copolimero realizzato: tracce di metalli di transizione all'interno del backbone polimerico abbatterebbero la mobilità dei portatori di carica e spegnerebbero la fluorescenza del materiale. Per monitorare l'efficacia dell'estrazione, le acque di lavaggio sono state sottoposte al saggio del tiocianato. L'aggiunta dello ione SCN- genera, in presenza di ioni Fe3+, un complesso di coordinazione caratterizzato da un'intensa colorazione rossa. I lavaggi acidi sono stati ripetuti fino all'ottenimento di un saggio negativo (soluzione incolore), a riprova della totale purificazione del sistema organico dai residui inorganici. +Inizialmente sono stati effettuati lavaggi con acido cloridrico, in questo modo si mantengono i sali di ferro disciolti nella fase acquosa, evitando che precipitino sotto forma di idrossidi insolubili all'interfaccia. La completa rimozione dell'ossidante inorganico è un requisito fondamentale per mantenere intatte le caratteristiche del trasporto di carica del copolimero realizzato: tracce di metalli di transizione all'interno del backbone polimerico abbatterebbero la mobilità dei portatori di carica e spegnerebbero la fluorescenza del materiale. Per monitorare l'efficacia dell'estrazione, le acque di lavaggio sono state sottoposte al saggio del tiocianato. L'aggiunta dello ione SCN- genera, in presenza di ioni Fe3+, un complesso di coordinazione caratterizzato da un'intensa colorazione rossa. I lavaggi acidi sono stati ripetuti fino all'ottenimento di un saggio negativo (soluzione incolore), a riprova della totale purificazione del sistema organico dai residui inorganici. -L'ultimo lavaggio con una soluzione acquosa mezza satura di cloruro di sodio (NaCl) sfrutta l'elevata forza ionica del sale per massimizzare l'effetto di salting-out: l'ambiente acquoso salino favorisce l'estrazione dell'acqua parzialmente disciolta nel solvente organico. Questa azione di pre-anidrificazione trascina nella fase acquosa anche le ultimissime tracce di impurità idrosolubili, come l'HCl residuo, garantendo l'isolamento di una fase organica di elevata purezza. +L'ultimo lavaggio con una soluzione acquosa satura di cloruro di sodio (NaCl) sfrutta l'elevata forza ionica del sale per massimizzare l'effetto di salting-out: l'ambiente acquoso salino favorisce l'estrazione dell'acqua parzialmente disciolta nel solvente organico. Dopo aver isolato e anidrificato la fase organica, e rimosso il solvente, è stata necessaria una purificazione del solido grezzo. Al fine di allontanare i sottoprodotti di sintesi, primo fra tutti l'omopolimero del 3-esiltiofene, si è ricorsi a una purificazione mediante precipitazione selettiva in un sistema solvente/non-solvente. Il grezzo di reazione è stato solubilizzato nel minor volume possibile di THF e fatto gocciolare in un ampio eccesso di metanolo freddo. @@ -859,15 +874,15 @@ In queste condizioni, il copolimero d'interesse mantiene un'affinità sufficient Al fine di indagare la relazione struttura-proprietà e di valutare l'incidenza del core fluorescente sulle caratteristiche finali del materiale, la reazione di polimerizzazione è stata condotta variando il rapporto stechiometrico tra i due monomeri. Nello specifico, sono stati sintetizzati tre differenti copolimeri, modulando la frazione molare del derivato dichetopirrolopirrolico (**2**) rispetto al 3-esiltiofene (**Tabella 6**). -L'obiettivo era prepare una serie di materiali per studiare l'andamento delle proprietà al variare dell'architettura macromolecolare, ipotizzando di passare da un sistema a maggioranza tiofenica fino a uno equimolare o dominato dal DPP. Tuttavia, specifiche problematiche di reazione hanno limitato l'integrazione del monomero DPP a un massimo del 35%. Tale discrepanza è riconducibile ad una differenza nei rapporti di reattività dei due comonomeri, fortemente influenzata dall'ingombro sterico del nucleo DPP. Quest'ultimo, infatti, risulta svantaggiato nell'accoppiamento rispetto al derivato tiofenico, la cui maggiore reattività e minor volume ne favoriscono l'addizione preferenziale. Si è quindi ottenuta una libreria di materiali in cui si passa da un *backbone* con minime quantità di DPP (copolimero **3a**), a uno in cui la sua percentuale aumenta (copolimero **3b**), fino a giungere al sistema maggiormente arricchito (copolimero **3c**), mantenendo però in tutti i casi un rapporto molare a favore delle unità di 3-esiltiofene. +L'obiettivo era prepare una serie di materiali per studiare l'andamento delle proprietà al variare dell'architettura macromolecolare, ipotizzando di passare da un sistema a maggioranza tiofenica fino a uno equimolare o dominato dal DPP. Tuttavia, specifiche problematiche di reazione hanno limitato l'integrazione del monomero DPP a un massimo del 35% mol/mol. Tale comportamento è riconducibile ad una differenza nei rapporti di reattività dei due comonomeri, fortemente influenzato dall'ingombro sterico del nucleo DPP. Quest'ultimo, infatti, risulta svantaggiato nell'accoppiamento rispetto al derivato tiofenico, la cui maggiore reattività e minor volume ne favoriscono l'addizione preferenziale. Si è quindi ottenuta una libreria di materiali in cui si passa da un *backbone* con minime quantità di DPP (copolimero **3a**), a uno in cui la sua percentuale aumenta (copolimero **3b**), fino a giungere al sistema maggiormente arricchito (copolimero **3c**), mantenendo però in tutti i casi un rapporto molare a favore delle unità di 3-esiltiofene. -| Copolimero | moli DPP 2 | moli 3HT | % DPP teorica (mol/mol) | % DPP reale (mol/mol) | +| Copolimero | % DPP teorica (mol/mol) | Area segnale CH3 (A3HT) | Area segnale CH2 (ADPP) | % 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 | +| 3a | 20 | 69,0 | 31,04 | 25,2 | +| 3b | 50 | 61,41 | 39,95 | 32,6 | +| 3c | 80 | 55,44 | 41,52 | 35,3 | -**Tabella 6** - *composizione dei copolimeri coniugati* +**Tabella 7** - *composizione dei copolimeri coniugati* La composizione percentuale reale delle unità di DPP all'interno dei copolimeri è stata determinata mediante spettroscopia 1H-NMR (**Figura 54**, **Figura 55**, **Figura 56**). L'analisi quantitativa si è basata sull'integrazione di due segnali: il picco relativo ai protoni del gruppo metilico (CH₃) del 3-esiltiofene e quello corrispondente ai protoni dei gruppi metilenici (CH₂) adiacenti alle funzioni idrossiliche del DPP. @@ -883,23 +898,25 @@ dove $A_{DPP}$ e $A_{3HT}$ rappresentano i valori delle aree integrate per i ris La percentuale reale di DPP 2 presente nei tre copolimeri è riportata in **Tabella 6**. +Inoltre, dall'analisi degli spettri 1H-NMR dei tre campioni, si nota come nel copolimero **3a** vi sia la presenza di segnali riconducibili al monomero 3HT non reagito, indicando un minor grado di purezza del prodotto rispetto agli altri campioni sintetizzati. + ![](immagini/a182a55cad5ef042b39852288ff9f6ae3b5f9c0fd758fd0815f0366e77b09a8e.jpg) -**Figura 54** - *spettro 1H-NMR del copolimero 3a in CDCl3* +**Figura 55** - *Spettro 1H-NMR del copolimero 3a in CDCl3* ![](immagini/5ab89fc3cc83f82abb39c0bfd40b1f0da53a8f88a4ca771e00621a476cf8901d.jpg) -**Figura 55** - *spettro 1H-NMR del copolimero 3b in CDCl3* +**Figura 56** - *Spettro 1H-NMR del copolimero 3b in CDCl3* ![](immagini/f078dd5e0992c244123ad8fcbd08d2f2235bffb15f21adcee16bef8ed40a1f4e.jpg) -**Figura 56** - *spettro 1H-NMR del copolimero 3c in CDCl3* +**Figura 57** - *Spettro 1H-NMR del copolimero 3c in CDCl3* In seguito all'analisi strutturale effettuata tramite spettroscopia NMR, i copolimeri sintetizzati sono stati caratterizzati mediante spettroscopia FT-IR, UV-Vis e di emissione, mentre la distribuzione dei pesi molecolari e il comportamento termico sono stati valutati rispettivamente tramite Cromatografia a Permeazione di Gel (GPC) e Calorimetria a Scansione Differenziale (DSC). ![](immagini/4b81d4490846b8b0f24cd7ae9e1ed776036c588345475c519334bef4eb76a684.jpg) -**Figura 57** - *spettro FT-IR dei copolimeri 3a (blu), 3b (verde), 3c (rosso)* +**Figura 58** - *spettro FT-IR dei copolimeri 3a (blu), 3b (verde), 3c (rosso)* L'analisi FT-IR (**Figura 57**) conferma l'avvenuta copolimerizzazione per i campioni **3a** (traccia verde), **3b** (traccia rossa) e **3c** (traccia blu). Tutti gli spettri mostrano gli stretching dei legami C-H alifatici (\~2920 e \~2850 cm⁻¹) e il segnale a \~820 cm⁻¹ caratteristico dell'anello del 3-esiltiofene. L'incorporazione del DPP è provata dall'intenso picco del carbonile lattamico (C=O) a \~1650 cm⁻¹ e dallo stretching C-O a \~1050 cm⁻¹. Come atteso dai dati NMR, la banda degli ossidrili terminali (3300-3400 cm⁻¹) risulta evidente nei polimeri **3b** e **3c**, mentre a minore intensità nel **3a**, confermando il minor contenuto di unità DPP in quest'ultimo campione. @@ -907,51 +924,53 @@ La caratterizzazione foto-fisica dei copolimeri sintetizzati è stata effettuata ![](immagini/585dc7627f409d974b2dda6d2db2fc8d1febafb609faba20d707f941b23f851c.jpg) -**Figura 58** - *spettro UV-Visibile e di emissione del copolimero 3a in THF* +**Figura 59** - *spettro UV-Visibile e di emissione del copolimero 3a in THF* ![](immagini/f8b0852a6a485472cb2438e024374bb56e26d87d86831f40903fd0be201d0771.jpg) -**Figura 59** - *spettro UV-Visibile e di emissione del copolimero 3b in THF* +**Figura 60** - *spettro UV-Visibile e di emissione del copolimero 3b in THF* ![](immagini/2b34f5439b53ddcf7aeff01949aba8f61aa554f29849c81d7c3922f06dd3bba9.jpg) -**Figura 60** - *spettro UV-Visibile e di emissione del copolimero 3c in THF* +**Figura 61** - *spettro UV-Visibile e di emissione del copolimero 3c in THF* I copolimeri **3a**, **3b** e **3c** in soluzione (THF) mostrano profili pressoché identici tra loro e fortemente simili a quello del monomero DPP di partenza (**Figura 58**, **Figura 59**, **Figura 60**). Sia l'ampia banda di assorbimento, con λmax a circa 540-545 nm, relativa alla transizione π→π\*, sia lo spettro di emissione, con λmax a circa 550 nm, ricalcano infatti il comportamento foto-fisico del core dichetopirrolopirrolico. Si nota come tutti i campioni presentino uno Stokes shift estremamente ridotto: questa forte sovrapposizione tra le bande di assorbimento ed emissione è indicativa di una notevole rigidità strutturale dello scheletro polimerico, il quale subisce una minima riorganizzazione conformazionale nel passaggio dallo stato fondamentale a quello eccitato. -| copolimero | λmax, abs (nm) | λmax, ecc (nm) | Stokes shift (nm) | +| copolimero | λmax, asb (nm) | λmax, ecc (nm) | Stokes shift (nm) | | --- | --- | --- | --- | | 3a | 540 | 547 | 7 | | 3b | 544 | 550 | 6 | | 3c | 542 | 552 | 10 | -**Tabella 7** - *dati spettroscopici dei copolimeri sintetizzati* +**Tabella 8** - *dati spettroscopici dei copolimeri sintetizzati in THF* -Tuttavia, sebbene in soluzione diluita i copolimeri mantengano queste eccellenti caratteristiche emissive, il loro comportamento allo stato solido risulta drasticamente differente. Come tipicamente si osserva nei sistemi $\pi$ -coniugati altamente planari, la deposizione allo stato solido favorisce una forte interazione intermolecolare. L'intenso impaccamento delle catene porta alla formazione di aggregati che disattivano i fluorofori attraverso percorsi di decadimento non radiativo. Questo effetto è visivamente confermato osservando i campioni polimerici depositati su vetrino: esposti all'illuminazione di una lampada UV (**Figura 61**), i film non mostrano alcuna emissione apprezzabile allo stato solido. +Tuttavia, sebbene in soluzione diluita i copolimeri mantengano proprietà emissive, il loro comportamento allo stato solido risulta drasticamente differente. Come tipicamente si osserva nei sistemi $\pi$ -coniugati altamente planari, allo stato solido viene favorita una forte interazione intermolecolare. L'intenso impaccamento delle catene porta alla formazione di aggregati che disattivano i fluorofori attraverso percorsi di decadimento non radiativo. Questo effetto è visivamente confermato osservando i campioni polimerici depositati su vetrino: esposti all'illuminazione di una lampada Kessil (456 nm) (**Figura 61**), i film non mostrano alcuna emissione apprezzabile allo stato solido. ![](immagini/efcc22eae8c7e8ff910d35fa7c018b13417126c67a70da70eed1784a889d6d32.jpg) -**Figura 61** - *film solidi dei copolimeri sotto lampada UV, in ordine copolimero 3a, 3b, 3c* +**Figura 62** - *film solidi dei copolimeri sotto lampada UV, in ordine copolimero 3a, 3b, 3c* -Proprio questa tendenza all'aggregazione, e al conseguente quenching emissivo nei film solidi, rappresenta la principale criticità per l'impiego di tali sistemi lineari in dispositivi optoelettronici. Per superare questo limite strutturale è necessario sfavorire l'avvicinamento incontrollato delle catene principali coniugate. È in quest'ottica che si è reso necessario il passaggio a un design macromolecolare più complesso, che giustifica la progettazione e la sintesi di un'architettura di tipo bottle brush. +Proprio questa tendenza all'aggregazione, e al conseguente quenching emissivo nei film solidi, rappresenta la principale criticità per l'impiego di tali sistemi lineari in dispositivi optoelettronici. Per superare questo limite strutturale è necessario sfavorire l'impacchettamento delle catene principali coniugate. È in quest'ottica che si è reso necessario il passaggio a un design macromolecolare più complesso, che giustifica la progettazione e la sintesi di un'architettura di tipo bottle brush. Successivamente, i copolimeri sono stati caratterizzati mediante cromatografia a permeazione di gel (GPC) per determinare la distribuzione dei pesi molecolari -I risultati dell'analisi cromatografica riportati in **Tabella 8** evidenziano masse molecolari medie numerali ( $\overline{M_{n}}$ ) comprese tra circa 1400 e 2150 Da per i copolimeri sintetizzati. I campioni **3a** e **3c** presentano valori di $\overline{M_{n}}$ del tutto equiparabili (rispettivamente 2149 e 2134 Da). Tuttavia, il copolimero **3c** si distingue per una distribuzione delle catene polimeriche maggiormente omogenea, confermata dal valore di polidispersità più contenuto della serie (PD = 1,979). +I risultati dell'analisi cromatografica riportati in **Tabella 8** evidenziano pesi molecolari medi numerali ( $\overline{M_{n}}$ ) comprese tra circa 1400 e 2150 Da per i copolimeri sintetizzati. I campioni **3a** e **3c** presentano valori di $\overline{M_{n}}$ del tutto equiparabili (rispettivamente 2149 e 2134 Da). Tuttavia, il copolimero **3c** si distingue per una distribuzione delle catene polimeriche maggiormente omogenea, confermata dal valore di polidispersità più contenuto della serie (PD = 1.979). -L'ottenimento di indici di polidispersità di questa entità è del tutto normale e atteso per questo sistema, trattandosi di una polimerizzazione non controllata. Nei processi convenzionali, infatti, l'assenza di un rigoroso controllo sulla cinetica di crescita e sulle reazioni di terminazione o trasferimento di catena porta a distribuzioni dei pesi molecolari ampie, con valori teorici e sperimentali di PD che si assestano tipicamente attorno a 2 (distribuzione più probabile di Flory) o superiori.[54](#ref-54) +L'ottenimento di indici di polidispersità di questa entità è del tutto normale e atteso per questo sistema, trattandosi di una polimerizzazione non controllata. Nei processi convenzionali, infatti, l'assenza di un rigoroso controllo sulla cinetica di crescita e sulle reazioni di terminazione o trasferimento di catena porta a distribuzioni dei pesi molecolari ampie, con valori teorici e sperimentali di PD che si assestano tipicamente attorno a 2 (distribuzione più probabile di Flory) o superiori.[55](#ref-55) -Il campione **3b** mostra invece un andamento differente: pur registrando il valore più basso di $\overline{M_{n}}$ (1402 Da), ad esso corrisponde la massa molecolare media ponderale ( $\overline{M_{w}}$ ) più elevata (6439 Da). Questa discrepanza si traduce in un indice di polidispersità nettamente superiore (PD = 4,592), indicando una distribuzione dei pesi molecolari marcatamente ampia. Tale risultato suggerisce la presenza di una frazione significativa di specie oligomeriche a catena corta, che abbassano la media numerica, e di una porzione di macromolecole a peso molecolare più elevato che incrementano il valore ponderale. +Il campione **3b** mostra invece un andamento differente: pur registrando il valore più basso di $\overline{M_{n}}$ (1402 Da), ad esso corrisponde la massa molecolare media ponderale ( $\overline{M_{w}}$ ) più elevata (6439 Da). Questa discrepanza si traduce in un indice di polidispersità nettamente superiore (PD = 4.592), indicando una distribuzione dei pesi molecolari marcatamente ampia. Tale risultato suggerisce la presenza di una frazione significativa di specie oligomeriche a catena corta, che abbassano la media numerica, e di una porzione di macromolecole a peso molecolare più elevato che incrementano il valore ponderale. | 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 | 2149 | 5526 | 2,5 | +| 3b | 1402 | 6439 | 4,5 | +| 3c | 2134 | 4223 | 1,9 | -**Tabella 8** - *pesi molecolari e polidispersità determinati mediante GPC per i copolimeri 3a, 3b e 3c* +**Tabella 9** - *Pesi molecolari e polidispersità determinati mediante GPC per i copolimeri 3a, 3b. 3c* -Al fine di valutare le proprietà termiche dei materiali sintetizzati, i tre copolimeri sono stati analizzati mediante calorimetria a scansione differenziale (DSC). Dai termogrammi ottenuti è emerso che per tutti i campioni la temperatura di transizione vetrosa (Tg) si attesta intorno a -10 °C. A differenza di quanto si osserva per il 3HT, per i campioni in esame non si rilevano invece transizioni di fusione. Questo dato conferma l'ottenimento di un copolimero random: l'elevato disordine strutturale che lo caratterizza, infatti, impedisce al materiale di cristallizzare, nonostante i bassi pesi molecolari. +Al fine di valutare le proprietà termiche dei materiali sintetizzati, i tre copolimeri sono stati analizzati mediante calorimetria a scansione differenziale (DSC). + +A differenza di quanto si osserva per l'omopolimero 3HT, che presenta tipicamente un picco endotermico di fusione, generalmente tra i 210 °C e i 240 °C, dovuto alla sua natura semicristallina, per i campioni in esame non si rilevano invece transizioni di fusione. Questo dato conferma l'ottenimento di un copolimero random: l'elevato disordine strutturale che lo caratterizza, infatti, impedisce al materiale di cristallizzare, nonostante i bassi pesi molecolari. ## 4.3 **Polimeri bottle brush** @@ -960,25 +979,25 @@ In questa fase del progetto di ricerca, l'attenzione si è focalizzata sulla sin ![](immagini/a3ecc2457962649d36b1824710784bec90b0e52d32275fc154743f9bf9f62339.jpg) -**Figura 62** - *effetto dell'intensità dello stacking π-π sull'emissione luminosa* +**Figura 63** - *Effetto dell'intensità dello stacking π-π sull'emissione luminosa* Dal punto di vista sintetico, la realizzazione di tale architettura mediante approccio "grafting from" richiede che la catena polimerica principale sia predisposta per comportarsi come macroiniziatore. Di conseguenza, al fine di innestare successivamente le catene laterali polimeriche, l'unità dichetopirrolopirrolica è stata progettata e sintetizzata introducendo una funzionalità ossidrilica terminale. Tale gruppo -OH costituisce il sito nucleofilo iniziatore per una reazione di polimerizzazione di tipo Ring Opening Polymerization (ROP), la quale permette di regolare il peso molecolare e mantenere una bassa dispersità delle catene laterali in accrescimento, parametri rilevanti per la sintesi di copolimeri bottle brush aventi un'architettura regolare e riproducibile. -Stabilita la tecnica di polimerizzazione, per la costituzione delle catene laterali da accrescere la scelta è ricaduta sul policaprolattone (PCL). Tale decisione deriva da precedenti studi condotti all'interno del gruppo di ricerca. L'impiego del PCL offre infatti un duplice vantaggio, sia a livello sintetico che applicativo. La polimerizzazione del caprolattone via ROP, infatti, risulta essere un processo lineare ed efficiente. Per quanto riguarda le proprietà chimico-fisiche, invece, il PCL è caratterizzato da una bassa temperatura di transizione vetrosa (Tg) e da una buona solubilità nei comuni solventi organici[55](#ref-55). Queste caratteristiche garantiscono una notevole semplicità di lavorazione del prodotto e integrazione del sistema bottle brush all'interno di una matrice polimerica per l'ottenimento dei materiali finali. +Stabilita la tecnica di polimerizzazione, per la costituzione delle catene laterali da accrescere la scelta è ricaduta sul policaprolattone (PCL). Tale decisione deriva da precedenti studi condotti all'interno del gruppo di ricerca. L'impiego del PCL offre infatti un duplice vantaggio, sia a livello sintetico che applicativo. La polimerizzazione del caprolattone via ROP, infatti, risulta essere un processo lineare ed efficiente. Per quanto riguarda le proprietà chimico-fisiche, invece, il PCL è caratterizzato da una bassa temperatura di transizione vetrosa (Tg) e da una buona solubilità nei comuni solventi organici[56](#ref-56). Queste caratteristiche garantiscono una maggiore lavorabilità e integrazione del sistema bottle brush all'interno di una matrice polimerica per l'ottenimento dei materiali finali. -La reazione di polimerizzazione ROP presenta diversi possibili meccanismi[56](#ref-56), uno dei più sfruttati è quello di coordinazione-inserzione del monomero sul centro attivo dell'iniziatore. In particolare, la reazione di apertura dell'anello catalizzata da stagno ottanoato (Sn(Oct)2) richiede generalmente l'aggiunta di co-iniziatori nucleofili come alcol[56](#ref-56). Si ha una prima reazione di scambio dei leganti, tra l'alcol e l'ottanoato del catalizzatore creando la specie attiva. A questo punto il centro metallico si coordina al carbonile del caprolattone, rendendo il carbonio più elettrofilo e favorendo l'attacco nucleofilo del gruppo alcolico con conseguente apertura dell'anello. La crescita del PCL prosegue quindi mediante attacchi successivi del terminale ossidrilico, che mantiene la reattività durante tutta la propagazione della catena (**Figura 63**). +La reazione di polimerizzazione ROP presenta diversi possibili meccanismi[57](#ref-57), uno dei più sfruttati è quello di coordinazione-inserzione del monomero sul centro attivo dell'iniziatore. In particolare, la reazione di apertura dell'anello catalizzata da stagno ottanoato (Sn(Oct)2) richiede generalmente l'aggiunta di co-iniziatori nucleofili come alcol[57](#ref-57). Si ha una prima reazione di scambio dei leganti, tra l'alcol e l'ottanoato del catalizzatore creando la specie attiva. A questo punto il centro metallico si coordina al carbonile del caprolattone, rendendo il carbonio più elettrofilo e favorendo l'attacco nucleofilo del gruppo alcolico con conseguente apertura dell'anello. La crescita del PCL prosegue quindi mediante attacchi successivi del terminale ossidrilico, che mantiene la reattività durante tutta la propagazione della catena (**Figura 63**). ![](immagini/86add528de15d390b0a228d524bbd008d318d4ae0e85530a063f2df5ddf904ee.jpg) -**Figura 63** - *meccanismo di reazione della ROP con gruppo alcolico come iniziatore* +**Figura 64** - *meccanismo di reazione della ROP con gruppo alcolico come iniziatore* La purificazione è stata condotta mediante precipitazione in non-solvente: la miscela di reazione è stata addizionata goccia a goccia all'interno di un largo eccesso di metanolo freddo. La scelta di questo specifico non-solvente è dettata dalle differenti solubilità delle specie in soluzione: mentre l'ε-caprolattone residuo e le altre specie a basso peso molecolare presentano un'elevata affinità per il metanolo, il copolimero ad alto peso molecolare vi risulta insolubile. Inoltre, l'impiego della bassa temperatura riduce ulteriormente la solubilità del polimero e ne favorisce la rapida coagulazione, massimizzando la resa del processo di precipitazione. Il polimero così precipitato è stato successivamente recuperato mediante filtrazione. -Allo scopo di valutare in modo sistematico l'influenza della lunghezza delle catene laterali sulle proprietà finali del materiale, sono state preparate due serie di polimeri bottle brush. Queste serie sono state ottenute impiegando rispettivamente i copolimeri **3b** e **3c** in qualità di macroiniziatori. Sebbene fosse stato sintetizzato anche un terzo copolimero **3a**, il suo impiego per le successive fasi di grafting è stato scartato a causa della scarsa efficienza della sua via sintetica. Nello specifico, le basse rese di reazione e le difficoltà incontrate nel work-up per l'isolamento del prodotto puro portavano a notevoli perdite di materiale. Inoltre, dal punto di vista dell'efficienza di processo, l'isolamento di quantità utili di questo copolimero avrebbe richiesto volumi di solventi e costi di reagenti molto elevati. Di conseguenza, per garantire la fattibilità tecnica ed economica della ricerca, si è scelto di utilizzare esclusivamente i macroiniziatori **3b** e **3c**. +Allo scopo di valutare in modo sistematico l'influenza della lunghezza delle catene laterali sulle proprietà finali del materiale, sono state preparate due serie di polimeri bottle brush. Queste serie sono state ottenute impiegando rispettivamente i copolimeri **3b** e **3c** in qualità di macroiniziatori. Sebbene fosse stato sintetizzato anche un terzo copolimero **3a**, il suo impiego per le successive fasi di grafting è stato scartato a causa della scarsa efficienza della sua via sintetica. Nello specifico, le basse rese di reazione e le difficoltà incontrate nel work-up portavano a notevoli perdite di materiale e non garantivano l'isolamento del prodotto puro: infatti, come visibile nello spettro 1H-NMR in **Figura 55**, anche dopo la purificazione era presente del poliesiltiofene residuo. Inoltre, dal punto di vista dell'efficienza di processo, l'isolamento di quantità utili di questo copolimero avrebbe richiesto volumi di solventi e costi di reagenti molto elevati. Di conseguenza, per garantire la fattibilità tecnica ed economica della ricerca, si è scelto di utilizzare esclusivamente i macroiniziatori **3b** e **3c**. -Sfruttando l'elevato grado di controllo della reazione di ROP, è stato possibile modulare la lunghezza delle catene in accrescimento variando il rapporto molare tra il monomero (ε-caprolattone) e i siti iniziatori (-OH) presenti sul backbone. Seguendo questo approccio, per ciascuno dei due precursori copolimerici sono stati sintetizzati tre differenti polimeri dotate di catene laterali in PCL con pesi molecolari di circa 1500 Da, 5000 Da e 10000 Da (**Tabella 9**). +Sfruttando l'elevato grado di controllo della reazione di ROP, è stato possibile modulare la lunghezza delle catene in accrescimento variando il rapporto molare tra il monomero (ε-caprolattone) e i siti iniziatori (-OH) presenti sul backbone. Seguendo questo approccio, per ciascuno dei due precursori copolimerici sono stati sintetizzati tre differenti polimeri dotate di catene laterali di PCL con pesi molecolari di circa 1500 Da, 5000 Da e 10000 Da (**Tabella 9**). -| Copolimero | Polimero bottle brush | Lunghezza catene di PCL (Da) | +| Copolimero | Polimero bottle brush | $M_{n}$ PCL (Da) | | --- | --- | --- | | 3b | 3.1b | 1500 | | 3b | 3.2b | 5000 | @@ -987,21 +1006,21 @@ Sfruttando l'elevato grado di controllo della reazione di ROP, è stato possibil | 3c | 3.2c | 5000 | | 3c | 3.3c | 10000 | -**Tabella 9** - *lunghezza delle catene in PCL nei polimeri bottle brush* +**Tabella 10** - *lunghezza delle catene in PCL nei polimeri bottle brush* Al fine di determinare la quantità esatta di monomero necessaria per raggiungere ciascuno di questi pesi molecolari target, è stata impiegata la seguente equazione: $$ -V_{CL}=\frac{\frac{m_{backbone}}{MW_{backbone}}\times DP_{backbone}\times \chi _{DPP}\times 2\times Mn_{teorico}}{\rho _{CL}} +V_{CL}=\frac{\frac{m_{copolimero}}{\left(MW_{DPP}\times \chi _{DPP}\right)+\left(MW_{3HT}\times \chi _{3HT}\right)}\times \chi _{DPP}\times 2\times Mn_{teorico}}{\rho _{CL}} $$ -Il termine $V_{CL}$ rappresenta il volume di caprolattone da prelevare e inserire in reazione espresso in mL. Questo parametro è calcolato a partire dalla massa del copolimero lineare di partenza pesata ( $m_{backbone}$ , in g) e dal suo peso molecolare ricavato via GPC ( $MW_{backbone}$ , in g/mol), il cui rapporto restituisce le moli di backbone utilizzate. Tale valore viene moltiplicato per il grado di polimerizzazione del copolimero lineare di partenza ( $DP_{backbone}$ ), per la frazione molare delle unità di DPP al suo interno ( $\chi _{DPP}$ ) e per il valore $2$ , corrispondente al numero di gruppi idrossilici presenti per ogni unità di DPP. Il prodotto ottenuto viene a sua volta moltiplicato per il peso molecolare teorico desiderato per la singola catena laterale di PCL ( $Mn_{teorico}$ , espresso in Da). Infine, l'intero numeratore è diviso per la densità dell' $\varepsilon$ -caprolattone liquido alla temperatura di prelievo ( $\rho _{CL}$ , in g/mL) per convertire la massa totale del monomero nel volume da prelevare. +Il termine $V_{CL}$ rappresenta il volume di caprolattone da prelevare e inserire in reazione espresso in mL. Questo parametro viene calcolato determinando innanzitutto il peso molecolare medio ponderale di una singola unità ripetente del copolimero lineare; tale valore si ottiene sommando il prodotto tra il peso molecolare dell'unità di DPP e la sua frazione molare ( $\chi _{DPP}$ ) con il prodotto tra il peso molecolare dell'unità di 3HT e la rispettiva frazione molare ( $\chi _{3HT}$ ). Dividendo la massa pesata del copolimero lineare di partenza ( $m_{copolimero}$ , in g) per questo peso molecolare medio, si ricavano le moli totali di unità ripetenti. Moltiplicando questo risultato per la frazione molare del DPP e per il valore $2$ , corrispondente al numero di gruppi idrossilici presenti per ogni unità di DPP, si ottengono le moli totali di siti di innesco (-OH) presenti nella miscela di reazione. Le moli di ossidrili vengono a loro volta moltiplicate per il peso molecolare teorico desiderato per la singola catena laterale di PCL ( $Mn_{teorico}$ ), fornendo la massa totale di monomero necessaria. Infine, tale massa viene divisa per la densità dell' $\varepsilon$ -caprolattone liquido alla temperatura di prelievo ( $\rho _{CL}$ ) per convertire il quantitativo nel volume esatto da prelevare. -Per confermare l'avvenuta formazione delle catene laterali, tutti i polimeri sintetizzati sono stati analizzati mediante spettroscopia 1H-NMR. L'effettiva polimerizzazione dell'ε-caprolattone è stata verificata osservando la comparsa dei segnali caratteristici del PCL, in particolare il caratteristico tripletto a circa 4,0 ppm, attribuibile ai protoni metilenici adiacenti all'ossigeno del legame estereo (-CH2-O-), e il segnale a 2,3 ppm relativo ai protoni in alfa al carbonile. Poiché gli spettri risultano del tutto analoghi per l'intera serie di campioni, differendo esclusivamente per i valori di integrazione dei segnali in funzione del peso molecolare, in **Figura 64** riporta lo spettro del polimero **3.1b**, rappresentativo per tutti i composti sintetizzati. +Per confermare l'avvenuta formazione delle catene laterali, tutti i polimeri sintetizzati sono stati analizzati mediante spettroscopia 1H-NMR. L'effettiva polimerizzazione dell'ε-caprolattone è stata verificata osservando la comparsa dei segnali caratteristici del PCL, in particolare il caratteristico tripletto a circa 4.0 ppm, attribuibile ai protoni metilenici adiacenti all'ossigeno del legame estereo (-CH2-O-), e il segnale a 2.3 ppm relativo ai protoni in alfa al carbonile. Poiché gli spettri risultano del tutto analoghi per l'intera serie di campioni, differendo esclusivamente per i valori di integrazione dei segnali in funzione del peso molecolare, in **Figura 64** riporta lo spettro del polimero **3.1b**, rappresentativo per tutti i composti sintetizzati. ![](immagini/aae4bec55b3a0f29e1dfa6231c86c1d0295d5d38f2f2e9f0af6a69eba8aa0231.jpg) -**Figura 64** - *spettro 1H-NMR del polimero 3.1b in CDCl3* +**Figura 65** - *spettro 1H-NMR del polimero 3.1b in CDCl3* Entrambe le serie di polimeri bottle brush sintetizzati sono state sottoposte a spettroscopia FT-IR. Al fine di evidenziare l'accrescimento delle catene laterali, sono stati riportati gli spettri infrarossi sovrapposti delle due serie polimeriche (**Figura 65**, **Figura 66**). Ponendo alla base la traccia del relativo copolimero macroiniziatore, è possibile apprezzare in modo diretto le variazioni spettrali indotte dalle catene laterali di policaprolattone. @@ -1011,13 +1030,13 @@ Come atteso, all'aumentare del peso molecolare delle catene laterali, il profilo ![](immagini/4cd08436660a2e3a6f913e54d196a0d183b780c3f5f915be6d22a563771d3e43.jpg) -**Figura 65** - *spettri FT-IR dei polimeri bottle brush ottenuti a partire dal copolimero 3b (verde)* +**Figura 66** - *spettri FT-IR dei polimeri bottle brush ottenuti a partire dal copolimero 3b (verde):* *polimero 3.1b (arancione), polimero 3.2b (rosa), polimero 3.3b (azzurro)* ![](immagini/d5559d2ff37ffb2861c2ac8eecbade7c09f8fc905c8363be4f48c06a0afae72e.jpg) -**Figura 66** - *spettri FT-IR dei polimeri bottle brush ottenuti a partire dal copolimero 3c (verde)* +**Figura 67** - *spettri FT-IR dei polimeri bottle brush ottenuti a partire dal copolimero 3c (verde):* *polimero 3.1c (arancione), polimero 3.2c (rosa), polimero 3.3c (azzurro)* @@ -1025,7 +1044,7 @@ La caratterizzazione foto-fisica dei polimeri è stata effettuata mediante spett ![](immagini/be53b102694fafa8036962962c8c0a3735cc1ec95cf721f163b7d25bdd7099fb.png) -**Figura 67** - *spettri UV-Visibile (linea continua) e di emissione (linea tratteggiata) dei polimeri bottle brush in THF* +**Figura 68** - *spettri UV-Visibile (linea continua) e di emissione (linea tratteggiata) dei polimeri bottle brush in THF (λecc=490 nm)* I massimi di assorbimento per l'intera libreria di polimeri (**Tabella 10**) rientrano in un range molto ristretto, compreso tra 544 e 554 nm, mentre i massimi di emissione ricadono nell'intervallo tra 557 e 564 nm. Le lievi fluttuazioni registrate all'interno delle due serie polimeriche (derivate rispettivamente dai copolimeri **3b** e **3c**) non seguono un andamento lineare in funzione del peso molecolare del PCL e risultano trascurabili. Tale costanza nei valori di λmax rappresenta una conferma del fatto che l'incremento dell'ingombro sterico non perturba i livelli energetici e la natura delle transizioni elettroniche del core dichetopirrolopirrolico. @@ -1040,61 +1059,61 @@ Un ulteriore dato quantitativo di particolare rilevanza è rappresentato dai val | 3.2c | 544 | 557 | 13 | | 3.3c | 553 | 564 | 11 | -**Tabella 10** - *dati spettroscopici dei polimeri sintetizzati* +**Tabella 11** - *dati spettroscopici dei polimeri sintetizzati* A completamento della caratterizzazione strutturale, l'effettivo accrescimento delle catene laterali e le dimensioni macromolecolari dei sistemi bottle brush sono stati valutati mediante Cromatografia a Permeazione di Gel (GPC). Questa indagine risulta fondamentale non solo per determinare i pesi molecolari medi ( $\overline{M_{n}}$ e $\overline{M_{w}}$ ) e gli indici di dispersità (PD) dei materiali sintetizzati, ma anche per verificare a posteriori il grado di controllo esercitato dalla polimerizzazione per apertura di anello (ROP). Il confronto tra i valori sperimentali ricavati dai cromatogrammi e i pesi molecolari target previsti in fase di progettazione sintetica (rispettivamente 1500, 5000 e 10000 Da) permette infatti di confermare l'efficacia dell'approccio grafting-from e la corretta architettura finale dei copolimeri. | 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 | +| 3.1b | 12188 | 18536 | 1,5 | +| 3.2b | 17302 | 22737 | 1,3 | +| 3.3b | 21269 | 26328 | 1,2 | +| 3.1c | 13999 | 18219 | 1,3 | +| 3.2c | 19119 | 24376 | 1,3 | +| 3.3c | 14445 | 19521 | 1,3 | -**Tabella 11** - *pesi molecolari e polidispersità dei polimeri bottle brush determinati mediante GPC* +**Tabella 12** - *Pesi molecolari e polidispersità dei polimeri bottle brush determinati mediante GPC* I valori di peso molecolare ottenuti tramite GPC (**Tabella 11**) risultano significativamente sottostimati rispetto ai valori teorici a causa del principio di funzionamento della tecnica unito alla particolare architettura bottle brush dei polimeri. La GPC, infatti, separa le macromolecole in base al loro volume idrodinamico, restituendo valori relativi agli standard di calibrazione utilizzati, in questo caso un polimero lineare corrispondente a polistirene. A parità di peso molecolare reale, un polimero altamente ramificato assume una conformazione in soluzione molto più compatta rispetto a un polimero lineare, possedendo quindi un volume idrodinamico nettamente inferiore. Questo fa sì che il polimero ramificato penetri maggiormente nei pori della colonna, eluendo agli stessi tempi di polimeri lineari molto più corti. Tale sottostima è proporzionale all'ingombro delle catene laterali: con innesti in PCL a basso peso molecolare (circa 1500 Da), l'approssimazione a un comportamento lineare risulta più attendibile, restituendo valori GPC attorno ai 12000 Da. -Al contrario, aumentando il peso molecolare dei segmenti laterali (ad esempio stimando tre catene per lato, per un peso teorico atteso di circa 62000 Da), la drastica compattazione strutturale porta a una sottostima del peso reale che si aggira intorno al 70%.[57](#ref-57) In questi sistemi, dunque, i dati ottenuti non indicano il peso molecolare assoluto o una bassa resa, ma confermano indirettamente la presenza di una struttura ramificata altamente impaccata e, sebbene non corrispondenti ai valori reali, permettono un confronto diretto tra i diversi polimeri sintetizzati. +Al contrario, aumentando il peso molecolare dei segmenti laterali (ad esempio stimando tre catene per lato, per un peso teorico atteso di circa 62000 Da), la drastica compattazione strutturale porta a una sottostima del peso reale che si aggira intorno al 70%.[58](#ref-58) In questi sistemi, dunque, i dati ottenuti non indicano il peso molecolare assoluto o una bassa resa, ma confermano indirettamente la presenza di una struttura ramificata altamente impaccata e, sebbene non corrispondenti ai valori reali, permettono un confronto diretto tra i diversi polimeri sintetizzati. Tuttavia, il polimero 3.3c presenta un valore di peso molecolare che si discosta dall'andamento generale degli altri campioni; ciò potrebbe essere dovuto al fatto che, essendo il materiale di partenza di natura random, la presenza di possibili elevate concentrazioni locali di dichetopirrolopirroli e relativi ossidrili nel copolimero, abbia causato una ridotta crescita dei polimeri laterali per via dell'ingombro sterico delle catene in crescita. Tali discrepanze nei valori di peso molecolare saranno comunque maggiormente investigate in futuro attraverso ulteriori analisi. -Al fine di superare le limitazioni associate all'analisi GPC, si è ricorsi all'utilizzo della spettroscopia H-NMR. Il calcolo si fonda sulla valutazione del grado di polimerizzazione delle singole catene laterali di PCL. +Al fine di superare le limitazioni associate all'analisi GPC, si è ricorsi all'utilizzo della spettroscopia H-NMR. -L'equazione generale utilizzata per ricavare il peso molecolare totale ( $MW_{tot}$ ) del copolimero ramificato è la seguente: +L'equazione generale utilizzata per ricavare il peso molecolare teorico l( $MW_{teor}$ ) del copolimero bottle-brush è la seguente: $$ -MW_{tot}=MW_{backbone}+\left[\left(\frac{I_{4{,}05}}{I_{3{,}65}}\times MW_{CL}\right)\times \left(DP_{backbone}\times \chi _{DPP}\times 2\right)\right] +MW_{teor}=MW_{backbone}+\left[\left(\frac{I_{4.05}}{I_{3.65}}\times MW_{CL}\right)\times \left(DP_{backbone}\times \chi _{DPP}\times 2\right)\right] $$ **Equazione 10** - *calcolo del peso molecolare dei polimeri bottle brush mediante 1H-NMR* -Nello specifico, il numero di unità ripetenti per catena laterale è stato ricavato dal rapporto tra l'area del segnale relativo ai protoni metilenici interni alla catena ( $I_{4{,}05}$ per il gruppo –CH2O–CO–, a circa 4,05 ppm) e l'integrale dei protoni metilenici terminali adiacenti al gruppo ossidrilico ( $I_{3{,}65}$ per il gruppo –CH2-OH, a circa 3,65 ppm), il cui valore è stato posto convenzionalmente pari a 1. +Nello specifico, il numero di unità ripetenti per catena laterale è stato ricavato dal rapporto tra l'area del segnale relativo ai protoni metilenici interni alla catena ( $I_{4.05}$ per il gruppo –CH2O–CO–, a circa 4.05 ppm) e l'integrale dei protoni metilenici terminali adiacenti al gruppo ossidrilico ( $I_{3.65}$ per il gruppo –CH2-OH, a circa 3.65 ppm), il cui valore è stato posto convenzionalmente pari a 1. -Il peso molecolare della singola catena di PCL così ottenuto, pari al termine $\left(\frac{I_{4{,}05}}{I_{3{,}65}}\times MW_{CL}\right)$ dove $MW_{CL}$ è il peso molecolare dell'unità ripetente del caprolattone, è stato successivamente moltiplicato per il numero medio di siti di polimerizzazione presenti per macromolecola. Quest'ultimo parametro è stato stimato a partire dal grado di polimerizzazione del copolimero lineare di partenza ( $DP_{backbone}$ ), ricavato dai valori GPC, e dal rapporto molare tra le unità di 3HT e DPP ottenuto via NMR (che definisce la frazione molare $\chi _{DPP}$ ), considerando che ogni unità di DPP reca due gruppi idrossilici di innesco. Infine, il peso molecolare totale dei copolimeri ramificati è stato calcolato sommando la massa complessiva delle catene laterali di PCL al peso molecolare del backbone lineare ( $MW_{backbone}$ ). +Il peso molecolare della singola catena di PCL così ottenuto, pari al termine $\left(\frac{I_{4.05}}{I_{3.65}}\times MW_{CL}\right)$ dove $MW_{CL}$ è il peso molecolare dell'unità ripetente del caprolattone, è stato successivamente moltiplicato per il numero medio di siti di polimerizzazione presenti per macromolecola. Quest'ultimo parametro è stato stimato a partire dal grado di polimerizzazione del copolimero lineare di partenza ( $DP_{backbone}$ ), ricavato dai valori GPC, e dal rapporto molare tra le unità di 3HT e DPP ottenuto via NMR (che definisce la frazione molare $\chi _{DPP}$ ), considerando che ogni unità di DPP reca due gruppi idrossilici di innesco. Infine, il peso molecolare totale dei copolimeri ramificati è stato calcolato sommando la massa complessiva delle catene laterali di PCL al peso molecolare del backbone lineare ( $MW_{backbone}$ ). I valori calcolati con questo metodo offrono una stima molto più vicina ai valori teorici e sono riassunti in **Tabella 12.** -| 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 | +| Polimero | Peso Molecolare da GPC (Da) | Peso Molecolare da 1H-NMR (Da) | Rapporto GPC/1H-NMR | +| --- | --- | --- | --- | +| 3.1b | 12188 | 8900 | 1,37 | +| 3.2b | 17302 | 20500 | 0,85 | +| 3.3b | 21269 | 88000 | | +| 3.1c | 13999 | 18200 | 0,77 | +| 3.2c | 19119 | 35500 | 0,54 | +| 3.3c | 14445 | 41300 | 0,35 | -**Tabella 12** - *pesi molecolari dei polimeri bottle brush determinati via 1H-NMR* +**Tabella 13** - *pesi molecolari dei polimeri bottle brush determinati via 1H-NMR* -Anche per i polimeri bottle brush è stata effettuata l'analisi termica mediante DSC. Dai termogrammi registrati è emerso che le principali transizioni termiche si mantengono pressoché costanti per tutti i polimeri sintetizzati, in quanto dominate dal comportamento del policaprolattone (PCL). Nello specifico, la temperatura di fusione (Tm) risulta compresa nel range tra 55 °C e 60 °C, mentre la temperatura di cristallizzazione (Tc) si attesta nell'intervallo tra 25 °C e 35 °C. +Anche per i polimeri bottle brush è stata effettuata l'analisi termica mediante DSC. Dai termogrammi registrati è emerso che le principali transizioni termiche si mantengono pressoché costanti per tutti i polimeri sintetizzati, in quanto dominate dal comportamento del policaprolattone (PCL). Nello specifico, la temperatura di fusione (Tm) risulta compresa nel range tra 55-60 °C, mentre la temperatura di cristallizzazione (Tc) si attesta nell'intervallo tra 25-35 °C. Questo comportamento è strettamente legato alla struttura tridimensionale di queste macromolecole: le transizioni termiche osservate sono infatti fondamentalmente governate dai segmenti a base di caprolattone che costituiscono le catene laterali. Data l'elevata densità di grafting e rappresentando il caprolattone la frazione preponderante del sistema, la mobilità di queste catene e la loro propensione a cristallizzare dettano le proprietà termiche dell'intero materiale. Di conseguenza, l'influenza dello scheletro polimerico principale viene minimizzata, rendendo i profili termici essenzialmente indipendenti dalle lievi variazioni strutturali tra i diversi polimeri. ![](immagini/d2ed44d32060aa9ee04e73304940b111e53bf65cf115a93ace696933048e308b.jpg) -**Figura 68** - *esempio di termogramma dei polimeri bottle brush realizzati (in figura l'analisi del campione 3.1c)* +**Figura 69** - *esempio di termogramma dei polimeri bottle brush realizzati (in figura l'analisi del campione 3.1c)* ## 4.4 **Ciclovoltammetrie** @@ -1127,7 +1146,7 @@ Per illustrare nel dettaglio la procedura pratica di elaborazione dei dati che ![](immagini/6afc0d601841f25b1c02e27bc6b1616abc101c5f1ceaa0ba9d30ed0f965ebed2.jpg) -**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* +**Figura 70** - *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.* L'analisi qualitativa delle curve corrente/potenziale rivela la natura dei processi di ossido-riduzione dello scheletro coniugato, evidenziandone il grado di reversibilità. @@ -1135,7 +1154,7 @@ In un sistema elettrochimicamente reversibile, il processo di trasferimento elet ![](immagini/5491a0651d00b47f168b335586b4f144e1b25834ff74113ff26b1d3a2c8cc991.jpg) -**Figura 70** - *voltammogramma ciclico del polimero 3.2.c registrato a diverse velocità di scansione* +**Figura 71** - *Voltammogramma ciclico del polimero 3.2.c registrato a diverse velocità di scansione* Questo comportamento è chiaramente evidenziato dai voltammogrammi riportati in **Figura 70**. Analizzando i tracciati ottenuti a velocità di scansione crescenti, non solo si osserva la totale assenza di onde di scarica simmetriche durante la scansione di ritorno, ma si rileva anche una progressiva diminuzione dell'intensità delle onde faradiche. Questa perdita di segnale indica che la specie generata durante l'analisi non è limitata a una semplice irreversibilità del trasferimento di carica, ma risulta intrinsecamente instabile. Il calo della corrente registrata testimonia infatti una degradazione e una conseguente perdita di materiale elettroattivo utile all'interfaccia elettrodo-soluzione. @@ -1151,12 +1170,12 @@ Applicando sistematicamente questo metodo a tutti i tracciati sperimentali, è s I valori di potenziale estratti graficamente sono quantità relative, strettamente dipendenti dalle caratteristiche specifiche dell'elettrodo di riferimento ad Ag/AgCl impiegato e dalle fluttuazioni termodinamiche del sistema solvente/elettrolita. Per convertire queste misure in parametri energetici assoluti, confrontabili con la letteratura, si rende indispensabile una calibrazione dell'asse dei potenziali. A tale scopo è stato impiegato il ferrocene come standard redox interno. -Quest'ultimo costituisce il classico riferimento per le misurazioni elettrochimiche in solventi organici poiché presenta una coppia redox (Fc/Fc+) altamente reversibile, chimicamente stabile e il cui potenziale è ben noto. Dal punto di vista termodinamico, l'energia associata al processo di ossidazione del ferrocene è convenzionalmente posta a - 4,8 eV rispetto al livello energetico del vuoto. Registrando il voltammogramma del ferrocene al termine di ogni analisi e ricavandone il potenziale di semionda sperimentale, è stato possibile calibrare i dati prima della loro elaborazione grafica. L'asse delle ascisse dei voltammogrammi è stato normalizzato sottraendo il potenziale di semionda del ferrocene a tutti i valori di potenziale registrati, riferendo così i tracciati direttamente alla scala del Fc/Fc+. +Quest'ultimo costituisce il classico riferimento per le misurazioni elettrochimiche in solventi organici poiché presenta una coppia redox (Fc/Fc+) altamente reversibile, chimicamente stabile e il cui potenziale è ben noto. Dal punto di vista termodinamico, l'energia associata al processo di ossidazione del ferrocene è convenzionalmente posta a - 4.8 eV rispetto al livello energetico del vuoto. Registrando il voltammogramma del ferrocene al termine di ogni analisi e ricavandone il potenziale di semionda sperimentale, è stato possibile calibrare i dati prima della loro elaborazione grafica. L'asse delle ascisse dei voltammogrammi è stato normalizzato sottraendo il potenziale di semionda del ferrocene a tutti i valori di potenziale registrati, riferendo così i tracciati direttamente alla scala del Fc/Fc+. I potenziali di onset ricavati graficamente da questi voltammogrammi normalizzati sono stati quindi impiegati per calcolare i livelli energetici degli orbitali di frontiera HOMO e LUMO dei copolimeri, applicando le seguenti equazioni empiriche: $$ -E_{HOMO}=-\left(E_{onset}^{ox}+4{,}8\right) eV E_{LUMO}=-\left(E_{onset}^{red}+4{,}8\right) eV +E_{HOMO}=-\left(E_{onset}^{ox}+4.8\right) eV E_{LUMO}=-\left(E_{onset}^{red}+4.8\right) eV $$ **Equazione 11** - *calcolo dei livelli energetici HOMO e LUMO* @@ -1172,7 +1191,7 @@ $$ L'applicazione sistematica di queste equazioni ha permesso di tradurre i dati voltammetrici normalizzati in un quadro quantitativo e completo delle proprietà optoelettroniche dei materiali. -### 4.4.3 **Proprietà elettrochimiche dei copolimeri lienari** +### 4.4.3 **Proprietà elettrochimiche dei copolimeri lineari** Definita la metodologia di indagine, l'analisi dei risultati è partita dallo studio dei copolimeri lineari precursori. L'analisi di questi precursori risulta di fondamentale importanza per valutare il comportamento redox dello scheletro coniugato puro, svincolando la lettura dei dati dalle potenziali variazioni conformazionali o dagli effetti di ingombro sterico indotti dai successivi passaggi di funzionalizzazione. @@ -1186,13 +1205,13 @@ I parametri termodinamici e i livelli energetici degli orbitali di frontiera, es | 3b | 32 | 0,054 | -1,262 | -4,854 | -3,538 | 1,316 | | 3c | 35 | 0,0006 | -1,372 | -4,799 | -3,428 | 1,371 | -**Tabella 13** - *dati voltammetrici dei copolimeri sintetizzati* +**Tabella 14** - *dati voltammetrici dei copolimeri sintetizzati* -A partire dai dati raccolti, il primo parametro optoelettronico preso in esame è il bandgap elettrochimico ( $E_{g}$ ). Il grafico in **Figura 71** illustra la correlazione sperimentale tra l'ampiezza del bandgap e la frazione reale di unità DPP incorporate nello scheletro dei copolimeri lineari analizzati. +A partire dai dati raccolti, il primo parametro elettrochimico preso in esame è il bandgap elettrochimico ( $E_{g}$ ). Il grafico in **Figura 71** illustra la correlazione sperimentale tra l'ampiezza del bandgap e la frazione reale di unità DPP incorporate nello scheletro dei copolimeri lineari analizzati. ![](immagini/6c7bd8393eb8c1a329f65b7fc74e5f338a866e514455c0122a43d13ca340ded5.jpg) -**Figura 71** - *correlazione tra bandgap elettrochimico e frazione reale di DPP nei copolimeri sintetizzati* +**Figura 72** - *correlazione tra bandgap elettrochimico e frazione reale di DPP nei copolimeri sintetizzati* L'analisi del grafico evidenzia una chiara dipendenza tra le due variabili: all'aumentare del contenuto effettivo di dichetopirrolopirrolo lungo la catena polimerica, si osserva un allargamento progressivo del bandgap elettrochimico. Questa tendenza suggerisce che la variazione dell'energia di gap sia governata dalla composizione stechiometrica effettiva del materiale. @@ -1204,11 +1223,11 @@ Proseguendo l'indagine sulle proprietà elettrochimiche, il grafico riportato il ![](immagini/d7a3694f2d97dcaa84465aeed07d8d26adca6a8f8ed64f7ea2bf86943b918b66.jpg) -**Figura 72** - *correlazione tra Epicco e frazione reale di DPP nei copolimeri sintetizzati* +**Figura 73** - *correlazione tra Epicco e frazione reale di DPP nei copolimeri sintetizzati* -La variazione più marcata si osserva a carico del processo di riduzione (drogaggio di tipo n): all'aumentare della frazione di DPP, il potenziale di picco catodico subisce un drastico spostamento verso valori significativamente più negativi. Passando dal copolimero con il contenuto di DPP più basso (25%), con $E_{pc}$ a circa – 1 V, ai materiali con frazioni superiori (32-35%), il picco si sposta nella regione compresa tra – 1,6 V e – 1,8 V. Questa traslazione indica che il processo di inserzione di elettroni diventa termodinamicamente più sfavorito all'aumentare della percentuale di DPP, richiedendo sovratensioni progressivamente maggiori per innescare la formazione delle specie radical-anioniche. +La variazione più marcata si osserva a carico del processo di riduzione (drogaggio di tipo n): all'aumentare della frazione di DPP, il potenziale di picco catodico subisce un drastico spostamento verso valori significativamente più negativi. Passando dal copolimero con il contenuto di DPP più basso (25%), con $E_{pc}$ a circa – 1 V, ai materiali con frazioni superiori (32-35%), il picco si sposta nella regione compresa tra – 1.6 V e – 1.8 V. Questa traslazione indica che il processo di inserzione di elettroni diventa termodinamicamente più sfavorito all'aumentare della percentuale di DPP, richiedendo sovratensioni progressivamente maggiori per innescare la formazione delle specie radical-anioniche. -Per quanto riguarda il processo di ossidazione (drogaggio di tipo p), l'impatto del contenuto di DPP risulta meno drastico ma ugualmente rilevabile. Il potenziale di picco anodico ( $E_{pa}$ ) mostra un moderato spostamento verso valori meno positivi, passando da circa 0,4 V per il polimero a minor contenuto di DPP a valori stabilizzati attorno a 0,2/0,25 V per le frazioni maggiori. +Per quanto riguarda il processo di ossidazione (drogaggio di tipo p), l'impatto del contenuto di DPP risulta meno drastico ma ugualmente rilevabile. Il potenziale di picco anodico ( $E_{pa}$ ) mostra un moderato spostamento verso valori meno positivi, passando da circa 0.4 V per il polimero a minor contenuto di DPP a valori stabilizzati attorno a 0.2/0.25 V per le frazioni maggiori. Analizzando il sistema nel suo complesso, l'effetto combinato di queste due traslazioni si traduce in un allargamento della separazione tra i picchi all'aumentare della percentuale di DPP incorporata. Questa divergenza progressiva tra i potenziali di picco è coerente con l'aumento lineare del band gap elettrochimico discusso precedentemente. @@ -1216,9 +1235,9 @@ Tuttavia, a causa dell'irreversibilità dei processi e delle cinetiche di degrad ![](immagini/b2931ebedd31df7df3b344c25fcbb4a64aceb7b356181adecf39363e49dcb0fe.jpg) -**Figura 73** - *correlazione tra Eonset e frazione reale di DPP nei copolimeri sintetizzati* +**Figura 74** - *correlazione tra Eonset e frazione reale di DPP nei copolimeri sintetizzati* -Come illustrato in **Figura 73**, l'andamento dei potenziali di onset in funzione della frazione di DPP rispecchia fedelmente le tendenze osservate per i potenziali di picco. Il potenziale di onset catodico ( $E_{onset}^{red}$ ), indicativo dell'energia del LUMO, mostra uno spostamento pronunciato verso valori più negativi, passando da circa – 0,75 V per il copolimero a basso contenuto di DPP a valori prossimi a – 1,4 V per le frazioni maggiori. Parallelamente, il potenziale di onset anodico ( $E_{onset}^{ox}$ ), correlato all'energia dell'HOMO, subisce una lieve traslazione verso potenziali meno positivi (da circa 0,25 V a quasi 0 V). La progressiva separazione tra $E_{onset}^{ox}$ ed $E_{onset}^{red}$ all'aumentare dell'unità DPP conferma l'allargamento del bandgap, dimostrando come la composizione macromolecolare agisca in modo sistematico sui livelli energetici di frontiera del materiale. +Come illustrato in **Figura 73**, l'andamento dei potenziali di onset in funzione della frazione di DPP rispecchia fedelmente le tendenze osservate per i potenziali di picco. Il potenziale di onset catodico ( $E_{onset}^{red}$ ), indicativo dell'energia del LUMO, mostra uno spostamento pronunciato verso valori più negativi, passando da circa – 0.75 V per il copolimero a basso contenuto di DPP a valori prossimi a – 1.4 V per le frazioni maggiori. Parallelamente, il potenziale di onset anodico ( $E_{onset}^{ox}$ ), correlato all'energia dell'HOMO, subisce una lieve traslazione verso potenziali meno positivi (da circa 0.25 V a quasi 0 V). La progressiva separazione tra $E_{onset}^{ox}$ ed $E_{onset}^{red}$ all'aumentare dell'unità DPP conferma l'allargamento del bandgap, dimostrando come la composizione macromolecolare agisca in modo sistematico sui livelli energetici di frontiera del materiale. A ulteriore conferma dell'impatto strutturale dell'unità dichetopirrolopirrolo, risulta logico un confronto con il comportamento elettrochimico del poli(3-esiltiofene) (P3HT) omopolimero. @@ -1235,16 +1254,16 @@ I parametri termodinamici ed energetici finali, calcolati per l'intera serie di | 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 | +| 3.1.b | -0,18 | -1,22 | -4,62 | -3,58 | 1,04 | +| 3.2.b | -0,18 | -1,27 | -4,63 | -3,53 | 1,10 | +| 3.3.b | -0,17 | -1,20 | -4,63 | -3,60 | 1,03 | +| 3.1.c | -0,03 | -1,55 | -4,77 | -3,25 | 1,52 | +| 3.2.c | -0,11 | -1,53 | -4,69 | -3,27 | 1,42 | +| 3.3.c | -0,32 | -1,25 | -4,48 | -3,55 | 0,93 | -**Tabella 14** - *dati voltammetrici dei polimeri sintetizzati* +**Tabella 15** - *dati voltammetrici dei polimeri sintetizzati* -Dal confronto tra questi dati e quelli dei precursori lineari discussi nel paragrafo XX (XX), è possibile valutare l'impatto dell'innesto delle catene laterali di policaprolattone (PCL) sulle proprietà optoelettroniche del materiale. +Dal confronto tra questi dati e quelli dei precursori lineari discussi nel paragrafo precedente (**Tabella 14**), è possibile valutare l'impatto dell'innesto delle catene laterali di policaprolattone (PCL) sulle proprietà optoelettroniche del materiale. Innanzitutto, l'analisi evidenzia che i copolimeri bottle brush mantengono la caratteristica elettroattività dello scheletro coniugato. Questo comportamento dimostra che i processi di ossido-riduzione avvengono coerentemente a carico del core a base di DPP e 3HT, mentre i rami alifatici fungono da matrice dielettrica circostante. @@ -1257,9 +1276,9 @@ Lo studio delle proprietà ottiche allo stato solido rappresenta un passaggio fo Negli spettri di assorbimento UV-Vis registrati allo stato solido, la limitata mobilità conformazionale e il forte impaccamento delle catene inducono generalmente una maggiore planarizzazione dello scheletro coniugato. Rispetto agli spettri in soluzione, questo fenomeno si traduce in una delocalizzazione elettronica più estesa lungo il backbone polimerico, portando a un aumento della lunghezza di coniugazione effettiva. Macroscopicamente, tale effetto genera un tipico spostamento batocromo del massimo di assorbimento e, in molti casi, la comparsa di una struttura vibronica più risolta, indice di un elevato grado di ordine strutturale locale. -La tipologia di aggregazione supramolecolare detta le regole di transizione elettronica. Secondo la teoria dell'accoppiamento eccitonico di Kasha, l'impaccamento delle catene coniugate può avvenire prevalentemente secondo due geometrie: gli aggregati di tipo H (impaccamento face-to-face, in cui prevalgono le interazioni π-π laterali) e gli aggregati di tipo J (impaccamento head-to-tail). Nei polimeri coniugati, le forti interazioni π-π favoriscono frequentemente la formazione di aggregati H, i quali presentano una transizione otticamente permessa verso lo stato eccitonico a maggiore energia.[58](#ref-58) +La tipologia di aggregazione supramolecolare detta le regole di transizione elettronica. Secondo la teoria dell'accoppiamento eccitonico di Kasha, l'impaccamento delle catene coniugate può avvenire prevalentemente secondo due geometrie: gli aggregati di tipo H (impaccamento face-to-face, in cui prevalgono le interazioni π-π laterali) e gli aggregati di tipo J (impaccamento head-to-tail). Nei polimeri coniugati, le forti interazioni π-π favoriscono frequentemente la formazione di aggregati H, i quali presentano una transizione otticamente permessa verso lo stato eccitonico a maggiore energia.[59](#ref-59) -Queste dinamiche di aggregazione hanno ripercussioni molto evidenti sulle proprietà di emissione allo stato solido. Il fenomeno più comunemente osservato nei sistemi π-coniugati altamente planari è l'estinzione dell'emissione causata dall'aggregazione (ACQ). La forte vicinanza tra gli anelli aromatici e la formazione di aggregati H, favoriscono il rilassamento non radiativo degli eccitoni attraverso la formazione di eccimeri o il trasferimento di energia verso siti di smorzamento (difetti conformazionali o trappole energetiche). Di conseguenza, le rese quantiche di fluorescenza allo stato solido subiscono un drastico abbattimento rispetto a quelle misurate in soluzione.[59](#ref-59) +Queste dinamiche di aggregazione hanno ripercussioni molto evidenti sulle proprietà di emissione allo stato solido. Il fenomeno più comunemente osservato nei sistemi π-coniugati altamente planari è l'estinzione dell'emissione causata dall'aggregazione (ACQ). La forte vicinanza tra gli anelli aromatici e la formazione di aggregati H, favoriscono il rilassamento non radiativo degli eccitoni attraverso la formazione di eccimeri o il trasferimento di energia verso siti di smorzamento (difetti conformazionali o trappole energetiche). Di conseguenza, le rese quantiche di fluorescenza allo stato solido subiscono un drastico abbattimento rispetto a quelle misurate in soluzione.[60](#ref-60) Nei copolimeri alternati a donatore-accettore (D-A), la struttura è ulteriormente arricchita dalla presenza della banda di trasferimento di carica intramolecolare (ICT). L'impaccamento solido riduce le distanze intermolecolari, facilitando anche fenomeni di trasferimento di carica intermolecolare. In sistemi che presentano forti cromofori elettron-accettori e unità elettron-donatrici, come i derivati tiofenici, la tendenza all'impaccamento intermolecolare ed alla cristallizzazione è notevole. Per modulare questi effetti e prevenire un quenching della luminescenza, l'introduzione di ingombri sterici mirati, come catene alchiliche ramificate, innesti polimerici laterali o architetture bottle brush, diventa una strategia cruciale. Tali modifiche strutturali agiscono da spaziatori fisici: pur mantenendo la coniugazione elettronica sul backbone principale, ostacolano l'eccessivo avvicinamento dei piani π, limitando la formazione di aggregati H non radiativi e preservando in parte le proprietà emissive del materiale. @@ -1267,7 +1286,7 @@ Al fine di indagare l'intricata correlazione tra la struttura supramolecolare e ![](immagini/04f625a8b25744bf2d07d569e55558174b59a5cb564c8bdd0a53c704dfbde545.jpg) -**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)* +**Figura 75** - *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)* L'analisi comparativa delle proprietà ottiche in soluzione liquida (LS) e allo stato solido (SS) permette di evidenziare l'effetto dell'impaccamento macromolecolare sulle transizioni elettroniche del materiale sintetizzato. Osservando i profili di assorbimento, in soluzione il polimero presenta una banda principale con un massimo di assorbimento centrato a circa 550 nm. Passando allo stato solido, il profilo di assorbimento subisce un significativo allargamento e un marcato spostamento batocromo, riposizionando il massimo di transizione nell'intervallo tra 570 e 580 nm, unitamente a una variazione dell'intensità relativa della spalla vibronica a energie maggiori. Questo slittamento verso lunghezze d'onda superiori è attribuibile alla planarizzazione del backbone coniugato indotta dai vincoli conformazionali dello stato solido, la quale favorisce un'estensione della lunghezza di coniugazione effettiva rispetto alle catene solvatate. @@ -1282,11 +1301,11 @@ Il presente lavoro di tesi si è prefissato l'obiettivo primario di progettare, Dal punto di vista sintetico, il percorso intrapreso ha dimostrato la piena efficacia e riproducibilità di una strategia basata sull'impiego di monomeri ortogonali e multifunzionali derivati dal dichetopirrolopirrolo (DPP). In primo luogo, la reazione di ciclizzazione tra il **2**-cianotiofene e il diisopropil succinato ha consentito di isolare con successo il fluoroforo tetraciclico **1**. La successiva funzionalizzazione mediante $N$ -alchilazione nucleofila con 6-bromo-**1**-esanolo ha portato all'ottenimento del monomero chiave bis-alchilato (composto **2**), confermato per via spettroscopica (-NMR e FT-IR). Tale monomero ha esibito la duplice funzionalità ricercata: la presenza degli eterocicli tiofenici ha fornito i siti reattivi per l'accrescimento della catena principale semiconduttrice, mentre i gruppi ossidrilici primari terminali hanno svolto il ruolo di iniziatori indipendenti per la successiva fase di innesto. La sintesi dello scheletro polimerico coniugato è stata condotta mediante polimerizzazione ossidativa diretta mediata da cloruro ferrico in presenza di nitrometano, accoppiando il monomero di DPP con il 3-esiltiofene (3HT). Questo approccio si è rivelato particolarmente vantaggioso rispetto ai canonici accoppiamenti incrociati mediati da palladio, eliminando la necessità di stadi di pre-funzionalizzazione e operando in condizioni termodinamiche blande. La sintesi di tre differenti copolimeri statistici a rapporto co-monomerico variabile (**3a**, **3b** e **3c**) ha confermato la versatilità della metodica, permettendo di ottenere materiali processabili con pesi molecolari compresi tra circa 1400 e 2150 Da e un intervallo di lavorabilità termica adeguato, caratterizzato da transizioni vetrose intorno a – 10 °C e temperature di fusione superiori a 110 °C. -L'accrescimento delle architetture bottle brush a partire dai macroiniziatori **3b** e **3c** è stato realizzato mediante polimerizzazione ad apertura d'anello (ROP) dell' $\varepsilon$ -caprolattone, catalizzata da ottanoato di stagno. Attraverso la modulazione del rapporto molare tra monomero ciclico e siti ossidrilici pendenti, sono state sintetizzate con successo due serie di copolimeri a spazzola con catene laterali di PCL a pesi molecolari nominali crescenti (1500, 5000 e 10000 Da). L'avvenuta reazione di innesto è stata verificata tramite FT-IR, registrando la completa scomparsa della banda associata agli ossidrili terminali e la concomitante comparsa dell'intenso assorbimento carbonilico estereo del PCL a circa $1720 cm^{-1}$ . L'indagine condotta mediante cromatografia a permeazione di gel (GPC) ha evidenziato indici di dispersità contenuti (1,23–1,52). Inoltre, la marcata contrazione del volume idrodinamico in soluzione rilevata rispetto ai pesi teorici lineari ha costituito una prova dell'ottenimento di macromolecole ramificate a densità elevata e struttura altamente compatta. Dal punto di vista termico, il comportamento dei sistemi bottle brush si è dimostrato governato dalla fase semicristallina dominante delle catene laterali di PCL, garantendo un profilo termico omogeneo e indipendente dalle minime oscillazioni della catena principale. +L'accrescimento delle architetture bottle brush a partire dai macroiniziatori **3b** e **3c** è stato realizzato mediante polimerizzazione ad apertura d'anello (ROP) dell' $\varepsilon$ -caprolattone, catalizzata da ottanoato di stagno. Attraverso la modulazione del rapporto molare tra monomero ciclico e siti ossidrilici pendenti, sono state sintetizzate con successo due serie di copolimeri a spazzola con catene laterali di PCL a pesi molecolari nominali crescenti (1500, 5000 e 10000 Da). L'avvenuta reazione di innesto è stata verificata tramite FT-IR, registrando la completa scomparsa della banda associata agli ossidrili terminali e la concomitante comparsa dell'intenso assorbimento carbonilico estereo del PCL a circa $1720 cm^{-1}$ . L'indagine condotta mediante cromatografia a permeazione di gel (GPC) ha evidenziato indici di dispersità contenuti (1.23–1.52). Inoltre, la marcata contrazione del volume idrodinamico in soluzione rilevata rispetto ai pesi teorici lineari ha costituito una prova dell'ottenimento di macromolecole ramificate a densità elevata e struttura altamente compatta. Dal punto di vista termico, il comportamento dei sistemi bottle brush si è dimostrato governato dalla fase semicristallina dominante delle catene laterali di PCL, garantendo un profilo termico omogeneo e indipendente dalle minime oscillazioni della catena principale. La caratterizzazione ottica in soluzione ha evidenziato che la funzionalizzazione sterica non perturba l'integrità elettronica del core dichetopirrolopirrolico: i massimi di assorbimento (544–554 nm) e di emissione (557–564 nm), unitamente a valori di Stokes shift costantemente contenuti (8–14 nm), hanno confermato la conservazione dell'assetto planare del cromoforo e la minima riorganizzazione strutturale tra stato fondamentale ed eccitato. Al contrario, le indagini spettroscopiche condotte allo stato solido su film sottili (esemplificate sul campione 3.2b) hanno fornito indicazioni determinanti: lo spostamento batocromo dell'assorbimento (fino a 570–580 nm) e l'allargamento spettrale dell'emissione, con un marcato red-shift centrato a circa 650–660 nm, hanno dimostrato come l'impaccamento supramolecolare promuova la migrazione dell'eccitone verso stati aggregati a minore energia. Nonostante l'insorgenza di tali riarrangiamenti, l'architettura bottle brush ha consentito il mantenimento di un'apprezzabile emissione nel rosso, attenuando i percorsi di disattivazione non radiativa totale tipici dell'ACQ non controllato. -Infine, l'approfondita indagine elettrochimica condotta mediante ciclovoltammetria ha fornito riscontri fondamentali circa le proprietà semiconduttrici e la struttura a bande dei materiali. Sebbene i polimeri esibiscano un meccanismo di trasferimento di carica irreversibile di tipo elettrochimico-chimico indotto dall'elevata reattività dei cationi e anioni radicalici all'interfaccia elettrodica, l'estrapolazione rigorosa dei potenziali di onset ha consentito di determinare con precisione la posizione dei livelli energetici HOMO e LUMO e l'ampiezza del bandgap elettrochimico. L'analisi comparativa ha evidenziato una correlazione lineare ( $R^{2}=0{,}9719$ ) tra la percentuale reale di DPP incorporata e l'allargamento del bandgap (da 3,42 eV a oltre 4,30 eV), guidata principalmente da uno spostamento del potenziale di riduzione catodica verso valori progressivamente più negativi. Tale sistematicità dimostra che la composizione monomerica funge da eccellente parametro di controllo per calibrare finemente i livelli elettronici di frontiera. +Infine, l'approfondita indagine elettrochimica condotta mediante ciclovoltammetria ha fornito riscontri fondamentali circa le proprietà semiconduttrici e la struttura a bande dei materiali. Sebbene i polimeri esibiscano un meccanismo di trasferimento di carica irreversibile di tipo elettrochimico-chimico indotto dall'elevata reattività dei cationi e anioni radicalici all'interfaccia elettrodica, l'estrapolazione rigorosa dei potenziali di onset ha consentito di determinare con precisione la posizione dei livelli energetici HOMO e LUMO e l'ampiezza del bandgap elettrochimico. L'analisi comparativa ha evidenziato una correlazione lineare ( $R^{2}=0{,}9719$ ) tra la percentuale reale di DPP incorporata e l'allargamento del bandgap (da 3.42 eV a oltre 4.30 eV), guidata principalmente da uno spostamento del potenziale di riduzione catodica verso valori progressivamente più negativi. Tale sistematicità dimostra che la composizione monomerica funge da eccellente parametro di controllo per calibrare finemente i livelli elettronici di frontiera. In conclusione, i risultati conseguiti nel presente lavoro di tesi confermano la validità del design macromolecolare proposto: 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. @@ -1362,7 +1381,7 @@ In conclusione, i risultati conseguiti nel presente lavoro di tesi confermano la 35. Kasha, M. Characterization of electronic transitions in complex molecules. *Discuss. Faraday Soc.* **9**, 14 (1950). -36. On the Change of Refrangibility of Light. By G. G. STOKES, ALA., F.R.S., Fellow of Pembroke College, and Lucasian Professor of -Mathematics in the University of Cambridge. +36. On the Change of Refrangibility of Light. 37. Prodi, L. & Credi, A. Spectrofluorimetry. in *The Exploration of Supramolecular Systems and Nanostructures by Photochemical Techniques* (ed. Ceroni, P.) vol. 78 97–129 (Springer Netherlands, Dordrecht, 2012). @@ -1392,20 +1411,22 @@ In conclusione, i risultati conseguiti nel presente lavoro di tesi confermano la 50. Cardona, C. M., Li, W., Kaifer, A. E., Stockdale, D. & Bazan, G. C. Electrochemical Considerations for Determining Absolute Frontier Orbital Energy Levels of Conjugated Polymers for Solar Cell Applications. *Adv. Mater.* **23**, 2367–2371 (2011). -51. Wang, L. *et al.* Robust singlet fission process in strong absorption π-expanded diketopyrrolopyrroles. *Chem. Sci.* **13**, 13907–13913 (2022). +51. Scurti, S. *et al.* Symmetric azobenzene-substituted diketopyrrolopyrroles dyes as acid-base switchable molecular-probe for colorimetric paper-based sensors. *Dyes Pigments* **245**, 113288 (2026). -52. 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.* **12**, 5570–5593 (2025). +52. Wang, L. *et al.* Robust singlet fission process in strong absorption π-expanded diketopyrrolopyrroles. *Chem. Sci.* **13**, 13907–13913 (2022). -53. Paganin, D. L., Bizzarri, P. C. & Lanzi, D. M. Sintesi e proprietà di nuovi polimeri tiofenici per applicazioni optoelettroniche. +53. 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.* **12**, 5570–5593 (2025). -54. Odian, G. G. *Principles of Polymerization*. (Wiley-Interscience, Hoboken, N.J, 2004). +54. Paganin, D. L., Bizzarri, P. C. & Lanzi, D. M. Sintesi e proprietà di nuovi polimeri tiofenici per applicazioni optoelettroniche. -55. Woodruff, M. A. & Hutmacher, D. W. The return of a forgotten polymer—Polycaprolactone in the 21st century. *Prog. Polym. Sci.* **35**, 1217–1256 (2010). +55. Odian, G. G. *Principles of Polymerization*. (Wiley-Interscience, Hoboken, N.J, 2004). -56. Labet, M. & Thielemans, W. Synthesis of polycaprolactone: a review. *Chem. Soc. Rev.* **38**, 3484 (2009). +56. Woodruff, M. A. & Hutmacher, D. W. The return of a forgotten polymer—Polycaprolactone in the 21st century. *Prog. Polym. Sci.* **35**, 1217–1256 (2010). -57. Floyd, T. G. *et al.* Cationic Bottlebrush Copolymers from Partially Hydrolyzed Poly(oxazoline)s. *Macromolecules* **54**, 9461–9473 (2021). +57. Labet, M. & Thielemans, W. Synthesis of polycaprolactone: a review. *Chem. Soc. Rev.* **38**, 3484 (2009). -58. Kasha, M., Rawls, H. R. & Ashraf El-Bayoumi, M. The exciton model in molecular spectroscopy. *Pure Appl. Chem.* **11**, 371–392 (1965). +58. Floyd, T. G. *et al.* Cationic Bottlebrush Copolymers from Partially Hydrolyzed Poly(oxazoline)s. *Macromolecules* **54**, 9461–9473 (2021). -59. Spano, F. C. & Silva, C. H- and J-Aggregate Behavior in Polymeric Semiconductors. *Annu. Rev. Phys. Chem.* **65**, 477–500 (2014). \ No newline at end of file +59. Kasha, M., Rawls, H. R. & Ashraf El-Bayoumi, M. The exciton model in molecular spectroscopy. *Pure Appl. Chem.* **11**, 371–392 (1965). + +60. Spano, F. C. & Silva, C. H- and J-Aggregate Behavior in Polymeric Semiconductors. *Annu. Rev. Phys. 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