From 3fb87cc39a7dda3d49723a394b01507b993235f1 Mon Sep 17 00:00:00 2001 From: Davide Grilli Date: Sun, 18 Oct 2026 15:56:59 +0200 Subject: [PATCH] Aggiunge slide Marp della presentazione con immagini Co-Authored-By: Claude Sonnet 5.5 --- .../images/fig-film-bottle-brush-uv.png | Bin 0 -> 171919 bytes .../images/fig-film-copolimeri-uv.jpg | Bin 0 -> 64701 bytes .../images/fig-sistemi-fluorofori.png | Bin 0 -> 183435 bytes presentazione/images/fig-uv-dpp1.jpg | Bin 0 -> 61337 bytes presentazione/images/fig-uv-dpp2.jpg | Bin 0 -> 54903 bytes presentazione/images/fig1-dpp.jpg | Bin 0 -> 13200 bytes presentazione/images/fig2-sintesi-dpp1.jpg | Bin 0 -> 21393 bytes .../images/fig3-alchilazione-dpp2.jpg | Bin 0 -> 21403 bytes .../images/fig4-copolimerizzazione.jpg | Bin 0 -> 23421 bytes .../images/fig5-rop-bottle-brush.jpg | Bin 0 -> 32846 bytes presentazione/images/fig6-uv-em-3.2b.jpg | Bin 0 -> 52818 bytes presentazione/images/fig7-bandgap-vs-dpp.png | Bin 0 -> 41807 bytes presentazione/slides.md | 181 ++++++++++++++++++ 13 files changed, 181 insertions(+) create mode 100644 presentazione/images/fig-film-bottle-brush-uv.png create mode 100644 presentazione/images/fig-film-copolimeri-uv.jpg create mode 100644 presentazione/images/fig-sistemi-fluorofori.png create mode 100644 presentazione/images/fig-uv-dpp1.jpg create mode 100644 presentazione/images/fig-uv-dpp2.jpg create mode 100644 presentazione/images/fig1-dpp.jpg create mode 100644 presentazione/images/fig2-sintesi-dpp1.jpg create mode 100644 presentazione/images/fig3-alchilazione-dpp2.jpg create mode 100644 presentazione/images/fig4-copolimerizzazione.jpg create mode 100644 presentazione/images/fig5-rop-bottle-brush.jpg create mode 100644 presentazione/images/fig6-uv-em-3.2b.jpg create mode 100644 presentazione/images/fig7-bandgap-vs-dpp.png create mode 100644 presentazione/slides.md diff --git a/presentazione/images/fig-film-bottle-brush-uv.png b/presentazione/images/fig-film-bottle-brush-uv.png 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100644 index 0000000..ac6cb2b --- /dev/null +++ b/presentazione/slides.md @@ -0,0 +1,181 @@ +--- +marp: true +paginate: true +--- + + + +## Tesi magistrale in Chimica Industriale · a.a. 2025-2026 + +# Sintesi e caratterizzazione di copolimeri bottle brush foto-elettro attivi + +**Candidata:** Aurora Luzi +**Relatore:** Dr. Stefano Scurti + +Dipartimento di Chimica Industriale "Toso Montanari" · Università di Bologna + +--- + +# Soft optoelectronics + +- **Semiconduttori organici π-coniugati**: leggeri, flessibili, depositabili da soluzione a bassa temperatura +- Convertono segnali elettrici in luce (**OLED**, diodi organici a emissione di luce) o viceversa (celle fotovoltaiche) +- Serve **ingegnerizzare il band gap**: approccio **donatore-accettore (D-A)** + +> **[Spazio per immagine]** Schema di un OLED (strati, iniezione di carica ed emissione) e struttura D-A con trasferimento di carica intramolecolare + +--- + +# Aggregation-Caused Quenching (ACQ) + +- Scheletro planare → **π-stacking** → dissipazione non radiativa → **fluorescenza spenta allo stato solido** +- In un OLED serve proprio l'emissione + +> **[Spazio per immagine]** Schema catene isolate in soluzione (emissione) vs catene impilate allo stato solido (quenching) + +**Domanda:** un'architettura **bottle brush** può superare l'ACQ mantenendo l'integrità elettrochimica del core DPP? + +--- + +# Dichetopirrolopirrolo (DPP) + +![bg right:46% fit](images/fig1-dpp.jpg) + +- Nucleo **planare, rigido ed elettron-povero** +- π-stacking e legami a idrogeno: molto stabile, ma **poco solubile** +- **N-alchilazione**: elimina i legami a idrogeno e aumenta la solubilità +- Tiofeni in posizione 3 e 6: siti di **polimerizzazione** + +--- + +# Monomero ortogonale e grafting-from + +![bg right:50% fit](images/fig-sistemi-fluorofori.png) + +- Fluoroforo legato **covalentemente** (a: host-guest, b: main-chain, c: side-chain, d: cross-linked) +- DPP con **due -OH**: tiofeni per lo scheletro (con **3-esiltiofene**, 3HT, via FeCl3), -OH come iniziatori della **ROP** (polimerizzazione ad apertura di anello) +- Catene laterali di **PCL** (poli(ε-caprolattone)) = spaziatore sterico + +--- + +# DPP **1** e monomero ortogonale **2** + +![w:520](images/fig2-sintesi-dpp1.jpg) ![w:520](images/fig3-alchilazione-dpp2.jpg) + +- **1**: ciclizzazione pseudo-Stobbe di 2-cianotiofene e diisopropil succinato +- **2**: N-alchilazione di **1** con 6-bromo-1-esanolo +- Conferma: 1H-NMR (4,1 e 3,6 ppm), FT-IR (O-H a ~3400 cm-1) + +--- + +# Proprietà ottiche di **1** e **2** in THF + +![w:520](images/fig-uv-dpp1.jpg) ![w:520](images/fig-uv-dpp2.jpg) + +- **1**: assorbimento 531 nm, emissione 542 nm, Stokes shift 11 nm +- **2**: assorbimento 541 nm (**red-shift**): le catene alifatiche destabilizzano l'HOMO e riducono il band gap ottico + +--- + +# Copolimerizzazione ossidativa DPP-3HT + +![bg right:50% fit](images/fig4-copolimerizzazione.jpg) + +- FeCl3 in nitrometano/CHCl3: nessuna pre-funzionalizzazione, T ambiente +- **3a, 3b, 3c**: 20, 50, 80% DPP in alimentazione + +| | DPP reale | Mn (Da) | +|---|---|---| +| **3a** | 3% | 2200 | +| **3b** | 12% | 2400 | +| **3c** | 35% | 2100 | + +DPP incorporato **≤ 35%** (3HT più reattivo, DPP ingombrante) + +--- + +# Copolimeri lineari: l'ACQ è confermata + +![bg right:44% fit](images/fig-film-copolimeri-uv.jpg) + +- **In soluzione (THF)**: profili ottici identici, assorbimento 540-544 nm, emissione ~550 nm +- **Allo stato solido**: nessuna emissione apprezzabile (lampada Kessil, 456 nm) +- DSC: nessuna fusione, struttura random + +--- + +# ROP del ε-caprolattone + +![bg right:50% fit](images/fig5-rop-bottle-brush.jpg) + +- Dai -OH di **3b** e **3c**, Sn(Oct)2 (stagno ottanoato), toluene, 110 °C +- Catene di PCL da **1500, 5000, 10000 Da** → 6 bottle brush +- Conferma: 1H-NMR (tripletto a ~4,0 ppm), FT-IR (sparisce O-H, compare C=O a ~1720 cm-1) +- GPC: PD 1,2-1,5; DSC: Tm 55-60 °C + +--- + +# Bottle brush allo stato solido + +![w:500](images/fig6-uv-em-3.2b.jpg) ![w:500](images/fig-film-bottle-brush-uv.png) + +- **3.2b**: emissione da ~560-565 nm (soluzione) a **~650-660 nm** (film): **emissione nel rosso** +- Catene lunghe: emissione intensa; **3 kDa**: spenta come nei lineari +- Il PCL funziona da **spaziatore sterico** + +--- + +# Integrità elettrochimica (ciclovoltammetria) + +![bg right:46% fit](images/fig7-bandgap-vs-dpp.png) + +- Processi **irreversibili**, a carico del core DPP-3HT +- Band gap: monomero **2** 2,01 eV; lineari **0,97-1,37 eV**, cresce con la % di DPP fino a un plateau +- Bottle brush: **0,929-1,521 eV** +- Il PCL non compromette l'elettroattività + +--- + +# Cosa abbiamo ottenuto + +- Il bottle brush **attenua l'ACQ**: lineari spenti, bottle brush con catene lunghe emettono nel rosso +- **Integrità elettrochimica** del core DPP preservata +- **Limiti**: DPP ≤ 35%, GPC sottostima i pesi molecolari, nessuna resa quantica allo stato solido +- **Prospettiva**: strato elettro-luminescente in OLED + +--- + + + +# Grazie per l'attenzione + +Aurora Luzi · Relatore: Dr. Stefano Scurti + +--- +# Pesi molecolari dei bottle brush + +| Polimero | Mn GPC (Da) | Mw GPC (Da) | PD | Mn 1H-NMR (Da) | +|---|---|---|---|---| +| **3.1b** | 12200 | 18500 | 1,5 | 8200 | +| **3.2b** | 17300 | 22700 | 1,3 | 18000 | +| **3.3b** | 21300 | 26300 | 1,2 | 28000 | +| **3.1c** | 14000 | 18200 | 1,3 | 18200 | +| **3.2c** | 19200 | 24400 | 1,3 | 35500 | +| **3.3c** | 14500 | 19500 | 1,3 | 41300 | + +GPC (volume idrodinamico, standard di polistirene) sottostima i pesi molecolari dei polimeri ramificati. + +--- +# HOMO, LUMO e band gap elettrochimici + +| Polimero | HOMO (eV) | LUMO (eV) | Bandgap (eV) | +|---|---|---|---| +| **3a** | -5,04 | -4,07 | 0,97 | +| **3b** | -4,85 | -3,54 | 1,32 | +| **3c** | -4,80 | -3,43 | 1,37 | +| **3.1b** | -4,62 | -3,58 | 1,04 | +| **3.2b** | -4,63 | -3,53 | 1,10 | +| **3.3b** | -4,63 | -3,60 | 1,03 | +| **3.1c** | -4,77 | -3,25 | 1,52 | +| **3.2c** | -4,69 | -3,27 | 1,42 | +| **3.3c** | -4,48 | -3,55 | 0,93 |