From db3bfedd52edd6a3329c89c7e48e3d54b782af57 Mon Sep 17 00:00:00 2001 From: Davide Grilli Date: Tue, 20 Oct 2026 14:11:19 +0200 Subject: [PATCH] Elimina la cartella presentazione Co-Authored-By: Claude Sonnet 5.5 --- presentazione/discorso.md | 158 ---------- .../images/fig-film-copolimeri-uv.jpg | Bin 64701 -> 0 bytes .../images/fig-sistemi-fluorofori.png | Bin 183435 -> 0 bytes presentazione/images/fig-uv-dpp1.jpg | Bin 61337 -> 0 bytes presentazione/images/fig-uv-dpp2.jpg | Bin 54903 -> 0 bytes presentazione/images/fig1-dpp.jpg | Bin 13200 -> 0 bytes presentazione/images/fig2-sintesi-dpp1.jpg | Bin 21393 -> 0 bytes .../images/fig3-alchilazione-dpp2.jpg | Bin 21403 -> 0 bytes .../images/fig4-copolimerizzazione.jpg | Bin 23421 -> 0 bytes .../images/fig5-rop-bottle-brush.jpg | Bin 32846 -> 0 bytes presentazione/images/fig6-uv-em-3.2b.jpg | Bin 52818 -> 0 bytes presentazione/images/fig7-bandgap-vs-dpp.png | Bin 41807 -> 0 bytes presentazione/presentazione.pptx | Bin 752270 -> 0 bytes presentazione/regole.md | 17 -- presentazione/slides.md | 274 ------------------ 15 files changed, 449 deletions(-) delete mode 100644 presentazione/discorso.md delete mode 100644 presentazione/images/fig-film-copolimeri-uv.jpg delete mode 100644 presentazione/images/fig-sistemi-fluorofori.png delete mode 100644 presentazione/images/fig-uv-dpp1.jpg delete mode 100644 presentazione/images/fig-uv-dpp2.jpg delete mode 100644 presentazione/images/fig1-dpp.jpg delete mode 100644 presentazione/images/fig2-sintesi-dpp1.jpg delete mode 100644 presentazione/images/fig3-alchilazione-dpp2.jpg delete mode 100644 presentazione/images/fig4-copolimerizzazione.jpg delete mode 100644 presentazione/images/fig5-rop-bottle-brush.jpg delete mode 100644 presentazione/images/fig6-uv-em-3.2b.jpg delete mode 100644 presentazione/images/fig7-bandgap-vs-dpp.png delete mode 100644 presentazione/presentazione.pptx delete mode 100644 presentazione/regole.md delete mode 100644 presentazione/slides.md diff --git a/presentazione/discorso.md b/presentazione/discorso.md deleted file mode 100644 index 8649fa7..0000000 --- a/presentazione/discorso.md +++ /dev/null @@ -1,158 +0,0 @@ -# Discorso della presentazione - -Testo da pronunciare per la presentazione di 14 diapositive (titolo, 12 di contenuto, ringraziamenti; più 3 di scorta in fondo), pensato per **12 minuti** (limite: 12 ± 1 min) a un ritmo di circa 135 parole al minuto. Il segno **▶ CAMBIA SLIDE** indica quando passare alla diapositiva successiva. Per ogni slide sono indicati il tempo previsto e il tempo cumulativo a cui dovresti trovarti all'inizio. - -## Tabella dei tempi - -| # | Slide | Durata | Inizio | -|---|---|---|---| -| 1 | Titolo | 0:20 | 0:00 | -| 2 | Soft optoelectronics | 0:55 | 0:20 | -| 3 | ACQ | 0:50 | 1:15 | -| 4 | DPP | 0:55 | 2:05 | -| 5 | Sistemi polimerici emissivi | 0:55 | 3:00 | -| 6 | Strategia bottle brush | 0:55 | 3:55 | -| 7 | Sintesi del monomero | 1:00 | 4:50 | -| 8 | Copolimerizzazione ossidativa | 1:05 | 5:50 | -| 9 | Copolimeri lineari spenti | 0:50 | 6:55 | -| 10 | ROP: bottle brush | 1:05 | 7:45 | -| 11 | Proprietà ottiche | 1:15 | 8:50 | -| 12 | Proprietà elettrochimiche | 1:10 | 10:05 | -| 13 | Conclusioni | 0:50 | 11:15 | -| 14 | Ringraziamenti | 0:10 | 12:05 | - -Se a metà (slide 8) sei oltre 6:15, taglia le frasi tra parentesi quadre: sono pensate per essere saltabili. - ---- - -## Slide 1 · Titolo (0:00 – 0:20) - -Buongiorno a tutti, sono Aurora Luzi e presento la mia tesi magistrale, dal titolo «Sintesi e caratterizzazione di copolimeri bottle brush foto-elettro attivi». Il lavoro è stato svolto con il relatore, il dottor Stefano Scurti, e con i correlatori, il professor Massimiliano Lanzi, il dottor Simone Gabellini e il dottor Riccardo Medri. - -**▶ CAMBIA SLIDE** - -## Slide 2 · Soft optoelectronics (0:20 – 1:15) - -Il lavoro si inserisce nella soft optoelectronics, il ramo che combina emissione e rilevamento della luce con dispositivi flessibili e adattabili. I semiconduttori organici con estesi sistemi π-coniugati sono leggeri e flessibili, e si depositano da soluzione a basse temperature, con una riduzione dei costi e dell'impatto ambientale rispetto ai semiconduttori inorganici rigidi come il silicio. - -Possono convertire segnali elettrici in fotoni, come negli OLED, i diodi organici a emissione di luce, oppure fare il contrario, come nelle celle fotovoltaiche. Per usarli in un dispositivo, però, bisogna governarne le proprietà ottiche ed elettroniche, cioè ingegnerizzare il band gap. - -La strategia d'elezione è l'approccio donatore-accettore: si alternano lungo lo scheletro unità elettron-ricche e unità elettron-deficienti, e il trasferimento di carica intramolecolare che ne deriva riduce il salto energetico e porta assorbimento ed emissione nel visibile. - -**▶ CAMBIA SLIDE** - -## Slide 3 · ACQ (1:15 – 2:05) - -Questi materiali hanno però un limite importante: spesso perdono le proprietà ottiche allo stato solido. Lo scheletro è altamente planare, quindi le catene vicine tendono a impilarsi, il cosiddetto π-stacking. - -In soluzione le catene sono isolate dal solvente e il materiale emette. Allo stato solido, invece, l'energia dell'eccitone viene dissipata in modo non radiativo e la fluorescenza si smorza. Questo fenomeno si chiama Aggregation-Caused Quenching, in sigla ACQ. - -Il problema è concreto: nello strato emissivo di un OLED serve proprio l'emissione, quindi l'ACQ ne limita le applicazioni pratiche. - -**▶ CAMBIA SLIDE** - -## Slide 4 · DPP (2:05 – 3:00) - -Come unità accettrice abbiamo scelto il dichetopirrolopirrolo, il DPP, in figura. Il suo nucleo è planare, rigido e fortemente elettron-deficiente. L'elevata coniugazione e i legami a idrogeno tra le unità lattamiche danno una grande stabilità termica, ma anche una scarsa solubilità nei comuni solventi organici. - -Il DPP è però molto versatile. I protoni ammidici si possono deprotonare con basi forti, e l'N-alchilazione elimina i legami a idrogeno e aumenta la solubilità: un semplice metile la accresce di 27 volte in DMF. I sostituenti tiofenici in posizione 3 e 6 sono invece i siti per bromurazione e cross-coupling, e per la polimerizzazione dello scheletro. - -**▶ CAMBIA SLIDE** - -## Slide 5 · Sistemi polimerici emissivi (3:00 – 3:55) - -Resta da decidere come legare il fluoroforo alla matrice polimerica, e questa scelta influenza drasticamente le proprietà finali. Nei sistemi host-guest, il caso a, il fluoroforo è disperso nella matrice: è semplice, ma l'ospite migra e aggrega, e la resa quantica cala. Nei sistemi cross-linked, il caso d, il cromoforo è ancorato da ponti chimici, ma il materiale diventa fragile e insolubile. - -Restano i sistemi side-chain, caso c, e main-chain, caso b, in cui il fluoroforo è legato covalentemente. Una strategia riuscita è il grafting-from: un DPP con due gruppi ossidrilici inizia la crescita di due catene di policaprolattone, il PCL, per polimerizzazione ad apertura di anello, dando PCL-DPP-PCL. Noi abbiamo esteso questa idea a uno scheletro semiconduttore DPP-3HT, dove 3HT è il 3-esiltiofene. - -**▶ CAMBIA SLIDE** - -## Slide 6 · Strategia bottle brush (3:55 – 4:50) - -Ecco quindi la domanda di ricerca: un'architettura bottle brush, cioè a spazzola, può superare l'ACQ allo stato solido mantenendo l'integrità elettrochimica del core DPP? L'idea è che le catene laterali separino fisicamente i segmenti planari coniugati. - -Il lavoro si articola in quattro fasi: la sintesi di un monomero ortogonale derivato dal DPP; la copolimerizzazione ossidativa con 3HT per ottenere lo scheletro; l'innesto delle catene laterali di PCL per ROP dell'ε-caprolattone; e infine la caratterizzazione dei materiali. - -Il monomero è ortogonale perché porta due gruppi con ruoli indipendenti: i tiofeni fanno crescere lo scheletro con il cloruro ferrico, mentre i due ossidrili sono gli iniziatori della ROP e daranno le catene di PCL. - -**▶ CAMBIA SLIDE** - -## Slide 7 · Sintesi del monomero (4:50 – 5:50) - -Prima fase: la sintesi del monomero. Il DPP tiofenico **1** si ottiene per ciclizzazione pseudo-Stobbe tra 2-cianotiofene e diisopropil succinato. Il succinato è aggiunto lentamente, e si è scelto quello diisopropilico, più ingombrato, per ridurre l'autocondensazione di Claisen. Il prodotto è un solido rosso scuro violaceo, con assorbimento a 531 nm ed emissione a 542 nm in THF. - -Poi l'N-alchilazione con 6-bromo-1-esanolo, in DMSO con ter-butossido di potassio, dà il monomero **2**, con due braccia idrossiesiliche. L'avvenuta alchilazione è confermata dal ¹H-NMR, con i multipletti a 4,1 e 3,6 ppm, e dal FT-IR, con la banda dell'O-H a circa 3400 cm⁻¹. - -**▶ CAMBIA SLIDE** - -## Slide 8 · Copolimerizzazione ossidativa (5:50 – 6:55) - -Seconda fase: il monomero **2** viene copolimerizzato con il 3HT per via ossidativa, con cloruro ferrico in nitrometano e cloroformio anidro. Abbiamo scelto il cloruro ferrico perché non richiede la pre-funzionalizzazione dei monomeri e lavora a temperatura e pressione ambiente, a fronte di un minor controllo su polidispersità e regioregolarità. [L'ossidante è stato rimosso con lavaggi acidi, perché tracce di metalli di transizione spegnerebbero la fluorescenza.] - -Abbiamo alimentato il 20, il 50 e l'80% in moli di DPP, ma, come mostra la tabella, la percentuale reale, determinata via ¹H-NMR, è del 3, 12 e 35% e non supera il 35%: il tiofene, più reattivo e meno voluminoso, addiziona preferenzialmente rispetto al DPP, ingombrante. Le masse molecolari medie in numero sono intorno ai 2000 dalton, e i valori di PDI, tra 1,9 e 3,6, sono attesi per una polimerizzazione non controllata. - -**▶ CAMBIA SLIDE** - -## Slide 9 · Copolimeri lineari spenti (6:55 – 7:45) - -Come si comportano questi copolimeri? In soluzione di THF i tre hanno profili ottici pressoché identici a quello del monomero, con assorbimento tra 540 e 544 nm ed emissione intorno a 550 nm. - -Allo stato solido, però, il comportamento cambia drasticamente. Come si vede dai film sotto lampada UV, non c'è emissione apprezzabile: l'intenso impaccamento delle catene forma aggregati che disattivano i fluorofori. L'ACQ è quindi confermata. [La DSC non mostra alcuna transizione di fusione, a differenza del P3HT, a conferma della natura random dei copolimeri.] Questo giustifica il passaggio al design bottle brush. - -**▶ CAMBIA SLIDE** - -## Slide 10 · ROP: i bottle brush (7:45 – 8:50) - -Terza fase: dagli ossidrili di **3b** e **3c** abbiamo fatto crescere le catene di PCL per ROP dell'ε-caprolattone, in toluene a 110 °C con stagno ottanoato come catalizzatore. Dosando il monomero sul numero di ossidrili, abbiamo ottenuto catene laterali nominali di 1500, 5000 e 10000 dalton, per un totale di sei bottle brush. Il copolimero **3a** non è stato usato per la scarsa efficienza della sua via sintetica. - -L'innesto è confermato dal ¹H-NMR, con il tripletto del PCL a circa 4,0 ppm, e dal FT-IR: scompare la banda dell'O-H e compare il C=O estereo a circa 1720 cm⁻¹. - -Le masse molecolari da GPC, in tabella, sono significativamente sottostimate rispetto ai valori teorici: la GPC separa per volume idrodinamico, e un polimero molto ramificato è compatto in soluzione. Questo conferma indirettamente la struttura ramificata e altamente impaccata. L'unica eccezione è **3.3c**, che si discosta dall'andamento. - -**▶ CAMBIA SLIDE** - -## Slide 11 · Proprietà ottiche (8:50 – 10:05) - -Veniamo alla caratterizzazione ottica. In soluzione di THF tutti i bottle brush hanno assorbimento tra 544 e 554 nm, emissione tra 557 e 564 nm e Stokes shift tra 8 e 14 nm. Quindi la funzionalizzazione sterica non perturba l'integrità elettronica del core DPP, e il basso Stokes shift conferma che il cromoforo resta planare. - -Poi il passaggio decisivo: lo stato solido, studiato sul campione **3.2b**. Nel grafico la linea continua è la soluzione e quella tratteggiata il solido; in nero l'assorbimento, in rosso l'emissione. Allo stato solido l'assorbimento si sposta verso il rosso, a 570-580 nm, per la planarizzazione dello scheletro. L'emissione si allarga e si sposta a 650-660 nm, con uno Stokes shift di circa 80-90 nm: è il segno di una forte aggregazione, con stati di tipo H e J secondo il modello di Kasha. - -Nonostante questi riarrangiamenti, però, il bottle brush mantiene un'apprezzabile emissione nel rosso. Le catene di PCL agiscono da spaziatore sterico e attenuano i percorsi di disattivazione non radiativa tipici dell'ACQ. - -**▶ CAMBIA SLIDE** - -## Slide 12 · Proprietà elettrochimiche (10:05 – 11:15) - -Resta da verificare che il design bottle brush non comprometta le proprietà elettroniche, da cui dipende il comportamento da semiconduttore. Con la ciclovoltammetria, calibrata sul ferrocene, abbiamo ricavato HOMO, LUMO e band gap elettrochimico. - -Nei copolimeri lineari il band gap cresce da 0,97 a 1,37 elettronvolt all'aumentare della frazione reale di DPP, dal 3 al 35%: la crescita è marcata a basse percentuali e poi tende a un plateau, come si vede nel grafico. Il DPP riduce la lunghezza di coniugazione effettiva e stabilizza il LUMO, favorendo l'iniezione di elettroni: la composizione monomerica diventa quindi un parametro di controllo del band gap. - -Nei bottle brush il band gap è compreso tra 0,929 e 1,521 elettronvolt. I processi redox avvengono sul core DPP-3HT, mentre i rami alifatici fungono da matrice dielettrica: l'elettroattività dello scheletro è conservata. - -**▶ CAMBIA SLIDE** - -## Slide 13 · Conclusioni (11:15 – 12:05) - -Per concludere. Abbiamo ottenuto tre copolimeri statistici e due serie di bottle brush con catene di PCL di lunghezza nominale crescente. Il design proposto combina proprietà elettrochimiche modulabili e capacità emissiva allo stato solido: il bottle brush **3.2b** mantiene un'apprezzabile emissione nel rosso, e il PCL agisce da spaziatore sterico. - -I limiti del lavoro sono l'integrazione di DPP non superiore al 35%, l'esclusione di **3a** dall'innesto, la sottostima dei pesi molecolari da GPC e le discrepanze di **3.3c**, da indagare con ulteriori analisi. - -La prospettiva è l'impiego di questi materiali in dispositivi optoelettronici, in particolare come strato elettro-luminescente in OLED. - -**▶ CAMBIA SLIDE** - -## Slide 14 · Ringraziamenti (12:05 – 12:15) - -Ringrazio il relatore, i correlatori e tutti voi per l'attenzione. Sono a disposizione per le domande. - ---- - -## Durante la discussione: slide di scorta - -Dopo la slide 14 ci sono tre diapositive di scorta; per mostrarle torna indietro con le frecce o digita il numero della slide. - -| Slide | Quando usarla | -|---|---| -| 15 · UV-Vis ed emissione di **1** e **2** | domande sull'effetto dell'alchilazione: 531 → 541 nm per l'effetto induttivo donatore delle catene alifatiche, che destabilizza l'HOMO e restringe il band gap ottico | -| 16 · Pesi molecolari dei bottle brush | domande su GPC e NMR: il rapporto GPC/¹H-NMR tende a 1 con pochi siti di innesco (3.2b: 1,0) e scende fino a 0,4-0,5 con più catene laterali (3.2c, 3.3c) | -| 17 · HOMO, LUMO e band gap | domande sui valori elettrochimici dei singoli campioni | diff --git a/presentazione/images/fig-film-copolimeri-uv.jpg b/presentazione/images/fig-film-copolimeri-uv.jpg deleted file mode 100644 index f445bfbb1b9d70a3ed8fe400b9d667b558cbba11..0000000000000000000000000000000000000000 GIT binary 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zz<GgRmvjH~@B-JEzTx#1b0F7n(zO>ypqX2ozkzX`xxX*nww`;K69ddWyVL297Vi3b zjX99US#4P+f@V%(<u2MC=KgM`HtaIZF;I}qBD&3-#p(^Oub2b51cUI^s@w-CU%4~v z#echjah<upue^HKGZ64ffkp4m?X3HL`wH$xr~kFc1l8$R$6+;VqJat<aAM<T^2SSn zyEA8JWckaa{q{{s{)84h6a0Tm-XN*EeLsdjXc{bc(eCK@chYX((BKcS1M3y=jpPk- zQF!}8sXrJx{5LSJ>-hJz;O)zd{=nG^-1YTZ4*+T0?JFz(pbZG!MZ3e?-_5*zZNeYm z<rg=+zUl!W7h|_Ka{a-$khy_zow>iS!EWz@`U8g~ch}cz%z-rS_70IhXwMYyqTONc z?`GcKV(|x9N$Cps#)gaAOY_^?8U8e<R=#R}V{^mp=C@C<|7reN<*NCu)9o+C?gJ;i TfLQ?W=K~(F!c_&P`(XbEp!1d# diff --git a/presentazione/regole.md b/presentazione/regole.md deleted file mode 100644 index c3c0ecc..0000000 --- a/presentazione/regole.md +++ /dev/null @@ -1,17 +0,0 @@ -# Regole della presentazione - -## Tempi -- Esposizione dell'elaborato: 12 ± 1 min. -- Discussione con la Commissione: circa 15 min. - -## Scelte per questa presentazione -- 12 diapositive di contenuto, escluse la prima (titolo) e l'ultima (ringraziamenti): 14 diapositive in totale. - -## Modalità -- Per esporre il vostro lavoro preparate una presentazione seguendo la struttura del Riassunto della Tesi. Accertatevi di esporla entro il tempo assegnato, utilizzando 12-13 diapositive. La media è quella di un minuto per diapositiva, ma potranno esserci diapositive su cui dovrete soffermarvi più a lungo e altre che prenderanno pochi secondi. -- Per la presentazione dovrà essere utilizzato il PC d'aula. Il file deve essere in formato PowerPoint o PDF. Accertatevi in anticipo che il file sia letto correttamente, soprattutto nel caso di impiego di animazioni. -- Esponete con un ritmo scorrevole e regolare i contenuti essenziali del vostro lavoro. Lo scopo non è quello di riferire minuziosamente ogni particolare dell'attività svolta, ma solo i passaggi importanti, considerando noto ciò che appartiene alla cultura generale di un chimico industriale. -- Se nella presentazione dovete tralasciare qualche precisazione che la appesantirebbe, preparate delle diapositive di scorta da mostrare, se necessario, durante la discussione con la Commissione. -- Evitate di leggere esclusivamente i testi delle diapositive, ma curate che questi siano sintetici e limitati a 1-2 argomenti per diapositiva. Evitate il ricorso ad acronimi senza averne prima espresso il significato. -- Accertatevi che testi, didascalie e immagini siano visibili con sufficiente chiarezza ed evitate accostamenti bizzarri. Utilizzate preferibilmente i caratteri "a bastone" (ad es. Verdana, Arial) di dimensione uguale o maggiore di 18. -- La Commissione valuterà soprattutto l'originalità dell'argomento, la correttezza metodologica, il livello di approfondimento, la capacità espositiva e di presentazione dell'elaborato. diff --git a/presentazione/slides.md b/presentazione/slides.md deleted file mode 100644 index 078454f..0000000 --- a/presentazione/slides.md +++ /dev/null @@ -1,274 +0,0 @@ ---- -marp: true -theme: default -paginate: true -size: 16:9 -footer: "Aurora Luzi · Tesi magistrale in Chimica Industriale · Università di Bologna" -style: | - section { - font-family: Arial, Verdana, sans-serif; - font-size: 28px; - color: #2b2233; - background: #ffffff; - padding: 64px 70px 70px; - line-height: 1.35; - justify-content: flex-start !important; - } - section::before { - content: ""; - position: absolute; left: 0; top: 0; width: 100%; height: 12px; - background: linear-gradient(90deg, #6b1d4a, #c2415b 60%, #f08a5d); - } - h1 { color: #6b1d4a; font-size: 42px; margin: 0 0 22px; letter-spacing: -0.3px; } - h1 small { display: block; font-size: 20px; font-weight: 400; color: #c2415b; letter-spacing: 1.5px; text-transform: uppercase; margin-bottom: 4px; } - h3 { color: #c2415b; font-size: 28px; margin: 0 0 6px; } - strong { color: #6b1d4a; } - ul { padding-left: 1.1em; } - li { margin: 0.28em 0; } - li::marker { color: #c2415b; } - blockquote { - background: #fbf1f4; border-left: 6px solid #c2415b; border-radius: 0 10px 10px 0; - margin: 18px 0; padding: 12px 22px; font-size: 27px; color: #4a1636; - } - table { font-size: 22px; border-collapse: collapse; margin: 10px auto; } - th { background: #6b1d4a; color: #fff; padding: 6px 16px; } - td { padding: 5px 16px; border-bottom: 1px solid #e6d6dd; text-align: center; } - tr:nth-child(even) td { background: #faf5f7; } - img { border-radius: 6px; } - p.cap, .cap { font-size: 18px; color: #7a6a73; text-align: center; margin: 4px 0; } - footer { font-size: 16px; color: #9a8a93; } - section::after { font-size: 18px; color: #9a8a93; } - section.title { - background: linear-gradient(135deg, #3d0f2b 0%, #6b1d4a 55%, #c2415b 100%); - color: #fff; justify-content: center !important; padding: 70px 90px; - } - section.title::before { display: none; } - section.title h1 { color: #fff; font-size: 54px; line-height: 1.15; } - section.title h2 { color: #ffd7c2; font-size: 28px; font-weight: 400; margin: 0 0 40px; } - section.title p { font-size: 26px; margin: 4px 0; } - section.title strong { color: #ffd7c2; } - section.title footer, section.title::after { display: none; } - section.center { text-align: center; justify-content: center !important; } - section.center h1 { font-size: 64px; } - section.backup h1 small { color: #7a6a73; } ---- - -<!-- _class: title --> -<!-- _paginate: false --> - -## 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 -**Correlatori:** Prof. Massimiliano Lanzi · Dr. Simone Gabellini · Dr. Riccardo Medri - -Dipartimento di Chimica Industriale "Toso Montanari" · Università di Bologna - ---- - -# <small>Contesto</small>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) -- Per usarli serve **ingegnerizzare il band gap** - -> **Approccio donatore-accettore (D-A)**: unità elettron-ricche ed elettron-deficienti alternate lungo lo scheletro → trasferimento di carica intramolecolare → assorbimento ed emissione nel visibile - ---- - -# <small>Il problema</small>Aggregation-Caused Quenching (ACQ) - -Lo scheletro π-coniugato è planare: le catene vicine si impilano (**π-stacking**). - -| | In soluzione | Allo stato solido | -|---|---|---| -| Catene | isolate dal solvente | vicine, π-stacking | -| Energia eccitonica | emissione | dissipazione non radiativa | -| Fluorescenza | presente | **smorzata (ACQ)** | - -> Nello strato emissivo di un OLED serve proprio l'emissione: l'ACQ ne limita le applicazioni - ---- - -# <small>L'unità accettrice</small>Dichetopirrolopirrolo (DPP) - -![bg right:46% fit](images/fig1-dpp.jpg) - -- Nucleo **planare, rigido ed elettron-deficiente** -- π-stacking e legami a idrogeno → alta stabilità termica, ma **scarsa solubilità** -- **N-alchilazione**: elimina i legami H e aumenta la solubilità (×27 con un metile in DMF) -- Tiofeni in posizione 3 e 6: siti di **polimerizzazione** - ---- - -# <small>Come legare il fluoroforo</small>Sistemi emissivi - -![bg right:50% fit](images/fig-sistemi-fluorofori.png) - -- **Host-guest**: migrazione e aggregazione dell'ospite -- **Cross-linked**: materiale fragile e insolubile -- **Side-chain** e **main-chain**: fluoroforo legato covalentemente -- **Grafting-from**: DPP con due OH innesca la ROP del PCL → PCL-DPP-PCL -- Qui: stessa strategia su scheletro **DPP-3HT** - ---- - -# <small>Scopo</small>Strategia bottle brush - -> Una architettura **bottle brush** può superare l'ACQ allo stato solido mantenendo l'integrità elettrochimica del core DPP? - -1. **Monomero ortogonale** derivato dal DPP -2. **Scheletro** DPP-3HT per polimerizzazione ossidativa -3. **Catene laterali** di PCL per ROP dell'ε-caprolattone -4. **Caratterizzazione**: ottica, strutturale, elettrochimica - -| Gruppo del monomero | Ruolo | -|---|---| -| Tiofeni | crescita dello scheletro (FeCl<sub>3</sub>) | -| Ossidrili (OH) | iniziatori della ROP: catene di PCL | - ---- - -# <small>Fase 1</small>Sintesi del monomero ortogonale - -![w:680](images/fig2-sintesi-dpp1.jpg) - -![w:760](images/fig3-alchilazione-dpp2.jpg) - -- **1**: ciclizzazione pseudo-Stobbe, 2-cianotiofene + diisopropil succinato -- **2**: N-alchilazione con 6-bromo-1-esanolo; <sup>1</sup>H-NMR 4,1 e 3,6 ppm, FT-IR O-H ~3400 cm<sup>-1</sup> - ---- - -# <small>Fase 2</small>Copolimerizzazione ossidativa con 3HT - -![w:960](images/fig4-copolimerizzazione.jpg) - -| Copolimero | % DPP teorica | % DPP reale | Mn (Da) | PDI | -|---|---|---|---|---| -| **3a** | 20 | 3 | 2200 | 2,5 | -| **3b** | 50 | 12 | 2400 | 3,6 | -| **3c** | 80 | 35 | 2100 | 1,9 | - -- FeCl<sub>3</sub> senza pre-funzionalizzazione; **DPP incorporato al massimo 35%** (reattività dei comonomeri) - ---- - -# <small>Risultato intermedio</small>Copolimeri lineari spenti allo stato solido - -![bg right:52% fit](images/fig-film-copolimeri-uv.jpg) - -- **In THF**: assorbimento 540-544 nm, emissione ~550 nm, come il monomero -- **Film solidi** sotto lampada UV: **nessuna emissione apprezzabile** -- DSC: nessuna transizione di fusione (a differenza del P3HT) → copolimeri random - -→ ACQ confermata: serve il design **bottle brush** - ---- - -# <small>Fase 3</small>ROP dell'ε-caprolattone: i bottle brush - -![w:960](images/fig5-rop-bottle-brush.jpg) - -| Polimero | Mn PCL teorico (Da) | Mn GPC (Da) | PDI | -|---|---|---|---| -| **3.1b** · **3.1c** | 1500 | 12200 · 14000 | 1,5 · 1,3 | -| **3.2b** · **3.2c** | 5000 | 17300 · 19200 | 1,3 · 1,3 | -| **3.3b** · **3.3c** | 10000 | 21300 · 14500 | 1,2 · 1,3 | - -- Innesto: <sup>1</sup>H-NMR PCL a ~4,0 ppm; FT-IR scompare O-H, compare C=O estereo ~1720 cm<sup>-1</sup> - ---- - -# <small>Fase 4 · proprietà ottiche</small>PCL come spaziatore sterico - -![bg right:48% fit](images/fig6-uv-em-3.2b.jpg) - -**In THF** (tutti i bottle brush): assorbimento 544-554 nm, emissione 557-564 nm, Stokes shift 8-14 nm → **core DPP integro** - -**3.2b, stato solido** -- Assorbimento 570-580 nm (da ~550 nm) -- Emissione **650-660 nm**, Stokes shift ~80-90 nm -- Aggregati H e J, ma **emissione nel rosso mantenuta** - ---- - -# <small>Fase 4 · proprietà elettrochimiche</small>Band gap regolabile con la composizione - -![bg right:46% fit](images/fig7-bandgap-vs-dpp.png) - -- Ciclovoltammetria: HOMO, LUMO e **band gap elettrochimico** -- Copolimeri lineari: da **0,97 a 1,37 eV** all'aumentare del DPP reale (3 → 35%): cresce, poi tende a un plateau -- Il DPP stabilizza il LUMO e favorisce l'iniezione di elettroni -- **Bottle brush: 0,929-1,521 eV**, elettroattività conservata: redox sul core, PCL come matrice dielettrica - ---- - -# <small>Conclusioni</small>Risultati, limiti e prospettive - -### Risultati -- Tre copolimeri statistici e due serie di bottle brush con PCL di 1500, 5000 e 10000 Da -- Il **3.2b** mantiene emissione nel rosso allo stato solido: il PCL è uno **spaziatore sterico** -- Il **band gap** è controllabile dalla composizione monomerica - -### Limiti -- DPP ≤ 35%; 3a escluso dall'innesto; GPC sottostima i pesi molecolari; 3.3c da approfondire - -### Prospettive -- Strato elettro-luminescente in **OLED** - ---- - -<!-- _class: center --> -<!-- _paginate: false --> - -# Grazie per l'attenzione - -Aurora Luzi - ---- - -<!-- _class: backup --> - -# <small>Diapositive di scorta</small>UV-Vis ed emissione dei DPP 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 (effetto induttivo delle catene alifatiche) - ---- - -<!-- _class: backup --> - -# <small>Diapositive di scorta</small>Bottle brush: pesi molecolari - -| Polimero | Mn PCL teorico (Da) | Mn GPC (Da) | PDI | Mn <sup>1</sup>H-NMR (Da) | Rapporto GPC/<sup>1</sup>H-NMR | -|---|---|---|---|---|---| -| **3.1b** | 1500 | 12200 | 1,5 | 8200 | 1,5 | -| **3.2b** | 5000 | 17300 | 1,3 | 18000 | 1,0 | -| **3.3b** | 10000 | 21300 | 1,2 | 28000 | 0,8 | -| **3.1c** | 1500 | 14000 | 1,3 | 18200 | 0,8 | -| **3.2c** | 5000 | 19200 | 1,3 | 35500 | 0,5 | -| **3.3c** | 10000 | 14500 | 1,3 | 41300 | 0,4 | - -GPC (standard di polistirene lineare): con pochi siti di innesco i valori sono coerenti con l'NMR (rapporto verso 1); con più catene laterali la GPC sottostima, perché i polimeri ramificati sono compatti in soluzione. - ---- - -<!-- _class: backup --> - -# <small>Diapositive di scorta</small>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 |