From 705cbedee64ec976ddc398ada7d4fee85b32a700 Mon Sep 17 00:00:00 2001 From: Davide Grilli Date: Sun, 11 Oct 2026 21:40:41 +0200 Subject: [PATCH] Aggiunge cartella riassunto con riassunto_tesi.md, .docx e images Co-Authored-By: Claude Sonnet 5.5 --- riassunto/Riassunto_tesi.docx | Bin 0 -> 504492 bytes riassunto/immagini/fig-film-copolimeri-uv.jpg | Bin 0 -> 64701 bytes riassunto/immagini/fig-sistemi-fluorofori.png | Bin 0 -> 183435 bytes riassunto/immagini/fig-uv-dpp1.jpg | Bin 0 -> 61337 bytes riassunto/immagini/fig-uv-dpp2.jpg | Bin 0 -> 54903 bytes riassunto/immagini/fig1-dpp.jpg | Bin 0 -> 13200 bytes riassunto/immagini/fig2-sintesi-dpp1.jpg | Bin 0 -> 21393 bytes riassunto/immagini/fig3-alchilazione-dpp2.jpg | Bin 0 -> 21403 bytes .../immagini/fig4-copolimerizzazione.jpg | Bin 0 -> 23421 bytes riassunto/immagini/fig5-rop-bottle-brush.jpg | Bin 0 -> 32846 bytes riassunto/immagini/fig6-uv-em-3.2b.jpg | Bin 0 -> 52818 bytes riassunto/immagini/fig7-bandgap-vs-dpp.jpg | Bin 0 -> 31109 bytes riassunto/riassunto_tesi.md | 125 ++++++++++++++++++ 13 files changed, 125 insertions(+) create mode 100644 riassunto/Riassunto_tesi.docx create mode 100644 riassunto/immagini/fig-film-copolimeri-uv.jpg create mode 100644 riassunto/immagini/fig-sistemi-fluorofori.png create mode 100644 riassunto/immagini/fig-uv-dpp1.jpg create mode 100644 riassunto/immagini/fig-uv-dpp2.jpg create mode 100644 riassunto/immagini/fig1-dpp.jpg create mode 100644 riassunto/immagini/fig2-sintesi-dpp1.jpg create mode 100644 riassunto/immagini/fig3-alchilazione-dpp2.jpg create mode 100644 riassunto/immagini/fig4-copolimerizzazione.jpg create mode 100644 riassunto/immagini/fig5-rop-bottle-brush.jpg create mode 100644 riassunto/immagini/fig6-uv-em-3.2b.jpg create mode 100644 riassunto/immagini/fig7-bandgap-vs-dpp.jpg create mode 100644 riassunto/riassunto_tesi.md diff --git a/riassunto/Riassunto_tesi.docx b/riassunto/Riassunto_tesi.docx new file mode 100644 index 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zwm%gxFTeHbo3-TiS2?Rehx5Z9d92q8XV#1@trO8C%=D5Hr!7K@H{R?m|AT zL-vq?4_M=Oc|e!Cbknn%Qh}KBP*fh7YI|i**_G&MskpBsa9(`VW50ra&)%Wr36hlm zLceICWz>snUB1E1CR-raGOnSmmsQ~>FOf-3Oh|>6WD_3jg!f*3P9}89@8Lvy-~a{>7Jr2!To{SEyAep z$k~;MqvqF=^LUKWt}?ZqFP-|UU>vj)t2d=4(mk}X4d(F`G`hmc5~e-17P=2BE;$7+N;HGK8T`yUaeV}K)bFxJ=FEIg5fD37_QeBR4>tm zle-pX>RleUD8Wa)Uo77~4nD}yacZcSMHSkKq-myye5B7t0oy-`S?D`aqU&fqgGDN= zoupNrreDJvm;+A|9fx)XXRpS|?wnT_Fta4YS@4q&1mS{wF1yC#p3&7GZ2VwdVz}g` z1 Per impiegarli in un dispositivo occorre però governarne le proprietà ottiche ed elettroniche, cioè ingegnerizzare il band gap. La strategia d'elezione è l'approccio donatore-accettore (D-A), che alterna unità elettron-deficienti e unità elettron-ricche lungo lo scheletro π-coniugato: il trasferimento di carica intramolecolare che ne deriva riduce il salto energetico e permette di centrare assorbimento ed emissione nel visibile.2 + +Un limite di questi materiali è che perdono spesso le proprietà ottiche allo stato solido. La natura altamente planare dello scheletro induce intense interazioni di π-stacking tra le catene adiacenti, che causano la dissipazione non radiativa dell'energia eccitonica e lo smorzamento della fluorescenza: è l'Aggregation-Caused Quenching (ACQ). Poiché nello strato emissivo di un OLED è richiesta proprio l'emissione, l'ACQ ne limita le applicazioni pratiche. + +Come unità accettrice è stato scelto il dichetopirrolopirrolo (DPP), formato da due anelli lattamici a cinque termini condensati, con sostituenti aromatici o eteroaromatici in posizione 3 e 6 *(Figura 1)*. Il sistema biciclico lattamico a otto elettroni π conferisce a questa classe di molecole particolari proprietà chimico-fisiche: l'elevata coniugazione e la vicinanza dei piani di molecole diverse generano forti interazioni di π-stacking intermolecolari, che rendono la struttura molto stabile termicamente, mentre i forti legami a idrogeno tra le unità lattamiche favoriscono aggregati stabili, causa della scarsa solubilità nei comuni solventi organici.3 Il nucleo è planare e fortemente elettron-deficiente, e la sua rigidità limita il rilassamento vibrazionale e lo Stokes shift. Il DPP è anche molto versatile dal punto di vista chimico: i protoni ammidici sono acidi, perché l'anione che si forma è stabilizzato per risonanza, e si deprotonano con basi forti, consentendo l'N-alchilazione, che elimina i legami a idrogeno e ne aumenta la solubilità (un semplice metile la accresce di 27 volte in DMF);4 i sostituenti eteroaromatici in posizione 3 e 6 sono invece siti per bromurazione e cross-coupling, che estendono la coniugazione. + +![](immagini/fig1-dpp.jpg) + +Figura 1. Struttura generica di un dichetopirrolopirrolo. + +Sfruttare queste proprietà in un materiale richiede di partire da un monomero progettato per la polimerizzazione. Il monomero scelto è un derivato del DPP ortogonale e tetrafunzionale: gli anelli tiofenici forniscono i siti per la polimerizzazione ossidativa dello scheletro, mentre i due gruppi ossidrilici primari, portati dalle catene esiliche sugli azoti lattamici, sono gli iniziatori per la polimerizzazione ad apertura di anello (ROP). I benzeni sono sostituiti da tiofeni e i gruppi ammidici sono N-alchilati, con maggiore solubilità e una procedura semplice e scalabile. Come comonomero donatore è stato scelto il 3-esiltiofene (3HT): i politiofeni sono tra i più efficienti polimeri semiconduttori organici5 e la catena esilica aumenta la solubilità; la sua scelta deriva anche dalla collaborazione con il gruppo del Prof. Lanzi, la cui esperienza ha convalidato la polimerizzazione ossidativa su questa classe di derivati. La polimerizzazione con FeCl3 è stata preferita ai cross-coupling al palladio perché non richiede pre-funzionalizzazione dei monomeri e opera a temperatura e pressione ambiente, a fronte di un controllo minore su polidispersità e regioregolarità. La distribuzione statistica dei monomeri aumenta l'entropia conformazionale, limita il packing e rende più accessibili gli ossidrili per la funzionalizzazione. + +Resta da stabilire come legare l'unità emissiva alla matrice polimerica, scelta che influenza drasticamente le proprietà finali *(Figura 2)*. Nei sistemi host-guest il fluoroforo è disperso fisicamente nella matrice: la preparazione è semplice, ma la scarsa stabilità a lungo termine, con migrazione e aggregazione dell'ospite, porta a perdita di resa quantica. Nei sistemi cross-linked il cromoforo è ancorato da ponti chimici e non aggrega, ma l'eccessiva rigidità rende il materiale fragile, insolubile e difficile da lavorare. Nei sistemi side-chain le unità luminescenti sono catene laterali, spesso con uno spaziatore flessibile che limita le interazioni tra cromofori. Nei sistemi main-chain il fluoroforo è parte della catena principale, con sintesi più complessa; una strategia riuscita è il grafting-from, in cui un DPP bifunzionalizzato con gruppi ossidrilici inizia la crescita di due catene di poli(ε-caprolattone) (PCL) per ROP, dando PCL-DPP-PCL.6 Questa strategia è stata estesa qui innestando catene di PCL su uno scheletro semiconduttore DPP-3HT. + +![](immagini/fig-sistemi-fluorofori.png) + +Figura 2. Sistemi polimerici con inserimento di fluorofori (in verde il polimero, in rosso le unità di fluoroforo): a) host-guest, b) main-chain, c) side-chain, d) cross-linked. + +Il PCL è stato scelto per la bassa temperatura di transizione vetrosa e la buona solubilità nei solventi organici, secondo studi precedenti del gruppo. La ROP dell'ε-caprolattone catalizzata da stagno ottanoato (Sn(Oct)2) è un processo lineare ed efficiente, che permette di regolare il peso molecolare e di mantenere bassa la dispersità.7 Variando il rapporto molare monomero/ossidrili si modula la lunghezza delle catene laterali (valori nominali di 1500, 5000 e 10000 Da), così da valutarne l'effetto sterico sullo scheletro coniugato. I copolimeri sono stati alimentati con il 20%, 50% e 80% in moli di DPP; i bottle brush sono stati preparati da **3b** e **3c**, mentre **3a** non è stato usato per la scarsa efficienza della sua via sintetica. + +Lo scopo del lavoro è sintetizzare e caratterizzare copolimeri bottle brush foto-elettro attivi a base di DPP e 3HT con catene laterali di PCL, al fine di superare l'ACQ allo stato solido mantenendo l'integrità elettrochimica del nucleo DPP. L'architettura a spazzola (bottle brush) mira a separare fisicamente i segmenti planari coniugati, ripristinando le proprietà emissive allo stato solido e preservando integrità elettrochimica e stabilità del sistema. Il lavoro si articola in quattro fasi: sintesi del monomero ortogonale, copolimerizzazione ossidativa con 3HT per ottenere lo scheletro coniugato, innesto delle catene laterali di PCL e caratterizzazione dei materiali. + +Il DPP tiofenico **1** *(Figura 3)* è stato ottenuto per ciclizzazione pseudo-Stobbe tra 2-cianotiofene e diisopropil succinato.4 La base forte, il teramilato di sodio, deprotona il succinato; il carbanione attacca il nitrile e, dopo tautomerizzazione a enammina e attacco al carbonile estereo, si chiude un anello a cinque termini; una seconda sequenza analoga porta al secondo. Il succinato è stato aggiunto lentamente e si è scelto il diisopropil succinato, più ingombrato, per ridurre l'autocondensazione di Claisen.8 Il prodotto, un solido rosso scuro violaceo, è stato purificato con lavaggi in acqua e metanolo; in THF **1** ha massimo di assorbimento a 531 nm, di emissione a 542 nm e Stokes shift di 11 nm *(Figura 4)*. + +![](immagini/fig2-sintesi-dpp1.jpg) + +Figura 3. Sintesi del DPP **1** da 2-cianotiofene e diisopropil succinato con teramilato di sodio e FeCl3 catalitico. + +![](immagini/fig-uv-dpp1.jpg) + +Figura 4. Spettro UV-Visibile e di emissione del DPP **1** in THF. + +L'N-alchilazione di **1** con 6-bromo-1-esanolo *(Figura 5)* sfrutta la reattività dei gruppi ammidici, deprotonati da ter-butossido di potassio in DMSO, e dà il monomero **2** con due braccia idrossiesiliche. L'N-alchilazione è confermata nel 1H-NMR dai multipletti a 4,1 ppm (metileni legati all'azoto lattamico) e a 3,6 ppm (metileni adiacenti all'ossidrile) e nel FT-IR dalla banda dell'O-H a circa 3400 cm-1. Il massimo di assorbimento passa da 531 nm (**1**, Figura 4) a 541 nm (**2**, Figura 6): lo spostamento batocromico è attribuito all'effetto induttivo elettron-donatore delle catene alifatiche, che destabilizzano l'HOMO e restringono il band gap ottico. + +![](immagini/fig3-alchilazione-dpp2.jpg) + +Figura 5. N-alchilazione del DPP **1** con 6-bromo-1-esanolo (DMSO, ter-butossido di potassio, 40 °C) a dare il monomero **2** con due catene idrossiesiliche. + +![](immagini/fig-uv-dpp2.jpg) + +Figura 6. Spettro UV-Visibile e di emissione del monomero **2** in THF. + +Il monomero **2** è stato copolimerizzato con 3HT per via ossidativa, con FeCl3 in nitrometano e cloroformio anidro *(Figura 7)*. Il FeCl3, in eccesso stechiometrico, estrae per trasferimento mono-elettronico un elettrone dagli anelli tiofenici, generando cationi radicalici delocalizzati che formano i nuovi legami C-C. Il nitrometano modera acidità di Lewis e potere ossidante del FeCl3, prevenendo sovraossidazione e difetti di reticolazione, mentre il cloroformio anidro evita che l'acqua spenga gli intermedi cationico-radicalici. L'ossidante è stato rimosso con lavaggi acidi, perché tracce di metalli di transizione abbatterebbero la mobilità dei portatori e spegnerebbero la fluorescenza, e l'omopolimero del 3HT è stato eliminato per precipitazione in metanolo freddo. L'integrazione di DPP si è limitata a un massimo del 35% *(Tabella 1)*, per la differenza nei rapporti di reattività dei comonomeri: il tiofene, più reattivo e meno voluminoso, addiziona preferenzialmente rispetto al DPP, ingombrante. Le percentuali reali sono state determinate via 1H-NMR. + +![](immagini/fig4-copolimerizzazione.jpg) + +Figura 7. Copolimerizzazione ossidativa del DPP **2** con 3-esiltiofene con FeCl3 a dare i copolimeri **3a**, **3b** e **3c**. + +Tabella 1. Composizione dei copolimeri e pesi molecolari da GPC. + +| **Copolimero** | **% DPP teorica (mol/mol)** | **% DPP reale (mol/mol)** | **Mn (Da)** | **Mw (Da)** | **PD** | +|---|---|---|---|---|---| +| **3a** | 20 | 25,2 | 2149 | 5526 | 2,571 | +| **3b** | 50 | 32,6 | 1402 | 6439 | 4,592 | +| **3c** | 80 | 35,3 | 2134 | 4223 | 1,979 | + +I copolimeri hanno Mn tra 1402 e 2149 Da. Valori di PD intorno a 2 o superiori sono attesi per una polimerizzazione non controllata, con distribuzione più probabile di Flory.9 **3c** ha la distribuzione più omogenea (PD 1,979), mentre **3b** contiene una frazione significativa di oligomeri a catena corta accanto a macromolecole più grandi. Il FT-IR conferma l'incorporazione del DPP con il C=O lattamico a circa 1650 cm-1, e la DSC mostra una transizione vetrosa intorno a −10 °C e nessuna fusione, a conferma della natura random dei copolimeri. In soluzione di THF i tre copolimeri hanno profili ottici pressoché identici, simili a quello del monomero (assorbimento tra 540 e 544 nm, emissione intorno a 550 nm). Allo stato solido il comportamento è drasticamente diverso: l'intenso impaccamento delle catene forma aggregati che disattivano i fluorofori per decadimento non radiativo, e i film su vetrino sotto lampada UV non mostrano emissione apprezzabile *(Figura 8)*. Ciò giustifica il passaggio al design bottle brush. + +![](immagini/fig-film-copolimeri-uv.jpg) + +Figura 8. Film solidi dei copolimeri **3a**, **3b**, **3c** sotto lampada UV: l'emissione è praticamente assente. + +I sei bottle brush **3.1b**, **3.2b**, **3.3b**, **3.1c**, **3.2c** e **3.3c** sono stati ottenuti per ROP dell'ε-caprolattone dagli ossidrili di **3b** e **3c**, in toluene a 110 °C con Sn(Oct)2 catalitico, con il monomero dosato sul numero di ossidrili per ottenere catene di 1500, 5000 e 10000 Da *(Figura 9)*. L'avvenuto innesto è verificato dal 1H-NMR, con il tripletto del PCL a circa 4,0 ppm (CH2-O estereo) e dal FT-IR, in cui scompare la banda dell'O-H dei macroiniziatori e compare il C=O estereo a circa 1720 cm-1. + +![](immagini/fig5-rop-bottle-brush.jpg) + +Figura 9. Polimerizzazione ad apertura di anello dell'ε-caprolattone sui gruppi OH dei copolimeri DPP-3HT, a dare i bottle brush con catene di PCL. + +I pesi molecolari da GPC *(Tabella 2)* sono significativamente sottostimati rispetto ai teorici: la GPC separa per volume idrodinamico, relativo a standard di polistirene lineare, e un polimero altamente ramificato assume in soluzione una conformazione compatta. I dati confermano quindi indirettamente una struttura ramificata altamente impaccata e permettono il confronto tra i polimeri. Il campione **3.3c** si discosta dall'andamento generale: elevate concentrazioni locali di DPP e di ossidrili nel materiale di partenza random possono aver ridotto la crescita delle catene laterali per ingombro sterico. Il peso molecolare calcolato via 1H-NMR dal grado di polimerizzazione delle catene di PCL è più vicino ai valori teorici. La DSC mostra per tutti i bottle brush transizioni dominate dal PCL. + +Tabella 2. Pesi molecolari dei bottle brush da GPC e da 1H-NMR, con il valore teorico. + +| **Polimero** | **Mn PCL teorico (Da)** | **Mn GPC (Da)** | **PD** | **Peso molecolare teorico (Da)** | **Peso molecolare da 1H-NMR (Da)** | +|---|---|---|---|---|---| +| **3.1b** | 1500 | 12188 | 1,521 | 6500 | 8900 | +| **3.2b** | 5000 | 17302 | 1,314 | 18000 | 20500 | +| **3.3b** | 10000 | 21269 | 1,238 | 34500 | 88000 | +| **3.1c** | 1500 | 13999 | 1,301 | 10000 | 18200 | +| **3.2c** | 5000 | 19119 | 1,275 | 28500 | 35500 | +| **3.3c** | 10000 | 14445 | 1,351 | 55000 | 41300 | + +La caratterizzazione ottica in soluzione di THF mostra che la funzionalizzazione sterica non perturba l'integrità elettronica del core DPP: i massimi di assorbimento cadono tra 544 e 554 nm, quelli di emissione tra 557 e 564 nm e gli Stokes shift tra 8 e 14 nm. Le piccole fluttuazioni non seguono un andamento lineare con il peso molecolare del PCL: l'ingombro sterico non perturba livelli energetici e natura delle transizioni. Il basso Stokes shift conferma la conservazione dell'assetto planare del cromoforo, mentre i domini flessibili di PCL allontanano le catene principali. + +La caratterizzazione allo stato solido è stata condotta sul campione **3.2b**, confrontando soluzione e solido *(Figura 10)*. In soluzione si osserva la singola catena isolata; allo stato solido la vicinanza tra le macromolecole genera forti interazioni intermolecolari che alterano assorbimento ed emissione. In soluzione il massimo di assorbimento è a circa 550 nm e quello di emissione a circa 560-565 nm, con banda stretta e strutturata. Allo stato solido l'assorbimento si allarga e si sposta verso il rosso (massimo a 570-580 nm), per la planarizzazione dello scheletro, che estende la lunghezza di coniugazione effettiva. L'emissione è notevolmente allargata e fortemente spostata verso il rosso, con massimo centrato intorno a 650-660 nm e Stokes shift di circa 80-90 nm, segno di una forte aggregazione intermolecolare. Dopo la fotoeccitazione l'energia si trasferisce ai siti a energia minore, creati dalla vicinanza dei piani coniugati, e l'emissione parte soprattutto da stati aggregati o da specie eccimeriche, come descritto dall'accoppiamento eccitonico di Kasha per gli aggregati H e J.10,11 Nonostante questi riarrangiamenti, l'architettura bottle brush mantiene un'apprezzabile emissione nel rosso, attenuando i percorsi di disattivazione non radiativa tipici dell'ACQ non controllato, in accordo con il ruolo del PCL come spaziatore sterico. + +![](immagini/fig6-uv-em-3.2b.jpg) + +Figura 10. Confronto tra spettri UV-Vis (in nero) ed emissione (in rosso) del polimero **3.2b** in soluzione (linea continua) e allo stato solido (linea tratteggiata). + +Accertato che il design bottle brush preserva le proprietà ottiche, resta da verificare che non comprometta quelle elettroniche, da cui dipende il comportamento del materiale come semiconduttore. La ciclovoltammetria mostra per i polimeri un trasferimento di carica irreversibile di tipo elettrochimico-chimico, dovuto all'elevata reattività dei cationi e degli anioni radicali all'interfaccia elettrodica. Dagli onset di ossidazione e riduzione, calibrati sul ferrocene (−4,8 eV rispetto al vuoto), sono stati ricavati HOMO, LUMO e band gap elettrochimico *(Tabella 3)*. Nei copolimeri lineari si osserva un allargamento progressivo del band gap all'aumentare della frazione reale di DPP, da 0,970 a 1,371 eV *(Figura 11)*, con andamento lineare guidato soprattutto dallo spostamento del potenziale di riduzione verso valori più negativi. Ciò è interpretato come riduzione della lunghezza di coniugazione effettiva dovuta all'unità DPP, che limita la delocalizzazione π, e indica la possibilità di controllare il band gap calibrando il rapporto tra i monomeri. Nei copolimeri il DPP, forte porzione elettron-attrattrice in un'architettura D-A, stabilizza il LUMO e rende favorevole l'iniezione di elettroni, a differenza del poli-3HT, che non mostra contributi faradici in riduzione. + +![](immagini/fig7-bandgap-vs-dpp.jpg) + +Figura 11. Correlazione tra band gap elettrochimico e frazione reale di DPP nei copolimeri lineari. + +Tabella 3. Livelli HOMO, LUMO e band gap elettrochimici dei copolimeri lineari e dei bottle brush. + +| **Polimero** | **HOMO (eV)** | **LUMO (eV)** | **Bandgap (eV)** | +|---|---|---|---| +| **3a** | -5,038 | -4,068 | 0,970 | +| **3b** | -4,854 | -3,538 | 1,316 | +| **3c** | -4,799 | -3,428 | 1,371 | +| **3.1b** | -4,617 | -3,580 | 1,037 | +| **3.2b** | -4,625 | -3,527 | 1,098 | +| **3.3b** | -4,630 | -3,598 | 1,032 | +| **3.1c** | -4,774 | -3,253 | 1,521 | +| **3.2c** | -4,688 | -3,269 | 1,419 | +| **3.3c** | -4,479 | -3,550 | 0,929 | + +I bottle brush mantengono l'elettroattività dello scheletro: i processi redox avvengono a carico del core DPP-3HT, mentre i rami alifatici fungono da matrice dielettrica circostante. Le ingombranti catene laterali modificano HOMO e LUMO rispetto ai lineari, e quindi il band gap, compreso nei bottle brush tra 0,929 e 1,521 eV, per l'effetto dell'ingombro dei rami di PCL sulla coplanarità locale dello scheletro. L'ingegnerizzazione con PCL non compromette le potenzialità optoelettroniche del sistema. + +In conclusione, i risultati confermano la validità del design proposto: l'approccio ortogonale basato su scheletri semiconduttori DPP-3HT modificati con catene laterali di PCL combina proprietà elettrochimiche modulabili e capacità emissiva allo stato solido. Sono stati ottenuti tre copolimeri statistici e due serie di bottle brush con catene laterali di PCL di lunghezza nominale crescente. Il nucleo DPP conserva in soluzione le proprietà ottiche e, allo stato solido, il bottle brush **3.2b** mantiene un'apprezzabile emissione nel rosso; la composizione monomerica si rivela un parametro di controllo del band gap. I limiti 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. + +**Bibliografia** +1. Ostroverkhova, O. Organic Optoelectronic Materials: Mechanisms and Applications. *Chem. Rev.* **2016**, *116*, 13279-13412. https://doi.org/10.1021/acs.chemrev.6b00127 +2. Kroon, R.; Lenes, M.; Hummelen, J. C.; Blom, P. W. M.; de Boer, B. Small Bandgap Polymers for Organic Solar Cells (Polymer Material Development in the Last 5 Years). *Polym. Rev.* **2008**, *48*, 531-582. https://doi.org/10.1080/15583720802231833 +3. Bao, W. W.; Li, R.; Dai, Z. C.; Tang, J. X.; Shi, X.; Geng, J. T.; Deng, Z. F.; Hua, J. Diketopyrrolopyrrole (DPP)-Based Materials and Its Applications: A Review. *Front. Chem.* **2020**, *8*, 679. https://doi.org/10.3389/fchem.2020.00679 +4. Iqbal, A. F. M.; Jost, M.; Kirchmayr, R.; Pfenninger, J.; Rochat, A.; Wallquist, O. The Synthesis and Properties of 1,4-Diketo-pyrrolo[3,4-C]pyrroles. *Bull. Soc. Chim. 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