From 48ce234789fdf64c437770e2e74c513930d718e1 Mon Sep 17 00:00:00 2001 From: Davide Grilli Date: Sun, 18 Oct 2026 11:24:14 +0200 Subject: [PATCH] Aggiorna bibliografia e citazioni del riassunto (IUPAC, Jarosz) e porta il docx a 10 pagine Rinumera le voci 6-8, aggiunge le voci 9 (Gritzner e Kuta, IUPAC) e 10 (Jarosz et al., P3HT) sia nel md sia nel docx, con il rimando 9 dopo il valore del ferrocene. Nel docx riduce le figure all'80% per stare in 10 pagine escluso il frontespizio. Co-Authored-By: Claude Sonnet 5.5 --- riassunto/riassunto_tesi.docx | Bin 1079517 -> 1072019 bytes riassunto/riassunto_tesi.md | 20 ++++++++++++-------- 2 files changed, 12 insertions(+), 8 deletions(-) diff --git a/riassunto/riassunto_tesi.docx b/riassunto/riassunto_tesi.docx index bea86bad027661edf7ae92df8c743ec3940f129a..8803ce7ff3ad670ad17ec09fbcbfa252b8b6913a 100644 GIT binary patch delta 100672 zcmY&fQ*`G|kj=!&#P)=fWMbPk|FLabzi5(7>||owwrxyo+xC9DZ~IWyefpsv>fBSO z``%j{H$n-`LV%(S1SAF+7#Qq-K>|j-FGU3b4hFV`00xHs--)(}y`77xor}Jzr-P}p zF1?4X&0vaL#2OlGNF)?WL7vf z{BO{O%Q$0QOOVTHv}|?f)^ED#AjX}}S>;%_k>(P;;7A=!E4Z=ID5!#UTo0WpA+)_t zpPB>UdskDGKA)BNtMy{nX{DxjiF~5RIfLcqlR6~hjVp^l13R+8iT@^~f)EzS*k_X1Jt(t#JnvO*b_U?d2B zy5>D;VprffNAiRqHy@*XHW!8h3`81A=Ba21B`lP>zL^81-+&}_t9@gtREm<>?GTwaUw)vGZExvYM-ZvC%K;KJM_EV>~-qDuxl@Jk^CNK!p41{6AZu{ zso*rM_j+gr{C@QOxDi7<)G2Us0=#$UesfH`c-+{ONqpv6tE5nMbbI+ZaC&;xy?j2I zd?NpU+z`d#HJ|>67y19N^Zmb7-^tX*nSuU)b7g$5Gz8OscnQ2hIo!;&g+jG#!bbH% 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ze&_y=9-FuFQNLQ~i6Hcx1?{;1FQbotaESipqJP1^`aemugMU5*UgvF1z?QBSB5Wq9|3lNH}Lrs-c-uMPV;y}uw!T~<6Y+r9AP8x|4c zTjB|?PaZW9!lBc=OTV}tdT-@Z)wx5@ z3C2~-$=ePivFWAb{>Ole2QjL2LE;FFA~ioCLevEDB4+%YZqgG^!zMtto3-r*xx0JE zILuscbPZfJoIN*Nsu1i5V=rl>j@9UtbJV1aR@qmH|01kWZp~vKPB2-DPP_wZH#yql z=Hy2o0l9rAYh3iuiTu%bWr`1ZEnF2T*U)e3Uv6n*Sd>(*(_H4hO-vDLbLJ;@V%o*` z%Posb$7m7^%i7JbY7X@CGEW&U25QdiPcezLcrGTWVfNZ;Xc_j~9uN^DAy@Br)QQk% zEkQcSA`Czl0h(q5exGm!WkF+o1h>U+K(1J}@>!@<4+4g!zIP-|CM)6UgPOmyS- z%&FZRP!p5-S`d;HJpgd*Kmz~=3b0)taghHv3+gPvtJwhnfNCItW(Ibqc`A_80KvWm z=~9>zgokK0L6U6PvF%hJ2AUfnIJO|EA0)#bL6CJ2!*K`loQ3e{XtTM{s-?0M3OXk zZ_|D|35FPNO3E7yzA{GeY}I}9s5oY5_~o;=?jwBA!CeS;f!{i}J34Hqz{HA(%~&y! zy>;9hA+?R9rUb^C?08A`h7fE+s;YtSOc1PFV*Fm1{|+he#&~f%EgB%et49%xe~7VX zd3hTH@G%0~qWjvd^zZlJyyVn6hnIAB0WGlT%SuiM5q;y*g51t92) è un processo controllato, che permette di regolare il peso molecolare e di mantenere bassa la dispersità.7 Le catene laterali di PCL sono state sintetizzate con lunghezze differenti (raggiungendo pesi molecolari di 1500, 5000 e 10000 Da), così da poterne valutare l'effetto sterico sullo scheletro coniugato. +Poiché le semplici dispersioni fisiche (host-guest) e i sistemi reticolati (cross-linked) limitano rispettivamente la stabilità nel tempo e la processabilità, l’inserzione covalente risulta preferibile. Nei sistemi side-chain il fluoroforo pende come catena laterale, mentre nei sistemi main-chain è integrato direttamente nello scheletro principale. Tra questi ultimi, una strategia particolarmente efficace sfrutta l'approccio grafting-from, in cui la molecola di partenza funge da iniziatore da cui le nuove catene polimeriche crescono direttamente verso l'esterno. Applicando questo principio, un DPP bifunzionalizzato avvia la polimerizzazione ROP di poli(ε-caprolattone) (PCL), generando architetture PCL-DPP-PCL. 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 controllato, che permette di regolare il peso molecolare e di mantenere bassa la dispersità.6 Le catene laterali di PCL sono state sintetizzate con lunghezze differenti (raggiungendo pesi molecolari di 1500, 5000 e 10000 Da), così da poterne valutare l'effetto sterico sullo scheletro coniugato. Lo scopo di questo lavoro di ricerca è stato 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 della catena polimerica coniugata. 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 **1** è stato ottenuto per ciclizzazione pseudo-Stobbe tra 2-cianotiofene e diisopropil succinato (**Figura 4**).4 La base forte, il ter-amilato 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 ed è stato scelto il diisopropil succinato, più ingombrato, per ridurre l'autocondensazione di Claisen.8 +Il DPP **1** è stato ottenuto per ciclizzazione pseudo-Stobbe tra 2-cianotiofene e diisopropil succinato (**Figura 4**).4 La base forte, il ter-amilato 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 ed è stato scelto il diisopropil succinato, più ingombrato, per ridurre l'autocondensazione di Claisen.7 ![](immagini/image4.jpg) @@ -125,7 +125,7 @@ Figura 10 – **sinistra**: confronto tra spettri UV-Vis (in nero) ed emissione **destra**: film solidi dei polimeri bottle brush sintetizzati sotto lampada Kessil (456 nm) -Allo stato solido, invece, l'assorbimento ed emissione mostrano spettri più allargati, con massimi a 570-580 nm e 650-660 nm, rispettivamente. Lo *Stokes shift* è di circa 80-90 nm, segno di forte aggregazione (**Figura 10-sinistra**): l'energia migra verso siti a energia minore, creati dalla vicinanza dei piani coniugati, e l'emissione parte da stati aggregati o specie eccimeriche.9 +Allo stato solido, invece, l'assorbimento ed emissione mostrano spettri più allargati, con massimi a 570-580 nm e 650-660 nm, rispettivamente. Lo *Stokes shift* è di circa 80-90 nm, segno di forte aggregazione (**Figura 10-sinistra**): l'energia migra verso siti a energia minore, creati dalla vicinanza dei piani coniugati, e l'emissione parte da stati aggregati o specie eccimeriche.8 Nonostante ciò, il *bottle brush* mantiene un'apprezzabile emissione nel rosso, in accordo con il ruolo del PCL come spaziatore sterico. L'effetto dipende dalla lunghezza delle catene laterali: nei film quelle più lunghe preservano un'intensa emissione, mentre con le più corte (3 kDa) l'ingombro non è sufficiente e la fluorescenza non è apprezzabile, portando ad un comportamento analogo ai copolimeri lineari DPP-3HT (**Figura 10-destra**). @@ -135,7 +135,7 @@ Per verificare che l'ingombro sterico del design *bottle brush* non alterasse le Figura 11 - Voltammogramma ciclico del polimero 3.2c registrato a una velocità di scansione di 0.05 V/s -Tale analisi ha evidenziato un trasferimento di carica irreversibile di tipo elettrochimico-chimico, legato all'elevata reattività delle specie radicaliche (cationi e anioni) all'interfaccia elettrodica; inoltre, dai relativi *onset* di ossidazione e riduzione calibrati sul ferrocene (−4,8 eV), è stato possibile calcolare i livelli di frontiera HOMO e LUMO ed il *band gap* elettrochimico. +Tale analisi ha evidenziato un trasferimento di carica irreversibile di tipo elettrochimico-chimico, legato all'elevata reattività delle specie radicaliche (cationi e anioni) all'interfaccia elettrodica; inoltre, dai relativi *onset* di ossidazione e riduzione calibrati sul ferrocene (−4,8 eV)9, è stato possibile calcolare i livelli di frontiera HOMO e LUMO ed il *band gap* elettrochimico. Per il monomero **2** l’*energy gap* è 2,01 eV; nei copolimeri lineari **3a**, **3b** e **3c** scende a 0,97-1,37 eV e cresce con la frazione reale di DPP (*χ**DPP**)* (**Figura 12**), con andamento che sembra tendere a un plateau, soprattutto per lo spostamento del potenziale di riduzione verso valori più negativi: il DPP riduce la lunghezza di coniugazione effettiva, per cui il rapporto tra i monomeri controlla il *band gap*. Rispetto al P3HT (LUMO −2,73 eV), il DPP, forte elettron-attrattore, stabilizza il LUMO e rende favorevole l'iniezione di elettroni; all'interno della serie, però, il LUMO sale con *χ*DPP (da −4,07 a −3,43 eV), coerentemente con la minore lunghezza di coniugazione effettiva. @@ -174,8 +174,12 @@ In conclusione, i risultati ottenuti confermano la validità del design molecola 5. Abdel Aziz, I.; Tullii, G.; Antognazza, M. R.; Criado-Gonzalez, M. Poly(3-hexylthiophene) as a Versatile Semiconducting Polymer for Cutting-Edge Bioelectronics. *Mater. 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