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Synthetic Nuances to Maximize n-Type Organic Electrochemical Transistor and Thermoelectric Performance in Fused Lactam Polymers.


ABSTRACT: A series of fully fused n-type mixed conduction lactam polymers p(g7NCnN), systematically increasing the alkyl side chain content, are synthesized via an inexpensive, nontoxic, precious-metal-free aldol polycondensation. Employing these polymers as channel materials in organic electrochemical transistors (OECTs) affords state-of-the-art n-type performance with p(g7NC10N) recording an OECT electron mobility of 1.20 × 10-2 cm2 V-1 s-1 and a μC* figure of merit of 1.83 F cm-1 V-1 s-1. In parallel to high OECT performance, upon solution doping with (4-(1,3-dimethyl-2,3-dihydro-1H-benzoimidazol-2-yl)phenyl)dimethylamine (N-DMBI), the highest thermoelectric performance is observed for p(g7NC4N), with a maximum electrical conductivity of 7.67 S cm-1 and a power factor of 10.4 μW m-1 K-2. These results are among the highest reported for n-type polymers. Importantly, while this series of fused polylactam organic mixed ionic-electronic conductors (OMIECs) highlights that synthetic molecular design strategies to bolster OECT performance can be translated to also achieve high organic thermoelectric (OTE) performance, a nuanced synthetic approach must be used to optimize performance. Herein, we outline the performance metrics and provide new insights into the molecular design guidelines for the next generation of high-performance n-type materials for mixed conduction applications, presenting for the first time the results of a single polymer series within both OECT and OTE applications.

SUBMITTER: Marks A 

PROVIDER: S-EPMC9084553 | biostudies-literature | 2022 Mar

REPOSITORIES: biostudies-literature

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Synthetic Nuances to Maximize n-Type Organic Electrochemical Transistor and Thermoelectric Performance in Fused Lactam Polymers.

Marks Adam A   Chen Xingxing X   Wu Ruiheng R   Rashid Reem B RB   Jin Wenlong W   Paulsen Bryan D BD   Moser Maximilian M   Ji Xudong X   Griggs Sophie S   Meli Dilara D   Wu Xiaocui X   Bristow Helen H   Strzalka Joseph J   Gasparini Nicola N   Costantini Giovanni G   Fabiano Simone S   Rivnay Jonathan J   McCulloch Iain I  

Journal of the American Chemical Society 20220308 10


A series of fully fused n-type mixed conduction lactam polymers <b>p(g</b><sub><b>7</b></sub><b>NC</b><i><sub><b>n</b></sub></i><b>N)</b>, systematically increasing the alkyl side chain content, are synthesized via an inexpensive, nontoxic, precious-metal-free aldol polycondensation. Employing these polymers as channel materials in organic electrochemical transistors (OECTs) affords state-of-the-art n-type performance with <b>p(g</b><sub><b>7</b></sub><b>NC</b><sub><b>10</b></sub><b>N)</b> recor  ...[more]

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