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Synthetic nuances to maximize n-type organic electrochemical transistor and thermoelectric performance in fused lactam polymers
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Marks, Adam, Chen, Xingxing, Wu, Ruiheng, Rashid, Reem B., Jin, Wenlong, Paulsen, Bryan D., Moser, Maximilian, Ji, Xudong, Griggs, Sophie, Meli, Dilara, Wu, Xiaocui, Bristow, Helen, Strzalka, Joseph, Gasparini, Nicola, Costantini, Giovanni, Fabiano, Simone, Rivnay, Jonathan and McCulloch, Iain (2022) Synthetic nuances to maximize n-type organic electrochemical transistor and thermoelectric performance in fused lactam polymers. Journal of the American Chemical Society, 144 (10). pp. 4642-4656. doi:10.1021/jacs.2c00735 ISSN 0002-7863.
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WRAP-Synthetic-nuances-to-maximise-n-type-organic-electrochemical-transistor-Wu-2022.pdf - Accepted Version - Requires a PDF viewer. Download (1320Kb) | Preview |
Official URL: http://dx.doi.org/10.1021/jacs.2c00735
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.
Item Type: | Journal Article | ||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||
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Subjects: | Q Science > QC Physics Q Science > QD Chemistry Q Science > QH Natural history |
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Divisions: | Other > Institute of Advanced Study Faculty of Science, Engineering and Medicine > Science > Chemistry |
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Library of Congress Subject Headings (LCSH): | Organic electrochemical transistors, Lactams, Polymers, Electron transport, Bioelectronics | ||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||
Journal or Publication Title: | Journal of the American Chemical Society | ||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||
Publisher: | American Chemical Society | ||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||
ISSN: | 0002-7863 | ||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||
Official Date: | 16 March 2022 | ||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||
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Volume: | 144 | ||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||
Number: | 10 | ||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||
Page Range: | pp. 4642-4656 | ||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||
DOI: | 10.1021/jacs.2c00735 | ||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||
Status: | Peer Reviewed | ||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||
Publication Status: | Published | ||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||
Reuse Statement (publisher, data, author rights): | This document is the Accepted Manuscript version of a Published Work that appeared in final form in Journal of the American Chemical Society, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://pubs.acs.org/doi/abs/10.1021/jacs.2c00735. | ||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||
Access rights to Published version: | Restricted or Subscription Access | ||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||
Copyright Holders: | American Chemical Society | ||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||
Date of first compliant deposit: | 30 March 2022 | ||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||
Date of first compliant Open Access: | 8 March 2023 | ||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||
RIOXX Funder/Project Grant: |
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