期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 144, 期 10, 页码 4642-4656出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.2c00735
关键词
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资金
- KAUST
- Office of Sponsored Research (OSR) award [OSR-2018-CRG/CCF-3079, OSR-2019CRG8-4086, OSR-2018-CRG7-3749]
- ERC Synergy Grant SC2 [610115]
- European Union [952911, 862474, 945380]
- EPSRC [EP/T026219/1]
- NSF [DMR-1751308]
- National Science Foundation [NSF DMR-1751308]
- DOE Office of Science [DE-AC02-06CH11357]
- SHyNE Resource [NSF ECCS-1542205]
- IIN
- Northwestern's MRSEC program [NSF DMR-1720139]
- Swedish Research Council [202003243]
- European Commission through the Marie Sklodowska-Curie project HORATES [GA-955837]
- Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linkoping University (Faculty Grant) [SFO-Mat-LiU 2009-00971]
A series of fully fused lactam polymers with increased alkyl side chain content were synthesized via an inexpensive and non-toxic method. These polymers showed state-of-the-art n-type performance in organic electrochemical transistors (OECTs) and high thermoelectric performance when solution-doped.
A series of fully fused n-type mixed conduction lactam polymers p(g(7)NC(n)N), 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(g(7)NC(10)N) recording an OECT electron mobility of 1.20 x 10(-2) cm(2) V-1 s(-1) and a mu C* 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(g(7)NC(4)N), with a maximum electrical conductivity of 7.67 S cm(-1) and a power factor of 10.4 mu Wm(-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.
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