Synthetic Nuances to Maximize n-Type Organic Electrochemical Transistor and Thermoelectric Performance in Fused Lactam Polymers.
Synthetic Nuances to Maximize n-Type Organic Electrochemical Transistor and Thermoelectric Performance in Fused Lactam Polymers.
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DOI：
10.1021/jacs.2c00735
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发表时间：
2022-03-16
影响因子：
15
通讯作者：
McCulloch, Iain
中科院分区：
文献类型：
--
作者：
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;McCulloch, Iain
通过廉价、无毒、无贵金属的羟醛缩聚反应，系统增加烷基侧链含量，合成了一系列全熔融n型混合导电内酰胺聚合物p(G7NCnN)。将这些聚合物用作有机电化学晶体管中的沟道材料提供了最先进的n型性能，p(G7NC10N)记录的电子迁移率为1.2 0×10-2cm2 V-1 S-1，μC*优值系数为1.83F cm-1V-1 S-1。与高的光电转换性能平行，当溶液掺杂DMBI(N-DMBI)时，观察到p(G7NC4N)的最高热电性能，最大电导率为7.67 S cm-1，功率因数为10.4μWm-1K-2。这些结果是已报道的n型聚合物中最高的。重要的是，虽然这一系列熔融聚内酰胺有机混合离子-电子导体(OMIEC)强调了提高OECT性能的合成分子设计策略可以转化为实现高有机热电(OTE)性能，但必须使用细微差别的合成方法来优化性能。在这里，我们概述了性能指标，并为下一代用于混合导电应用的高性能n型材料的分子设计指南提供了新的见解，首次展示了在OECT和OTE应用中单一聚合物系列的结果。
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.
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影响因子：
16.6
作者：
Inal S;Malliaras GG;Rivnay J
通讯作者：
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影响因子：
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作者：
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DOI：
10.1073/pnas.1510231112
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通讯作者：
Müller C