Polaron interfacial entropy as a route to high thermoelectric performance in DAE-doped PEDOT:PSS films

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外文摘要：Enhancing the thermoelectric transport properties of conductive polymer materials has been a long-term challenge,in spite of the success seen with molecular doping strategies.However,the strong coupling between the thermopower and the electrical conductivity limits thermoelectric performance.Here,we use polaron interfacial occupied entropy engineering to break through this intercoupling for a PEDOT:PSS(poly(3,4-ethylenedioxythiophene)-poly(4-styrenesulfonate))thin film by using photochromic diarylethene(DAE)dopants coupled with UV-light modulation.With a 10-fold enhancement of the thermopower from 13.5 μV K-1to 135.4 μV K-1 and almost unchanged electrical conductivity,the DAE-doped PEDOT:PSS thin film achieved an extremely high power factor of521.28 µW m-1 K-2 from an original value of 6.78 μW m-1 K-2.The thermopower was positively correlated with the UV-light intensity but decreased with increasing temperature,indicating resonant coupling between the planar closed DAE molecule and PEDOT.Both the experiments and theoretical calculations consistently confirmed the formation of an interface state due to this resonant coupling.Interfacial entropy engineering of polarons could play a critical role in enhancing the thermoelectric performance of the organic film.

外文关键词：

thermoelectricPEDOT:PSSinterfacial occupied entropyresonant couplingUV-light modulation

作者：

Jiajia Zhang、Caichao Ye、Genwang Wei、Liang Guo、Yuhang Cai、Zhi Li、Xinzhi Wu、Fangyi Sun、Qikai Li、Yupeng Wang、Huan Li、Yuchen Li、Shuaihua Wang、Wei Xu、Xuefeng Guo、Wenqing Zhang、Weishu Liu

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作者单位：

Department of Materials Science and Engineering,Southern University of Science and Technology,Shenzhen 518055,China

Academy for Advanced Interdisciplinary Studies and Guangdong Provincial Key Laboratory of Computational Science and Material Design,Southern University of Science and Technology,Shenzhen 518055,China

Department of Mechanical and Energy Engineering,Southern University of Science and Technology,Shenzhen 518055,China

Beijing National Laboratory for Molecular Sciences,Key Laboratory of Organic Solids,Institute of Chemistry,Chinese Academy of Sciences,Beijing 100190,China

College of Chemistry and Molecular Engineering,National Biomedical Imaging Centre,Peking University,Beijing 100091,China

Guangdong Provincial Key Laboratory of Functional Oxide Materials and Devices,Southern University of Science and Technology,Shenzhen 518055,China

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基金：

Center for Computational Science and Engineering at the Southern University of science and TechnologyShenzhen Innovation Program for Distinguished Young Scholars国家重点研发计划Guangdong Provincial Key Laboratory of Computational Science and Material DesignGuangdong Innovation Research Team ProjectTencent Foundation through the Xplorer Prize

项目编号：

RCJC202107060919490182022YFA12034002019B0303010012017ZT07C062

出版年：

2024

DOI：

10.1093/nsr/nwae009

国家科学评论(英文版)

CSTPCD

ISSN：

年,卷(期)：2024.11(3)

参考文献量64