The Critical Role of Dopant Cations in Electrical Conductivity and Thermoelectric Performance of n-Doped Polymers

化学 掺杂剂 兴奋剂 热电效应 电阻率和电导率 聚合物 热电材料 电导率 导电聚合物 化学工程 高分子化学 无机化学 物理化学 凝聚态物理 有机化学 热力学 电气工程 物理 工程类
作者
Yang Lu,Zi‐Di Yu,Yi Liu,Yifan Ding,Jing Wang,Ze‐Fan Yao,Ziyuan Wang,Hao‐Yang You,Hao Chen,Bo Tang,Jie‐Yu Wang,Jian Pei
出处
期刊:Journal of the American Chemical Society [American Chemical Society]
卷期号:142 (36): 15340-15348 被引量:120
标识
DOI:10.1021/jacs.0c05699
摘要

The low n-doping efficiency of conjugated polymers with the molecular dopants limits their availability in electrical conductivity, thermoelectrics, and other electric applications. Recently, considerable efforts have focused on improving the ionization of dopants by modifying the structures of host polymers or n-dopants; however, the effect of ionized dopants on the electrical conductivity and thermoelectric performance of the polymers is still a puzzle. Herein, we try to reveal the role of molecular dopant cations on carrier transport through the systematic comparison of two n-dopants, TAM and N-DMBI-H. These two n-dopants exhibit various doping features with the polymer due to their different chemical structure characteristics. For instance, while doping, TAM negligibly perturbs the polymer backbone conformation and microstructural ordering; then after ionization, TAM cations possess weak π-backbone affinity but strong intrinsic affinity with side chains, which enables the doped system to screen the Coulomb potential spatially. Such doping features lead to high carrierization capabilities for TAM-doped polymers and further result in an excellent conductivity of up to 22 ± 2.5 S cm–1 and a power factor of over 80 μW m–1 K–2, which are significantly higher than the state of the art values of the common n-dopant N-DMBI-H. More importantly, this strategy has also proven to be widely applicable in other doped polymers. Our investigations indicate the vital role of dopant counterions in high electrical and thermoelectric performance polymers and also suggest that, without sacrificing Seebeck coefficients, high conductivities can be realized with precise regulation of the interaction between the cations and the host.
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