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N-doping semiconductive polymer by methoxy-modified JLBI towards optimized miscibility and Coulomb interactions for high thermoelectric performance
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2024-12-20 , DOI: 10.1039/d4ta07144a Dingchang Su, Chun Zhan, Yang Xiang, Wei Wang, Chenglong Li, Qisheng Zhou, Defu Dong, Shengqiang Xiao
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2024-12-20 , DOI: 10.1039/d4ta07144a Dingchang Su, Chun Zhan, Yang Xiang, Wei Wang, Chenglong Li, Qisheng Zhou, Defu Dong, Shengqiang Xiao
Molecular doping of n-type polymers creates Coulombically bound charge carriers or counterion pairs via a charge-transfer process. Synergistic optimization of the miscibility and free charge carriers release within a specific polymer:n-dopant pair poses a formidable challenge for high-performance n-type organic thermoelectrics. In this work, the density of free charge carriers and the thermoelectric properties are greatly enhanced in the n-doped benchmark semiconductive polymer N2200 by harnessing a novel n-dopant of 9-(1,3-dimethyl-2,3-dihydro-1H-benzo[d]imidazol-2-yl)-8-methoxy-julolidine (MeO-JLBI), which derived from our previously reported JLBI molecule by employing the lipophilicity of julolidine group and the electron-donating characteristic of MeO group. As contrast to the N2200 films doped with the common benzimidazoline n-dopant of N-DMBI and JLBI, which have very similar low performance, the MeO-JLBI doped one exhibits ∼4 times higher free-charge carrier density and ~10 times higher conductivity (1.02 × 10-2 S cm-1), ultimately leading to a ~5 times higher room temperature power factor of 3.54 × 10-2 μW m-1 K-2 at optimized conditions, among the highest values for the doped N2200 films to date. Experimental findings demonstrate that MeO group enhances the driving force on charge transfer, reduces the Coulomb interactions between the counterion pairs in the doped state, and consequently generates free charges more easily while maintaining the similar enhanced miscibility with N2200 as that of JLBI. This study offers an approach that synergistically utilizes electron-donating and lipophilic effects to tackle the requirements of high miscibility, charge transfer driving force, and reduced Coulomb interactions in n-doped polymers for thermoelectrics.
更新日期：2024-12-20
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