Organic superbase-induced polaron modulation enables high thermoelectric performance in solid PEDOT:PSS films.

Authors

Zhijun Chen, Yonggang Zhao, Cheng Xu, Qiujian Le, Yu Wu, Liyao Liu, Jianyong Ouyang

Published in

Materials horizons. Sep 16, 2026. Epub Sep 16, 2026.

Abstract

Organic thermoelectric (TE) materials are attractive for sustainable energy harvesting owing to their mechanical flexibility, low cost, and intrinsically low thermal conductivity. Among them, PEDOT:PSS is one of the most promising candidates. However, its relatively low Seebeck coefficient limits further improvement in TE performance. Here, we demonstrate that treatment with the organic superbase 1-tert-butyl-2,2,4,4,4-pentakis(dimethylamino)-2λ⁵,4λ⁵-catenadi(phosphazene) (P2-t-Bu) of PEDOT:PSS films can enhance the Seebeck coefficient and preserve high electrical conductivity. A PEDOT:PSS film sequentially treated with H₂SO₄ and P2-t-Bu can exhibit a Seebeck coefficient of 81.7 µV K^-1, an electrical conductivity of 1265.3 S cm^-1, and a low thermal conductivity of 0.42 W m^-1 K^-1, yielding a power factor of 845.3 µW m^-1 K^-2 and a high room-temperature ZT value of 0.60 for solid organic thermoelectric materials. Spectroscopic and electronic structure analyses reveal that the exceptional TE performance originates from synergistic dedoping and lower-polaron-level splitting induced by the coupling between the polarons of PEDOT and the lone electron pairs of P2-t-Bu. This work establishes organic superbase engineering as an effective strategy for high-performance organic thermoelectrics.

PMID:
42747270
Bibliographic data and abstract were imported from PubMed on 16 Sep 2026.

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