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

ABSTRACT: 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^-1 to 135.4 μV K^-1 and almost unchanged electrical conductivity, the DAE-doped PEDOT:PSS thin film achieved an extremely high power factor of 521.28 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.

SUBMITTER: Zhang J

PROVIDER: S-EPMC10858646 | biostudies-literature | 2024 Mar

REPOSITORIES: biostudies-literature

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

Zhang Jiajia J Ye Caichao C Wei Genwang G Guo Liang L Cai Yuhang Y Li Zhi Z Wu Xinzhi X Sun Fangyi F Li Qikai Q Wang Yupeng Y Li Huan H Li Yuchen Y Wang Shuaihua S Xu Wei W Guo Xuefeng X Zhang Wenqing W Liu Weishu W

National science review 20240109 3

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 photochrom ...[more]

PMID: 38344115

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Project description:Poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) is one of the most popular conducting polymers and widely used as polymer thermoelectric materials, and its thermoelectric performance could be improved by a variety of post-treatment processes. This paper reported two series of post-treatment methods to enhance the thermoelectric performance. The first series method included pre-treatment of PEDOT:PSS film with formamide, followed by imidazolium-based ionic liquids. The second series method included pre-treatment of PEDOT:PSS film with formamide, followed by sodium formaldehyde sulfoxylate, and finally imidazolium-based ionic liquids. Two series of post-treatment methods significantly improved the power factor of PEDOT:PSS when compared to that of PEDOT:PSS treated with formamide only. For example, using the first series post-treatment method with 40 vol.% ionic liquid 1-butyl-3-methylimidazolium bis(trifluoromethanesulfonyl) amide, the Seebeck coefficient of the PEDOT:PSS film increased from 14.9 to 28.5 μV/K although the electrical conductivity reduced from 2,873 to 1,701 S/cm, resulting in a substantial improvement in the overall power factor from 63.6 to 137.8 μW/K2m. The electrical conductivity enhancement in the formamide-treatment process was in part ascribed to the removal of the insulating PSS component. Further treatment of PEDOT:PSS film with ionic liquid caused dedoping of PEDOT and hence increased in Seebeck coefficient. In contrast, second series post-treatment method led to the reduction in electrical conductivity from 2,873 to 641 S/cm but a big improvement in the Seebeck coefficient from 14.9 to 61.1 μV/K and thus the overall power factor reached up to ~239.2 μW/K2m. Apart from the improvement in electrical conductivity, the increase in Seebeck coefficient is on account of the substantial dedoping of PEDOT polymer to its neutral form and thus leads to the big improvement of its Seebeck coefficient. The environmental stability of ionic liquid-treated PEDOT:PSS films were examined. It was found that the ionic liquid treated PEDOT:PSS retained more than 70% Seebeck coefficient and electrical conductivity at 75% RH humidity and 70°C for 480 h. The improved long-term TE stability is attributed to the strong ionic interaction between sulfonate anions and bulky imidazolium cations that effectively block the penetration of water and lessen the tendency to take up water from the air.

Dataset Information

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

Publications

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

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