High Thermoelectric Performance in Solution‐Processed Semicrystalline PEDOT:PSS Films by Strong Acid–Base Treatment: Limitations and Potential

Author:

Park Juhyung1,Jang Jae Gyu2,Kang Keehoon3ORCID,Kim Sung Hyun2,Kwak Jeonghun1ORCID

Affiliation:

1. Department of Electrical and Computer Engineering Inter‐University Semiconductor Research Center Soft Foundry Institute Seoul National University Seoul 08826 Republic of Korea

2. Department of Carbon Convergence Engineering Wonkwang University Iksan 54538 Republic of Korea

3. Department of Materials Science and Engineering Research Institute of Advanced Materials Institute of Applied Physics Seoul National University Seoul 08826 Republic of Korea

Abstract

AbstractThermoelectric (TE) generation with solution‐processable conducting polymers offers substantial potential in low‐temperature energy harvesting based on high tunability in materials, processes, and form‐factors. However, manipulating the TE and charge transport properties accompanies structural and energetic disorders, restricting the enhancement of thermoelectric power factor (PF). Here, solution‐based strong acid–base treatment techniques are introduced to modulate the doping level of poly(3,4‐ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) thin films with preserving its molecular orientation, enabling to achieve a remarkably high PF of 534.5 µW m−1 K−2. Interestingly, theoretical modeling suggested that further de‐doping can increase the PF beyond the experimental value. However, it is impossible to reach this value experimentally, even without any degradation of PEDOT crystallinity. Uncovering the underlying reason for the limitation, an analysis of the relationship among the microstructure–thermoelectric performance–charge transport property revealed that inter‐domain connectivity via tie‐chains and the resultant percolation for transport are crucial factors in achieving high TE performance, as in charge transport. It is believed that the methods and fundamental understandings in this work would contribute to the exploitation of conducting polymer‐based low‐temperature energy harvesting.

Funder

Ministry of Science and ICT, South Korea

Ministry of Education

Publisher

Wiley

Subject

General Physics and Astronomy,General Engineering,Biochemistry, Genetics and Molecular Biology (miscellaneous),General Materials Science,General Chemical Engineering,Medicine (miscellaneous)

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