A New Polystyrene-Poly(vinylpyridinium) Ionic Copolymer Dopant for n-Type All-Polymer Thermoelectrics with High and Stable Conductivity Relative to the Seebeck Coefficient giving High Power Factor

Jinfeng Han; Emma Tiernan; Taein Lee; Arlene Chiu; Patty McGuiggan; Nicholas Adams; John A Tomko; Patrick E Hopkins; Susanna M Thon; John D Tovar; Howard E Katz

doi:10.1002/adma.202201062

A New Polystyrene-Poly(vinylpyridinium) Ionic Copolymer Dopant for n-Type All-Polymer Thermoelectrics with High and Stable Conductivity Relative to the Seebeck Coefficient giving High Power Factor

Adv Mater. 2022 Jul;34(27):e2201062. doi: 10.1002/adma.202201062. Epub 2022 May 29.

Authors

Affiliations

¹ Department of Materials Science and Engineering and Department of Chemistry, Johns Hopkins University, 3400 North Charles Street, Baltimore, MD, 21218, USA.
² Department of Mechanical and Aerospace Engineering, University of Virginia, Charlottesville, VA, 22904, USA.
³ Department of Electrical and Computer Engineering, Johns Hopkins University, 3400 North Charles Street, Baltimore, MD, 21218, USA.
⁴ Department of Materials Science and Engineering, University of Virginia, Charlottesville, VA, 22904, USA.
⁵ Department of Physics, University of Virginia, Charlottesville, VA, 22904, USA.

PMID: 35441380
DOI: 10.1002/adma.202201062

Abstract

A novel n-type copolymer dopant polystyrene-poly(4-vinyl-N-hexylpyridinium fluoride) (PSpF) with fluoride anions is designed and synthesized by reversible addition-fragmentation chain transfer (RAFT) polymerization. This is thought to be the first polymeric fluoride dopant. Electrical conductivity of 4.2 S cm^-1 and high power factor of 67 µW m^-1 K^-2 are achieved for PSpF-doped polymer films, with a corresponding decrease in thermal conductivity as the PSpF concentration is increased, giving the highest ZT of 0.1. An especially high electrical conductivity of 58 S cm^-1 at 88 °C and outstanding thermal stability are recorded. Further, organic transistors of PSpF-doped thin films exhibit high electron mobility and Hall mobility of 0.86 and 1.70 cm² V^-1 s^-1 , respectively. The results suggest that polystyrene-poly(vinylpyridinium) salt copolymers with fluoride anions are promising for high-performance n-type all-polymer thermoelectrics. This work provides a new way to realize organic thermoelectrics with high conductivity relative to the Seebeck coefficient, high power factor, thermal stability, and broad processing window.

Keywords: Seebeck coefficient; all-polymer thermoelectrics; electrical conductivity; electron mobility; n-type polymer dopants.

Abstract

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