Blended Conjugated Host and Unconjugated Dopant Polymers Towards N-type All-Polymer Conductors and High-ZT Thermoelectrics

Jinfeng Han; Yufeng Jiang; Emma Tiernan; Connor Ganley; Yunjia Song; Taein Lee; Arlene Chiu; Patty McGuiggan; Nicholas Adams; Paulette Clancy; Thomas P Russell; Patrick E Hopkins; Susanna M Thon; John D Tovar; Howard E Katz

doi:10.1002/anie.202219313

Blended Conjugated Host and Unconjugated Dopant Polymers Towards N-type All-Polymer Conductors and High-ZT Thermoelectrics

Angew Chem Int Ed Engl. 2023 Jun 5;62(23):e202219313. doi: 10.1002/anie.202219313. Epub 2023 Apr 26.

Authors

Jinfeng Han¹, Yufeng Jiang², Emma Tiernan³, Connor Ganley⁴, Yunjia Song¹, Taein Lee¹, Arlene Chiu⁵, Patty McGuiggan¹, Nicholas Adams¹, Paulette Clancy⁴, Thomas P Russell², Patrick E Hopkins^{3

6

7}, Susanna M Thon⁵, John D Tovar¹, Howard E Katz¹

Affiliations

¹ Department of Materials Science and Engineering and Department of Chemistry, Johns Hopkins University, 3400 North Charles Street, Baltimore, MD 21218, USA.
² Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA.
³ Department of Mechanical and Aerospace Engineering, University of Virginia, Charlottesville, VA 22904, USA.
⁴ Department of Chemical and Biomolecular Engineering, Johns Hopkins University, 3400 North Charles Street, Baltimore, MD 21218, USA.
⁵ Department of Electrical and Computer Engineering, Johns Hopkins University, 3400 North Charles Street, Baltimore, MD 21218, USA.
⁶ Department of Materials Science and Engineering, University of Virginia, Charlottesville, VA 22904, USA.
⁷ Department of Physics, University of Virginia, Charlottesville, VA 22904, USA.

PMID: 37021740
DOI: 10.1002/anie.202219313

Abstract

N-Type thermoelectrics typically consist of small molecule dopant+polymer host. Only a few polymer dopant+polymer host systems have been reported, and these have lower thermoelectric parameters. N-type polymers with high crystallinity and order are generally used for high-conductivity ( $σ$ ) organic conductors. Few n-type polymers with only short-range lamellar stacking for high-conductivity materials have been reported. Here, we describe an n-type short-range lamellar-stacked all-polymer thermoelectric system with highest $σ$ of 78 S^-1 , power factor (PF) of 163 μW m^-1 K^-2 , and maximum Figure of merit (ZT) of 0.53 at room temperature with a dopant/host ratio of 75 wt%. The minor effect of polymer dopant on the molecular arrangement of conjugated polymer PDPIN at high ratios, high doping capability, high Seebeck coefficient (S) absolute values relative to $σ$ , and atypical decreased thermal conductivity ( $κ$ ) with increased doping ratio contribute to the promising performance.

Keywords: All-Polymer Thermoelectrics; Electrical Conductivity; Power Factor; Semiconducting Polymer; ZT.

Abstract

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