Metal-like Charge Transport in PEDOT(OH) Films by Post-processing Side Chain Removal from a Soluble Precursor Polymer

James F Ponder Jr; Shawn A Gregory; Amalie Atassi; Abigail A Advincula; Joshua M Rinehart; Guillaume Freychet; Gregory M Su; Shannon K Yee; John R Reynolds

doi:10.1002/anie.202211600

Metal-like Charge Transport in PEDOT(OH) Films by Post-processing Side Chain Removal from a Soluble Precursor Polymer

Angew Chem Int Ed Engl. 2023 Jan 2;62(1):e202211600. doi: 10.1002/anie.202211600. Epub 2022 Nov 30.

Authors

James F Ponder Jr^{1

2

3}, Shawn A Gregory⁴, Amalie Atassi⁴, Abigail A Advincula⁴, Joshua M Rinehart⁴, Guillaume Freychet⁵, Gregory M Su⁶, Shannon K Yee¹, John R Reynolds^{4

7}

Affiliations

¹ George W. Woodruff School of Mechanical Engineering, Georgia Institute of Technology, Atlanta, GA 30332, USA.
² Materials and Manufacturing Directorate, Air Force Research Laboratory, Wright-Patterson AFB, Ohio, 45433, United States.
³ UES, Inc., Dayton, Ohio 45432, USA.
⁴ School of Materials Science and Engineering, Georgia Institute of Technology, Atlanta, GA 30332, USA.
⁵ NSLS-II, Brookhaven National Laboratory, Upton, New York, 11973, USA.
⁶ Advanced Light Source & Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California, 94720, USA.
⁷ School of Chemistry and Biochemistry, Center for Organic Photonics and Electronics, Georgia Tech Polymer Network, Georgia Institute of Technology, Atlanta, GA 30332, USA.

PMID: 36269867
DOI: 10.1002/anie.202211600

Abstract

Herein, a route to produce highly electrically conductive doped hydroxymethyl functionalized poly(3,4-ethylenedioxythiophene) (PEDOT) films, termed PEDOT(OH) with metal-like charge transport properties using a fully solution processable precursor polymer is reported. This is achieved via an ester-functionalized PEDOT derivative [PEDOT(EHE)] that is soluble in a range of solvents with excellent film-forming ability. PEDOT(EHE) demonstrates moderate electrical conductivities of 20-60 S cm^-1 and hopping-like (i.e., thermally activated) transport when doped with ferric tosylate (FeTos₃ ). Upon basic hydrolysis of PEDOT(EHE) films, the electrically insulative side chains are cleaved and washed from the polymer film, leaving a densified film of PEDOT(OH). These films, when optimally doped, reach electrical conductivities of ≈1200 S cm^-1 and demonstrate metal-like (i.e., thermally deactivated and band-like) transport properties and high stability at comparable doping levels.

Keywords: Charge Transport; Conductive Polymers; PEDOT; Post-Polymerization Functionalization.

Abstract

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