Radical Polymer-Based Organic Electrochemical Transistors

Kim, Ho Joong; Perera, Kuluni; Liang, Zihao; Bowen, Brennen; Mei, Jianguo; Boudouris, Bryan W.

doi:10.1021/acsmacrolett.1c00695

Title: Radical Polymer-Based Organic Electrochemical Transistors

Journal Article · 20 January 2022 · ACS Macro Letters

DOI: https://doi.org/10.1021/acsmacrolett.1c00695 · OSTI ID:1864771

Kim, Ho Joong ^[1]; Perera, Kuluni ^[2]; Liang, Zihao ^[2]; Bowen, Brennen ^[2];

^[2];

^[2]

Purdue Univ., West Lafayette, IN (United States); Purdue University
Purdue Univ., West Lafayette, IN (United States)

Organic electrochemical transistors (OECTs) are an emerging platform for bioelectronic applications. Significant effort has been placed in designing advanced polymers that simultaneously transport both charge and ions (i.e., macromolecules that are mixed conductors). Furthermore, the considerations for mixed organic conductors are often different from the established principles that are well-known in the solid-state organic electronics field; thus, the discovery of new OECT macromolecular systems is highly desired. Here, we demonstrate a new materials system by blending a radical polymer (i.e., a macromolecule with a nonconjugated backbone and with stable open-shell sites at its pendant group) with a frequently used conjugated polymer. Specifically, poly(4-glycidyloxy-2,2,6,6-tetramethylpiperidine-1-oxyl) (PTEO) was blended with poly(3-hexylthiophene) (P₃HT) to create thin films with distinct closed-shell and open-shell domains. Importantly, the sharp and unique oxidation–reduction (redox) potential associated with the radical moieties of the PTEO chain provided a distinct actuation feature to the blended films that modulated the ionic transport of the OECT devices. In turn, this led to controlled regulation of the doping of the P₃HT phase in the composite film. By decoupling the ionic and electronic transport into two distinct phases and by using an ion transport phase with well-controlled redox activity, never-before-seen performance for a P3HT-based OECT was observed. That is, at loadings as low as 5% PTEO (by weight) OECTs achieved figure-of-merit (i.e., μC*) values >150 F V^–1 cm^–1 s^–1, which place the performance on the same order as state-of-the-art conjugated polymers despite the relatively common conjugated macromolecular moiety implemented. As such, this effort presents a design platform by which to readily create a tailored OECT response through strategic macromolecular selection and polymer processing.

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Research Organization:: Purdue Univ., West Lafayette, IN (United States); Purdue University, West Lafayette, IN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0021967

OSTI ID:: 1864771

Journal Information:: ACS Macro Letters, Journal Name: ACS Macro Letters Journal Issue: 2 Vol. 11; ISSN 2161-1653

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Related Subjects

36 MATERIALS SCIENCE
Conjugated polymers
Organic Electrochemical Transistors
Organic polymers
Polymers
Radical Polymers
Redox reactions
Thin films

Title: Radical Polymer-Based Organic Electrochemical Transistors

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