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Side-Chain Free Semiconducting Polymer for High-Performance n‑Type Organic Electrochemical Transistors

Abstract:
The development of organic electrochemical transistors (OECTs) critically depends on the design and characterization of mixed-conducting, high-performance conjugated polymers (CPs) as channel materials, particularly for n-type OECTs. In this study, we present a novel strategy to enhance the OECT performance of a semiconducting polymer film via a postdeposition ester pyrolysis of thermally cleavable side chains, thus facilitating ion incorporation and transport within the bulk. Our approach relies on the synthesis of a high glass-transition, rigid-rod polymer, able to withstand the pyrolysis temperature without deformation and maintain the voids formed from the pyrolysis reaction which removes the thermally cleavable ester side chains. After side-chain cleavage, the resulting film exhibits increased porosity, hydrophilicity, and crystallinity. By creating bulk porosity in thin films via this approach, ion diffusion is enhanced, resulting in a superior μC* figure of merit up to 158.85 F cm–1 V–1 s–1, and a corresponding increase in normalized transconductance (31.67 S cm–1). In addition, the device switching speed and long-term stability are also observed to increase, further demonstrating the benefit of nanoscale porosity for mixed conductivity semiconductors.
Publication status:
Published
Peer review status:
Peer reviewed

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Publisher copy:
10.1021/jacs.5c19399

Authors

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Institution:
University of Oxford
Division:
MPLS
Department:
Chemistry
Sub department:
Chemistry Research Laboratory
Role:
Author
More by this author
Institution:
University of Oxford
Division:
MPLS
Department:
Chemistry
Sub department:
Chemistry Research Laboratory
Role:
Author
ORCID:
0000-0003-3403-667X
More by this author
Institution:
University of Oxford
Division:
MPLS
Department:
Chemistry
Sub department:
Chemistry Research Laboratory
Role:
Author


More from this funder
Funder identifier:
10.13039/100010661
Grant:
952911
More from this funder
Funder identifier:
10.13039/501100000266
Grant:
EP/T026219/1
More from this funder
Funder identifier:
https://ror.org/05etxs293
Grant:
SI39430
More from this funder
Funder identifier:
https://ror.org/01ar8dr59
Grant:
2404409


Publisher:
American Chemical Society
Journal:
Journal of the American Chemical Society More from this journal
Volume:
148
Issue:
9
Pages:
9494-9503
Publication date:
2026-02-26
Acceptance date:
2026-02-19
DOI:
EISSN:
1520-5126
ISSN:
0002-7863


Language:
English
Keywords:
Pubs id:
2382063
Local pid:
pubs:2382063
Source identifiers:
3846013
Deposit date:
2026-03-12
ARK identifier:
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