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Hole-limited electrochemical doping in conjugated polymers.

Accepted version
Peer-reviewed

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Type

Article

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Authors

Laulainen, Joonatan EM  ORCID logo  https://orcid.org/0000-0003-0596-1663
Pandya, Raj 
Schnedermann, Christoph  ORCID logo  https://orcid.org/0000-0002-2841-8586

Abstract

Simultaneous transport and coupling of ionic and electronic charges is fundamental to electrochemical devices used in energy storage and conversion, neuromorphic computing and bioelectronics. While the mixed conductors enabling these technologies are widely used, the dynamic relationship between ionic and electronic transport is generally poorly understood, hindering the rational design of new materials. In semiconducting electrodes, electrochemical doping is assumed to be limited by motion of ions due to their large mass compared to electrons and/or holes. Here, we show that this basic assumption does not hold for conjugated polymer electrodes. Using operando optical microscopy, we reveal that electrochemical doping speeds in a state-of-the-art polythiophene can be limited by poor hole transport at low doping levels, leading to substantially slower switching speeds than expected. We show that the timescale of hole-limited doping can be controlled by the degree of microstructural heterogeneity, enabling the design of conjugated polymers with improved electrochemical performance.

Description

Keywords

3403 Macromolecular and Materials Chemistry, 34 Chemical Sciences, 3406 Physical Chemistry, 40 Engineering, 4016 Materials Engineering, 7 Affordable and Clean Energy

Journal Title

Nat Mater

Conference Name

Journal ISSN

1476-1122
1476-4660

Volume Title

Publisher

Springer Science and Business Media LLC
Sponsorship
European Commission Horizon 2020 (H2020) Marie Sk?odowska-Curie actions (101022365)
EPSRC (EP/W017091/1)
Engineering and Physical Sciences Research Council (EP/R008779/1)
European Research Council (758826)
European Commission Horizon 2020 (H2020) Research Infrastructures (RI) (823717)
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