Direct quantification of ion composition and mobility in organic mixed ionic-electronic conductors

Wu, Ruiheng; Ji, Xudong; Ma, Qing; Paulsen, Bryan D.; Tropp, Joshua; Rivnay, Jonathan

doi:10.1126/sciadv.adn8628

Title: Direct quantification of ion composition and mobility in organic mixed ionic-electronic conductors

Journal Article · 26 April 2024 · Science Advances

DOI: https://doi.org/10.1126/sciadv.adn8628 · OSTI ID:2470103

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Northwestern Univ., Evanston, IL (United States)
Northwestern Univ., Evanston, IL (United States). DND-CAT, Synchrotron Research Center

Ion transport in organic mixed ionic-electronic conductors (OMIECs) is crucial due to its direct impact on device response time and operating mechanisms but is often assessed indirectly or necessitates extra assumptions. Operando x-ray fluorescence (XRF) is a powerful, direct probe for elemental characterization of bulk OMIECs and was used to directly quantify ion composition and mobility in a model OMIEC, poly(3,4-ethylenedioxythiophene)-poly(styrene sulfonate) (PEDOT:PSS), during device operation. The first cycle revealed slow electrowetting and cation-proton exchange. Subsequent cycles showed rapid response with minor cation fluctuation (~5%). Comparison with optical-tracked electrochromic fronts revealed mesoscale structure–dependent proton transport. The calculated effective ion mobility demonstrated thickness-dependent behavior, emphasizing an interfacial ion transport pathway with a higher mobile ion density. The decoupling of interfacial effects on bulk ion mobility and the decoupling of cation and proton migration elucidate ion transport in conventional and emerging OMIEC-based devices and has broader implications for other ionic conductors writ large.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)

Sponsoring Organization:: USDOE Office of Science (SC); National Science Foundation (NSF); US Office of Naval Research (ONR)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 2470103

Journal Information:: Science Advances, Journal Name: Science Advances Journal Issue: 17 Vol. 10; ISSN 2375-2548

Publisher:: AAASCopyright Statement

Country of Publication:: United States

Language:: English

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