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

Author:

Wu Ruiheng1ORCID,Ji Xudong2ORCID,Ma Qing3ORCID,Paulsen Bryan D.2ORCID,Tropp Joshua2ORCID,Rivnay Jonathan24ORCID

Affiliation:

1. Department of Chemistry, Northwestern University, Evanston, IL 60208, USA.

2. Department of Biomedical Engineering, Northwestern University, Evanston, IL 60208, USA.

3. DND-CAT, Synchrotron Research Center, Northwestern University, Evanston, IL 60208, USA.

4. Department of Material Science and Engineering, Northwestern University, Evanston, IL 60611, USA.

Abstract

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.

Publisher

American Association for the Advancement of Science (AAAS)

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