Probing consequences of anion-dictated electrochemistry on the electrode/monolayer/electrolyte interfacial properties

Raymond A. Wong, Yasuyuki Yokota (), Mitsuru Wakisaka, Junji Inukai and Yousoo Kim ()
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Raymond A. Wong: RIKEN
Yasuyuki Yokota: RIKEN
Mitsuru Wakisaka: Toyama Prefectural University
Junji Inukai: University of Yamanashi
Yousoo Kim: RIKEN

Nature Communications, 2020, vol. 11, issue 1, 1-9

Abstract: Abstract Altering electrochemical interfaces by using electrolyte effects or so-called “electrolyte engineering” provides a versatile means to modulate the electrochemical response. However, the long-standing challenge is going “beyond cyclic voltammetry” where electrolyte effects are interrogated from the standpoint of the interfacial properties of the electrode/electrolyte interface. Here, we employ ferrocene-terminated self-assembled monolayers as a molecular probe and investigate how the anion-dictated electrochemical responses are translated in terms of the electronic and structural properties of the electrode/monolayer/electrolyte interface. We utilise a photoelectron-based spectroelectrochemical approach that is capable of capturing “snapshots” into (1) anion dependencies of the ferrocene/ferrocenium (Fc/Fc+) redox process including ion-pairing with counter anions (Fc+–anion) caused by differences in Fc+–anion interactions and steric constraints, and (2) interfacial energetics concerning the electrostatic potential across the electrode/monolayer/electrolyte interface. Our work can be extended to provide electrolyte-related structure-property relationships in redox-active polymers and functionalised electrodes for pseudocapacitive energy storage.

Date: 2020
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DOI: 10.1038/s41467-020-18030-6

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