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    Monitoring transient changes in the structure of water at a polarised liquid-liquid interface using electrocapillary curves

    Year: 2019

    Journal: Electrochem. Commun., Volume 109, DEC

    Authors: Suarez-Herrera, Marco F.; Cazade, Pierre-Andre; Thompson, Damien; Scanlon, Micheal D.

    Organizations: Science Foundation Ireland (SFI)Science Foundation Ireland [13/SIRG/2137]; European Research CouncilEuropean Research Council (ERC)European Commission [716792]; SFIScience Foundation Ireland [15/CDA/3491, 12/RC/2275]

    Keywords: Interface between two immiscible electrolyte solutions; Liquid-liquid interface; Electrochemical double layer; Electrocapillary curves; Differential capacitance; Interfacial energy

    The interface between two immiscible electrolyte solutions (ITIES) is a close approximation of an ideally polarisable interface, being non-equilibrated upon formation. Despite this, the formalism of equilibrium thermodynamics, e.g., electrocapillary equations, are universally applied to interpret electrochemical processes at the ITIES. This communication shows that interfacial energy measurements in real time during step potential experiments are a useful tool to detect transient changes in the structure of the electrolyte solutions at the ITIES, in particular in the presence of chaotropes or kosmotropes in the aqueous electrolyte. Molecular dynamics computer simulations substantiate our findings, quantifying the perturbation of the atomic-scale structure, dynamics and energetics of the interface in the presence of a kosmotrope.
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