Nanoscale heterogeneity at the aqueous electrolyte-electrode interface

TL;DR

This study uses molecular dynamics simulations to uncover nanoscale heterogeneity in the aqueous electrolyte-electrode interface, revealing how disordered water layers influence ion behavior and electrode properties over time.

Contribution

It introduces a detailed molecular-level analysis of hydrated electrode interfaces, highlighting the impact of disordered water layers on electrolyte structure and dynamics.

Findings

Density and mobility heterogeneity of water and ions at the interface

Impact of water layer disorder on electrochemical behavior

Correlation with experimental surface science data

Abstract

Using molecular dynamics simulations, we reveal emergent properties of hydrated electrode interfaces that while molecular in origin are integral to the behavior of the system across long times scales and large length scales. Specifically, we describe the impact of a disordered and slowly evolving adsorbed layer of water on the molecular structure and dynamics of the electrolyte solution adjacent to it. Generically, we find that densities and mobilities of both water and dissolved ions are spatially heterogeneous in the plane parallel to the electrode over nanosecond timescales. These and other recent results are analyzed in the context of available experimental literature from surface science and electrochemistry. We speculate on the implications of this emerging microscopic picture on the catalytic proficiency of hydrated electrodes, offering an new direction for study in heterogeneous catalysis at the nanoscale.