Molecular Simulation of Electrode-Solution Interfaces

TL;DR

This review discusses recent advances in classical molecular simulations of electrode-electrolyte interfaces, emphasizing the structure, thermodynamics, and dynamics at the atomic level for various electrolytes and metals.

Contribution

It provides a comprehensive overview of classical simulation techniques applied to electrode-electrolyte interfaces, highlighting recent progress and challenges in modeling these complex systems.

Findings

Enhanced understanding of ion and solvent behavior at interfaces

Insights into the role of electrostatic interactions in interface properties

Progress in modeling water-in-salt electrolytes

Abstract

Many key industrial processes, from electricity production, conversion and storage to electrocatalysis or electrochemistry in general, rely on physical mechanisms occurring at the interface between a metallic electrode and an electrolyte solution, summarized by the concept of electric double layer, with the accumulation/depletion of electrons on the metal side and of ions on the liquid side. While electrostatic interactions play an essential role on the structure, thermodynamics, dynamics and reactivity of electrode-electrolyte interfaces, these properties also crucially depend on the nature of the ions and solvent, as well as that of the metal itself. Such interfaces pose many challenges for modeling, because they are a place where Quantum Chemistry meets Statistical Physics. In the present review, we explore the recent advances on the description and understanding of electrode-electrolyte interfaces with classical molecular simulations, with a focus on planar interfaces and solvent-based liquids, from pure solvent to water-in-salt-electrolytes.