Molecular Simulation of Electrode-Solution Interfaces

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.

References in corpus (7)

• The electric double layer has a life of its own
• Simulations of room temperature ionic liquids: From polarizable to coarse-grained force fields
• Finite Field Methods for the Supercell Modelling of Charged Insulator-Electrolyte Interfaces
• Molecular modeling of aqueous electrolytes at interfaces: effects of long-range dispersion forces and of ionic charge rescaling
• Simulations of ionic liquids confined by metal electrodes using periodic Green functions
• Nanoscale heterogeneity at the aqueous electrolyte-electrode interface
• Mass-zero constrained molecular dynamics for electrode charges in simulations of electrochemical systems

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