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 (30)

• Double layer in ionic liquids: Overscreening vs. crowding
• Diffuse-Charge Dynamics in Electrochemical Systems
• Solvation at Aqueous Metal Electrodes
• ESPResSo 4.0 -- An Extensible Software Package for Simulating Soft Matter Systems
• The electric double layer has a life of its own
• Electric displacement as the fundamental variable in electronic-structure calculations
• Simulations of room temperature ionic liquids: From polarizable to coarse-grained force fields
• Charge fluctuations in nano-scale capacitors
• Water at an electrochemical interface - a simulation study
• Nanoscale capillary freezing of ionic liquids confined between metallic interfaces and the role of electronic screening
• Structural Transitions at Ionic Liquids Interfaces
• Charge fluctuations from molecular simulations in the constant-potential ensemble
• Simulating electrochemical systems by combining the finite field method with a constant potential electrode
• Multi-scale modelling of supercapacitors: From molecular simulations to a transmission line model
• A semiclassical Thomas-Fermi model to tune the metallicity of electrodes in molecular simulations
• Voltage equilibration for reactive atomistic simulations of electrochemical processes
• Efficient and accurate simulation of dynamic dielectric objects
• Finite Field Methods for the Supercell Modelling of Charged Insulator-Electrolyte Interfaces
• How strongly do hydrogen and water molecules stick to carbon nanomaterials?
• Study of a water-graphene capacitor with molecular density functional theory
• Characterizing heterogeneous dynamics at hydrated electrode surfaces
• Molecular modeling of aqueous electrolytes at interfaces: effects of long-range dispersion forces and of ionic charge rescaling
• Microscopic dynamics of charge separation at the aqueous electrochemical interface
• Simulations of ionic liquids confined by metal electrodes using periodic Green functions
• Nanoscale heterogeneity at the aqueous electrolyte-electrode interface
• A Molecular Density Functional Theory Approach to Electron Transfer Reactions
• Charge compensation at the interface between the polar NaCl(111) surface and a NaCl aqueous solution
• Mass-zero constrained molecular dynamics for electrode charges in simulations of electrochemical systems
• Lattice Boltzmann Electrokinetics simulation of nanocapacitors
• Fluctuations of local electric field and dipole moments in water between metal walls

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• On the Gibbs-Thomson equation for the crystallization of confined fluids
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• Multi-scale simulation of the adsorption of lithium ion on graphite surface: from Quantum Monte Carlo to Molecular Density Functional Theory
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• Ionic liquid-electrode interface: classification of ions, saturation of layers, and structure-determined potentials
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• Deriving effective electrode-ion interactions from free-energy profiles at electrochemical interfaces