Numerical simulations of electrocatalytic processes

Abstract

Recent developments in the computer simulation of electrocatalytic processes are discussed. The type of computer simulation chosen for a particular application depends on the time scale of the process and the level of molecular detail desired. Quantum‐chemical electronic structure calculations utilizing the density functional formalism give information about the details of the chemical bonding of molecules at surfaces. Application of the bonding of carbon monoxide to transition metal surfaces and alloys is described, including the role of the electric field. The link to macroscopically measurable kinetics, like voltammetry, can be made by resorting to Dynamic Monte Carlo methods. In this method, reaction events are mapped on to a lattice‐gas model of the catalyst surface and the statistical mechanics is solved exactly by Monte Carlo simulation algorithms. The reactant parameters can either be obtained from first‐principles quantum chemical calculations, or be adjusted so as to mimic as closely as possible the experimental results. An example of this method as applied to the oxidation of CO on platinum–ruthenium alloys is discussed.

Electrocatalysis for Polymer Electrolyte Fuel Cells: Recent Achievements and Future Challenges

“…Many of these catalyst developments, including the in-depth understanding of reaction mechanisms, was possible through the important breakthrough developments in computational studies, i.e., the application of molecular dynamics, quantum mechanical, and density functional theory (DFT) calculations. − These studies not only helped for a better understanding but also proved predictive capabilities for novel improved catalysts. In addition to the advanced theoretical tools that have helped to improve electrocatalysts, the progress in the application of new experimental techniques is closely related to electrocatalyst research.…”