(55f) Effects of Electrified Interface on Ammonia Dissociation Reaction.

Ammonia oxidation is an important reaction in both energy-converting devices and nitrogen cycle management, with applications ranging from fuel cells to wastewater treatment. The author's earlier work investigated the fundamental mechanisms of ammonia electrooxidation on transition metal surfaces including platinum and iridium, with special focus on the adsorption properties of pertinent intermediates, reaction routes, and the impact of catalytic surface properties on activity and selectivity. The study provided mechanistic data on rate-determining steps and illustrated that the mechanisms of ammonia oxidation on Pt and Ir are different. In another study, the author explored the effect of electric fields on solvation energy during methanol oxidation.
Building on this foundation, the current study probes the effects of external electric fields and solvent environments on the ammonia oxidation reaction. Electric fields are used to control reaction energetics and intermediate stability by modifying the electronic structure of catalysts, adsorbates, and solvents. The electric field at the interface between solvent and adsorbates, where local field intensities can reach 0.5–1 V/Å, is of particular interest as it affects the course of the reaction. Solvent effects are central and may significantly influence adsorption behavior, reaction barriers, and charge transfer kinetics within the solid–liquid interface. By integrating multiscale computational electrochemistry approaches—density functional theory (DFT) and classical molecular dynamics (cMD)—this research aims to provide a more realistic and predictive understanding of ammonia oxidation under electrochemical conditions. These observations, compared to the author's previous publications, will be analyzed and presented.