Design and screening of bimetallic catalysts for nitric oxide reduction by CO: a study of kinetic Monte Carlo simulation based on first-principles calculations

Abstract

Nitric oxide (NO) emissions pose a significant environmental challenge, and the development of effective catalysts for NO reduction is crucial. This study investigates the potential of striped bimetallic catalysts for NO reduction by CO using kinetic Monte Carlo (KMC) simulations based on first-principles calculations. The simulations reveal that the activity on the striped Ni–Pt–Pt (111) surface is 1–2 orders of magnitude higher than that on the terraced Ni–Pt–Pt (111) surface at the same temperatures, demonstrating the importance of defect engineering. Sensitivity analysis identifies CO oxidation as the rate-determining step, although the 2N* association barrier is higher than CO oxidation, highlighting the need to consider reaction conditions in kinetic simulations. Volcano plots based on the formation energies of NO* and CO* successfully predict the striped Ni–Pd–Pd (111) and Ni–Rh–Rh (111) surfaces as optimal catalysts, which were further validated through DFT calculations and ab initio molecular dynamics simulations. This study offers valuable insights for designing high-performance bimetallic catalysts for NO reduction and underscores the importance of considering specific reaction conditions in kinetic simulations.