Unraveling the Detailed Interactions between the Surface Species and Nanoparticle Catalyst by a Temperature-Programed Desorption Spectrum at the Molecular Level via a Multi-Scale Simulation and Modeling Experiment

Abstract

Exploring the binding information of surface species with the active sites of a catalyst plays a key role in reaction mechanism study. The temperature-programed desorption (TPD) spectrum is a powerful approach to probe the interactions between surface species and a catalyst. However, it is hard to unravel their detailed interactions at the molecular level because TPD peaks are the statistical information derived from all surfaces of the nanoparticle catalyst. How to unravel these bonding details at the molecular level remains a substantial challenge in TPD spectrum analysis. To solve this difficult problem, a new strategy combining a density functional theory calculation, kinetic Monte Carlo simulation, and modeling experiment was proposed using CO TPD on χ-Fe5C2 nanoparticles as a demonstration. The good agreement between the simulated and experimental TPD spectra indicates the reasonability and feasibility of our strategy. It is anticipated to be a general method to unravel the interactions between surface species and catalysts at the molecular level.