Exploration of Dynamic Structure–Activity Relationship of a Platinum Nanoparticle in the CO Oxidation Reaction

Conventional modeling of heterogeneous catalysis is usually based on well-defined structures, which are independent of reaction conditions. However, recent in situ experiments indicated that the morphologies of nanoparticles (NPs) changed greatly under reactive environments. How to correlate the changed structures of the NPs with their catalytic activities in reactions is a challenge in experiment and theory. Herein, we used the multiscale structure reconstruction (MSR) model to generate equilibrium Pt NPs under different CO reaction conditions and then performed surface kinetics modeling to explore the corresponding catalytic activities. Our results show that the structure and catalytic activity of the NP may both change in changing gaseous environments, which are completely different from the results using the stationary model. We also predict the optimized CO oxidation over the Pt catalyst with the consideration of the dependence of reaction condition on the nanoparticle morphology. This work enlightens the importance of modeling the reaction-condition dependent morphology on the understanding of realistic catalytic activity of NPs.