In heterogeneous catalysis, the structures of nanocatalysts are crucial for their activities. Although these structures have long been considered as invariable during the reactions, recent in-situ experiments indicate they are actually variable under reaction conditions. However, whether the structural reconstructions take place in real reactions and how to correlate these changes with their activities remains elusive yet. Herein, we employed the density functional theory calculations and scaling methods to parameterize a simplified force field, and further applied it to kinetic Monte Carlo simulations. Using CO oxidation on Pt surfaces as the model systems, the atomistic simulations showed the notable surface reconstructions under the different reaction conditions, which significant influenced the turnover frequencies. This study exemplifies the plausibility of operando simulation of heterogeneous reactions at the atomic level.

Atomistic simulating the CO oxidation on Pt surfaces under operando conditions

ACS Fall 2021

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