Theoretical advances of simulating the dynamic structures of metal nanocatalysts under reaction conditions

Metal catalysts are among the most widely used in heterogeneous catalysis. For decades, it was tacitly assumed that reactive molecules undergo adsorption, reaction, and desorption on a static catalyst structure. However, recent in-situ studies have revealed that the structures and surface compositions of metal catalysts continuously evolve under reactive conditions. Consequently, the conventional approach of correlating catalytic activity with fixed catalyst structures fails to capture the true structure-activity relationship under operational conditions. Understanding the dynamic evolution of metal catalyst structures during reactions is therefore essential for establishing accurate structure-activity relationships. In this paper, we first briefly review recent advances in theoretical methods in this field, then focus on the multiscale simulation techniques developed by our group and their applications in predicting morphological changes and real-time restructuring processes of metal catalysts. Finally, we provide a perspective on the future of in-situ simulations in heterogeneous catalysis.