Abstract

Electronic structures play a key role in the activities of supported metal catalysts. In this work, by using the ab initio molecular dynamics simulations and density functional theory calculations, we report the fluxional electronic structures of supported Pd clusters driven by the dramatic fluctuation of electronic configurations at the CeO2(111) substrate during the dynamics process. The binding energies, charges, magnetic moments, and density of states of supported Pd clusters change substantially, even if their structures vary slightly. It indicates that the dynamic evolution of electronic structures cannot be ignored to precisely evaluate the activities of supported nanoclusters in catalytic reactions.