Long-Range Oxygen Spillover at the Cu/CeO 2 Interface

High Resolution Image Download MS PowerPoint Slide Reverse oxygen spillover (ROS) from ceria (CeO 2 ) to supported metal species, driven by strong metal–support interactions, profoundly impacts not only their catalytic efficacy but also the structural stability, dispersion, and electronic characteristics of the metal active sites. Herein, we for the first time observed a long-range dynamic ROS phenomenon at the interface of Cu/CeO 2 catalysts by means of first-principles calculations and ab initio and deep-potential molecular dynamics (DPMD) simulations. The ROS process is initiated by interfacial lattice oxygen transfer to Cu species, followed by the sequential migration of adjacent O atoms through oxygen vacancies, resulting in the progressive oxidation of supported Cu species. In addition, DPMD simulations reveal the persistence of the long-range ROS process over larger time and spatial scales, with larger Cu nanoparticles exhibiting faster and more extensive ROS. These findings provide mechanistic insights into the importance of long-range ROS behaviors in the preparation of oxide-supported metal catalysts.