Design of CuCs-doped Ag-based Catalyst for Ethylene Epoxidation

Our recent theoretical studies have screened out CuCs-doped Ag-based promising catalysts for ethylene epoxidation ACS Catal. 11 , 3371 (2021)]. The theoretical results were based on surface modeling, while in the actual reaction process Ag catalysts are particle shaped. In this work, we combine density functional theory (DFT), Wulff construction theory, and micro kinetic analysis to study the catalytic performance of Ag catalysts at the particle model. It demonstrates that the CuCs-doped Ag catalysts are superior to pure Ag catalysts in terms of selectivity and activity, which is further proved by experimental validation. The characterization analysis finds that both Cu and Cs dopant promote particle growth as well as particle dispersion, resulting in a grain boundary-rich Ag particle. Besides, CuCs also facilitate electrophilic atomic oxygen formation on catalyst surface, which is benefitial for ethylene oxide formation and desorption. Our work provides a case study for catalyst design by combining theory and experiment.