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 den-sity 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 activ-ity,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,result-ing 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.