Design of CuCs-doped Ag-based Catalyst for Ethylene Epoxidation |
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Authors: | Qi-xing Wen Haoxiang Xu Yang Nan Yuan Xie Daojian Cheng |
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Affiliation: | a.State Key Laboratory of Organic-Inorganic Composites, Beijing Key Laboratory of Energy Environmental Catalysis, Beijing University of Chemical Technology, Beijing 100029, Chinab.Lanzhou Petrochemical Research Center, Petrochemical Research Institute, PetroChina, LanZhou 730060, China |
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Abstract: | 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. |
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Keywords: | Ethylene epoxidation Ag catalyst CuCs dopant Particle model Density functional theory calculation Microkinetic analysis |
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