文献类型：期刊文献

英文题名：Insights into Coverage-Affected Selective Catalytic Oxidation of Ethylene on Ag(111) from Comprehensive Microkinetical Analyses

作者：Wang, Zhuozheng[1]; Xie, Wenbo[1]; Xu, Yarong[1,2]; Jia, Menglei[1,3]; Xu, Jiayan[1]; Hu, Peijun[1,3]

机构：[1] School of Chemistry and Chemical Engineering, The Queen's University of Belfast, Belfast, BT9 5AG, United Kingdom; [2] Research Institute of Urumqi Petrochemical Company, Petrochina Company Limited, Urumqi, 830019, China; [3] Key Laboratory for Advanced Materials, Centre for Computational Chemistry, Research Institute of Industrial Catalysis, East China University of Science and Technology, 130 Meilong Road, Shanghai, 200237, China

年份：2022

外文期刊名：SSRN

收录：EI(收录号：20220284310)

语种：英文

外文关键词：Catalytic oxidation - Ethylene

摘要：Ethylene epoxidation is one of the most important industrial reactions. Although there have been many studies on the reaction, details of the reaction kinetics remain elusive. Herein, an extensive microkinetic modelling based on DFT calculations was carried out to study the ethylene epoxidation on Ag(111). Coverage-dependent and coverage-independent microkinetic modellings were performed with rigorous energetics including coveragedependent transition states. Detailed comparisons between these two modellings show that the coverage-independent modelling is inadequate even though the coverage is very low at the steady state. Compared with the experimental turnover frequency (log(TOF) = 2.52), the result of the coverage-dependent (2.53) agrees well with the experimental value but considerably deviates from the coverage-independent result (-1.87). A comprehensive kinetic analysis under industrial conditions was conducted, which shows that increasing the temperature and pressure can effectively enhance the activity and EO selectivity. The work provides some significant insights into the reaction at the atomic level. ? 2022, The Authors. All rights reserved.