Pd-based catalysts are extensively employed to catalyze CO oxidative coupling to generate DMO,while the expensive price and high usage of Pd hinder its massive application in industrial production.Designing Pd-based c...Pd-based catalysts are extensively employed to catalyze CO oxidative coupling to generate DMO,while the expensive price and high usage of Pd hinder its massive application in industrial production.Designing Pd-based catalysts with high efficiency and low Pd usage as well as expounding the catalytic mechanisms are significant for the reaction.In this study,we theoretically predict that Pd stripe doping Co(111)surface exhibits excellent performance than pure Pd(111),Pd monolayer supporting on Co(111)and Pd single atom doping Co(111)surface,and clearly expound the catalytic mechanisms through the density functional theory(DFT)calculation and micro-reaction kinetic model analysis.It is obtained that the favorable reaction pathway is COOCH_(3)-COOCH_(3)coupling pathway over these four catalysts,while the rate-controlling step is COOCH_(3)+CO+OCH_(3)→2COOCH_(3)on Pd stripe doping Co(111)surface,which is different from the case(2COOCH_(3)→DMO)on pure Pd(111),Pd monolayer supporting on Co(111)and Pd single atom doping Co(111)surface.This study can contribute a certain reference value for developing Pd-based catalysts with high efficiency and low Pd usage for CO oxidative coupling to DMO.展开更多
基金financially supported by the National Key Research and Development Program of China(2021YFA1502804)the Regional Innovation and Development Joint Fund of the National Natural Science Foundation of China(U22A20430)+3 种基金the Shanxi-Zheda Institute of Advanced Materials and Chemical Engineering(2022SX-FR001)the Natural Science Foundation of Shanxi Province(202203021212201)the Scientific and Technological Innovation Programs of Higher Education Institutions in Shanxithe Foundation of Taiyuan University of Technology(2022QN138)
文摘Pd-based catalysts are extensively employed to catalyze CO oxidative coupling to generate DMO,while the expensive price and high usage of Pd hinder its massive application in industrial production.Designing Pd-based catalysts with high efficiency and low Pd usage as well as expounding the catalytic mechanisms are significant for the reaction.In this study,we theoretically predict that Pd stripe doping Co(111)surface exhibits excellent performance than pure Pd(111),Pd monolayer supporting on Co(111)and Pd single atom doping Co(111)surface,and clearly expound the catalytic mechanisms through the density functional theory(DFT)calculation and micro-reaction kinetic model analysis.It is obtained that the favorable reaction pathway is COOCH_(3)-COOCH_(3)coupling pathway over these four catalysts,while the rate-controlling step is COOCH_(3)+CO+OCH_(3)→2COOCH_(3)on Pd stripe doping Co(111)surface,which is different from the case(2COOCH_(3)→DMO)on pure Pd(111),Pd monolayer supporting on Co(111)and Pd single atom doping Co(111)surface.This study can contribute a certain reference value for developing Pd-based catalysts with high efficiency and low Pd usage for CO oxidative coupling to DMO.
