Generating different types of defects in heterogeneous catalysts for synergetic promotion of the reactivity and selectivity in catalytic reactions is highly challenging due to the lack of effective theoretical guidanc...Generating different types of defects in heterogeneous catalysts for synergetic promotion of the reactivity and selectivity in catalytic reactions is highly challenging due to the lack of effective theoretical guidance.Herein,we demonstrate a facile strategy to introduce two types of defects into the CuO-ZnO model catalyst,namely oxygen vacancies(OVs)induced by H2 partial reduction and localized amorphous regions(LARs)generated via the ball milling process.Using industrially important Rochow–Müller reaction as a representative,we found OVs predominantly improved the target product selectivity of dimethyldichlorosilane,while LARs significantly increased the conversion of reactant Si.The CuO-ZnO catalyst with optimized OVs and LARs contents achieved the best catalytic property.Theoretical calculation further revealed that LARs promote the generation of the Cu3Si active phase,and OVs impact the electronic structure of the Cu3Si active phase.This work provides a new understanding of the roles of different catalyst defects and a feasible way of engineering the catalyst structure for better catalytic performances.展开更多
基金support from the National Natural Science Foundation of China(Nos.21878301 and 21978299)the Open Research Fund of State Key Laboratory of Multiphase Complex Systems(No.MPCS-2021-D-08)+4 种基金GRINM Group.Y.J.J.thanks the financial support from the Research Foundation for Advanced Talents of Beijing Technology and Business University(No.19008020159)X.L.C.thanks the financial support from the project for improving the research ability of postgraduate from Beijing Technology and Business University(No.19008022056)L.W.X.thanks the financial support from the Research Foundation for Youth Scholars of Beijing Technology and Business University(No.QNJJ2022-22)Z.Y.Z.thanks the financial support of Guangdong Provincial Key Laboratory of Materials and Technologies for Energy Conversion(MATEC)Guangdong Technion-Israel Institute of Technology and Guangdong Key Discipline Fund(2022)for this collaboration。
文摘Generating different types of defects in heterogeneous catalysts for synergetic promotion of the reactivity and selectivity in catalytic reactions is highly challenging due to the lack of effective theoretical guidance.Herein,we demonstrate a facile strategy to introduce two types of defects into the CuO-ZnO model catalyst,namely oxygen vacancies(OVs)induced by H2 partial reduction and localized amorphous regions(LARs)generated via the ball milling process.Using industrially important Rochow–Müller reaction as a representative,we found OVs predominantly improved the target product selectivity of dimethyldichlorosilane,while LARs significantly increased the conversion of reactant Si.The CuO-ZnO catalyst with optimized OVs and LARs contents achieved the best catalytic property.Theoretical calculation further revealed that LARs promote the generation of the Cu3Si active phase,and OVs impact the electronic structure of the Cu3Si active phase.This work provides a new understanding of the roles of different catalyst defects and a feasible way of engineering the catalyst structure for better catalytic performances.
