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Engineering oxygen vacancies and localized amorphous regions in CuO-ZnO separately boost catalytic reactivity and selectivity

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Nano Research 2023年第2期16卷 2126-2132页

作者： Yongjun Ji Xiaoli Chen Shaomian Liu Liwen Xing Xingyu Jiang Bin Zhang Huifang Li Wenxing Chen Ziyi Zhong Ligen Wang Guangwen Xu Fabing Su School of Light Industry Beijing Technology and Business UniversityBeijing 100048China Institute of Process Engineering Chinese Academy of SciencesBeijing 100190China College of Chemistry and Materials Engineering Beijing Technology and Business UniversityBeijing 100048China Institute of Industrial Chemistry and Energy Technology Shenyang University of Chemical TechnologyShenyang 110142China Analytical and Testing Center Chongqing UniversityChongqing 401331China Energy&Catalysis Center School of Materials Science and EngineeringBeijing Institute of TechnologyBeijing 100081China Department of Chemical Engineering Guangdong Technion-Israel Institute of Technology(GTIIT)Shantou 515063China Guangdong Provincial Key Laboratory of Materials and Technologies for Energy Conversion(MATEC) GTIITGuangdong 515063China Gripm Advanced Materials Co. Ltd.Beijing 101407China

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.

关键词： oxygen vacancy localized amorphous region CuO-ZnO catalyst reactivity selectivity

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