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Nano Research 2023, 16(2): 2126-2132 https://doi.org/10.1007/s12274-022-4940-3
Research Article | Issue | Published: 07 October 2022

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

Show Author's Information Yongjun Ji1,§( ),  Xiaoli Chen1,§,  Shaomian Liu2,§,  Liwen Xing3( ),  Xingyu Jiang4,  Bin Zhang5,  Huifang Li2,  Wenxing Chen6,  Ziyi Zhong7,8,  Ligen Wang9( ),  Guangwen Xu4,  Fabing Su2,4( )
School of Light Industry, Beijing Technology and Business University, Beijing 100048, China
Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China
College of Chemistry and Materials Engineering, Beijing Technology and Business University, Beijing 100048, China
Institute of Industrial Chemistry and Energy Technology, Shenyang University of Chemical Technology, Shenyang 110142, China
Analytical and Testing Center, Chongqing University, Chongqing 401331, China
Energy & Catalysis Center, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing 100081, China
Department of Chemical Engineering, Guangdong Technion-Israel Institute of Technology (GTIIT), Shantou 515063, China
Guangdong Provincial Key Laboratory of Materials and Technologies for Energy Conversion (MATEC), GTIIT, Guangdong 515063, China
Gripm Advanced Materials Co., Ltd., Beijing 101407, China

§ Yongjun Ji, Xiaoli Chen, and Shaomian Liu contributed equally to this work.

Keywords:
oxygen vacancy, selectivity, reactivity, localized amorphous region, CuO-ZnO catalyst
Topics:
Catalyst activityCatalyst selectivity
Cite this article:
Ji Y, Chen X, Liu S, et al. Engineering oxygen vacancies and localized amorphous regions in CuO-ZnO separately boost catalytic reactivity and selectivity. Nano Research, 2023, 16(2): 2126-2132. https://doi.org/10.1007/s12274-022-4940-3
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Abstract Full text Electronic supplementary material About this article

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.


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Electronic supplementary material
About this article

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

Show Author's information Yongjun Ji1,§( ), Xiaoli Chen1,§, Shaomian Liu2,§, Liwen Xing3( ), Xingyu Jiang4, Bin Zhang5, Huifang Li2, Wenxing Chen6, Ziyi Zhong7,8, Ligen Wang9( ), Guangwen Xu4, Fabing Su2,4( )
School of Light Industry, Beijing Technology and Business University, Beijing 100048, China
Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China
College of Chemistry and Materials Engineering, Beijing Technology and Business University, Beijing 100048, China
Institute of Industrial Chemistry and Energy Technology, Shenyang University of Chemical Technology, Shenyang 110142, China
Analytical and Testing Center, Chongqing University, Chongqing 401331, China
Energy & Catalysis Center, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing 100081, China
Department of Chemical Engineering, Guangdong Technion-Israel Institute of Technology (GTIIT), Shantou 515063, China
Guangdong Provincial Key Laboratory of Materials and Technologies for Energy Conversion (MATEC), GTIIT, Guangdong 515063, China
Gripm Advanced Materials Co., Ltd., Beijing 101407, China

§ Yongjun Ji, Xiaoli Chen, and Shaomian Liu contributed equally to this work.

Abstract

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.

Keywords: oxygen vacancy, selectivity, reactivity, localized amorphous region, CuO-ZnO catalyst

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Publication history
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Acknowledgements

Publication history

Received: 28 July 2022
Revised: 19 August 2022
Accepted: 19 August 2022
Published: 07 October 2022
Issue date: February 2023

Copyright

© Tsinghua University Press 2022

Acknowledgements

Acknowledgements

We gratefully acknowledge the financial 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), and 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.

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