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

TY - JOUR

T1 - Engineering oxygen vacancies and localized amorphous regions in CuO-ZnO separately boost catalytic reactivity and selectivity

AU - Ji, Yongjun

AU - Chen, Xiaoli

AU - Liu, Shaomian

AU - Xing, Liwen

AU - Jiang, Xingyu

AU - Zhang, Bin

AU - Li, Huifang

AU - Chen, Wenxing

AU - Zhong, Ziyi

AU - Wang, Ligen

AU - Xu, Guangwen

AU - Su, Fabing

PY - 2022/10/7

Y1 - 2022/10/7

N2 - 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.

AB - 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.

U2 - 10.1007/s12274-022-4940-3

DO - 10.1007/s12274-022-4940-3

M3 - 文章

SN - 1998-0124

JO - Nano Research

JF - Nano Research

ER -