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single-atom Sn-Zn pairs in CuO catalyst promote dimethyldichlorosilane synthesis

National Science Review 2020年第3期7卷 600-608页

作者： Qi Shi Yongjun Ji Wenxin Chen Yongxia Zhu Jing Li Hezhi Liu Zhi Li Shubo Tian Ligen Wang Ziyi Zhong Limin Wang Jianmin Ma Yadong Li Fabing Su Gripm Advanced Materials Co. Ltd State Key Laboratory of Multiphase Complex Systems Institute of Process EngineeringChinese Academy of Sciences Zhongke Langfang Institute of Process Engineering Beijing Key Laboratory of Construction Tailorable Advanced Functional Materials and Green Applications School of Materials Science and Engineering Beijing Institute of Technology Department of Chemistry Tsinghua University College of Engineering Guangdong Technion–Israel Institute of Technology (GTIIT) Technion–Israel Institute of Technology (IIT) School of Physics and Electronics Hunan University Institute of Industrial Chemistry and Energy Technology Shenyang University of Chemical Technology

single-atom catalysts are of great interest because they can maximize the atom-utilization efficiency and generate unique catalytic properties; however, much attention has been paid to single-site active components, rarely to catalyst promoters. promoters can significantly affect the activity and selectivity of a catalyst, even at their low concentrations in catalysts. In this work, we designed and synthesized Cu O catalysts with atomically dispersed co-promoters of Sn and Zn. When used as the catalyst in the Rochow reaction for the synthesis of dimethyldichlorosilane, this catalyst exhibited much-enhanced activity,selectivity and stability compared with the conventional Cu O catalysts with promoters in the form of nanoparticles. Density functional theory calculations demonstrate that single-atomic Sn substitution in the Cu O surface can enrich surface Cu vacancies and promote dispersion of Zn to its atomic levels. Sn and Zn single sites as the co-promoters cooperatively generate electronic interaction with the Cu O support, which further facilitates the adsorption of the reactant molecules on the surface, thereby leading to the superior catalytic performance.

关键词： dual single-atom promoters CuO catalyst dimethyldichlorosilane synthesis Rochow reaction catalytic performance

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