ZnO supported on Cu2O{100} enhances charge transfer in dimethyldichlorosilane synthesis

被引:27
作者
Li, Jing [1 ]
Ni, Zibin [2 ]
Ji, Yongjun [1 ,5 ]
Zhu, Yongxia [1 ]
Liu, Hezhi [1 ]
Zhang, Yu [1 ]
Gong, Xue-Qing [2 ]
Zhong, Ziyi [3 ]
Su, Fabing [1 ,4 ,5 ]
机构
[1] Chinese Acad Sci, Inst Proc Engn, State Key Lab Multiphase Complex Syst, Beijing 100190, Peoples R China
[2] East China Univ Sci & Technol, Sch Chem & Mol Engn, Ctr Computat Chem, Key Lab Adv Mat,Res Inst Ind Catalysis, Shanghai 200237, Peoples R China
[3] GTIIT, Coll Engn, 241 Daxue Rd, Shantou 515063, Peoples R China
[4] Shenyang Univ Chem Technol, Inst Ind Chem & Energy Technol, Shenyang 110142, Liaoning, Peoples R China
[5] Langfang Econ & Tech Dev Zone, Zhongke Langfang Inst Proc Engn, Fenghua Rd 1, Langfang 065001, Hebei, Peoples R China
基金
中国国家自然科学基金;
关键词
Cu2O nanocrystal; Exposed facet; ZnO/Cu2O heterostructure; Rochow reaction; Catalytic activity; INITIO MOLECULAR-DYNAMICS; METAL-CATALYZED SYNTHESIS; CUO MICROSPHERES; ROCHOW REACTION; COPPER-CATALYSTS; METHYL-CHLORIDE; PHASE; PERFORMANCE; MECHANISM; METHYLCHLOROSILANES;
D O I
10.1016/j.jcat.2019.02.029
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
In this work, three types of ZnO/Cu2O heterostructures were synthesized by depositing ZnO nanoparticles on the supports of Cu2O cubes, Cu2O octahedrons and Cu2O dodecahedrons with different exposed facets. These catalysts were used for the Rochow reaction, which is an important industrial process for the synthesis of organosilicon polymers. It was demonstrated that Cu2O cubes-supported ZnO catalyst is the most active toward dimethyldichlorosilane formation, while Cu2O dodecahedrons-supported ZnO catalyst is the least active. Both experimental results and density functional theory calculations show that, in the three cases, the charge transfer efficiency between the ZnO nanoparticle and the Cu2O{1 0 0} plane is the highest, which enhances the dissociative adsorption of methylchloride at Cu2O{1 0 0}, the subsequent reduction of Cu+ into Cu-0 and the final formation of the Cu3Si active phases. This work reveals essential information about how the Rochow reaction proceeds on the ZnO/Cu2O catalyst and demonstrates a practical strategy to rationally design highly efficient catalytic system in heterogeneous catalysis. (C) 2019 Elsevier Inc. All rights reserved.
引用
收藏
页码:284 / 296
页数:13
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