Facile Synthesis of Cu@CeO2 and Its Catalytic Behavior for the Hydrogenation of Methyl Acetate to Ethanol

被引:52
|
作者
Wang, Yue [1 ]
Zhao, Yujun [1 ]
Lv, Jing [1 ]
Ma, Xinbin [1 ]
机构
[1] Tianjin Univ, Sch Chem Engn & Technol, Collaborat Innovat Ctr Chem Sci & Engn, Key Lab Green Chem Technol,Minist Educ, Tianjin 300072, Peoples R China
基金
中国国家自然科学基金;
关键词
copper; core-shell structures; ethanol; heterogeneous catalysis; hydrogenation; CU/SIO2; CATALYSTS; DIMETHYL OXALATE; ETHYLENE-GLYCOL; PERFORMANCE; SYNGAS; SITES; METHANOL; ETHER;
D O I
10.1002/cctc.201700111
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
The hydrogenation of methyl acetate (MA) is one of the key steps in the synthesis of ethanol from syngas. Given previous studies in this area, synergy of the Cu-0 and Cu+ species is the crux to improving catalytic performance. However, neither Cu-0 nor Cu+ is easy to maintain under reaction conditions comprising abundant H-2 and high temperature. Here, a Cu@CeO2 core-shell catalyst was fabricated by using a facile sol-gel method, and this catalyst exhibited excellent activity and stability in the hydrogenation of MA. It was revealed that the Cu@CeO2 core-shell structure prevented the metallic copper particles from migrating and aggregating and also significantly increased the amount of Cu+ species by enlarging the intimate contact area of copper and ceria. Furthermore, the Cu-0 and Cu+ species were found to be well distributed on the interface between the Cu core and the CeO2 shell. The close relative position of the two active sites is probably the main reason for the enhanced synergetic effect in the hydrogenation of MA. New insight into the core-shell structure-function relationship introduces new possibilities for the rational design of catalysts.
引用
收藏
页码:2085 / 2090
页数:6
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