Insight into the Synergism between Copper Species and Surface Defects Influenced by Copper Content over Copper/Ceria Catalysts for the Hydrogenation of Carbonate

被引:40
作者
Li, Huabo [1 ]
Cui, Yuanyuan [1 ]
Liu, Qianqian [1 ]
Dai, Wei-Lin [1 ]
机构
[1] Fudan Univ, Shanghai Key Lab Mol Catalysis & Innovat Mat, Dept Chem, Shanghai 200433, Peoples R China
基金
上海市自然科学基金; 中国国家自然科学基金;
关键词
copper; hydrogenation; supported catalysts; surface defects; synergism; DIMETHYL OXALATE; ETHYLENE-GLYCOL; HETEROGENEOUS HYDROGENATION; EFFICIENT HYDROGENATION; STRUCTURAL EVOLUTION; METHANOL SYNTHESIS; CYCLIC CARBONATES; CU/SIO2; CATALYSTS; OXYGEN VACANCIES; NANOSCALE CERIA;
D O I
10.1002/cctc.201701384
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
Various Cu/CeO2 nanorod catalysts with different copper contents were synthesized through a facile coprecipitation method for the hydrogenation of diethyl carbonate to methanol in a fixed-bed reactor. The methanol yield increased upon increasing the copper loading, but large excess amounts of copper led to deactivation of the catalyst at a high liquid hourly space velocity because of aggregation of the active metal. The 20Cu/CeO2 and 30Cu/CeO2 catalysts displayed superior catalytic performance with methanol space-time yields of 8.4 and 8.1 mmol g(cat)(-1)h(-1), respectively. The remarkably enhanced catalytic performance was mainly ascribed to a high Cu-0 surface area, appropriate ratio of Cu+/Cu-0, and more surface oxygen vacancies associated with Ce3+, which stemmed from a strong interaction between Cu and the CeO2 support.
引用
收藏
页码:619 / 624
页数:6
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