CU/SiO2 catalysts prepared by the ammonia-evaporation method:: Texture, structure, and catalytic performance in hydrogenation of dimethyl oxalate to ethylene glycol

被引:565
作者
Chen, Liang-Feng [1 ,2 ]
Guo, Ping-Jun [1 ,2 ]
Qiao, Ming-Hua [1 ,2 ]
Yan, Shi-Run [1 ,2 ]
Li, He-Xing [3 ]
Shen, Wei [1 ,2 ]
Xu, Hua-Long [1 ,2 ]
Fan, Kang-Nian [1 ,2 ]
机构
[1] Fudan Univ, Dept Chem, Shanghai 200433, Peoples R China
[2] Fudan Univ, Shanghai Key Lab Mol Catalysis & Innovat Mat, Shanghai 200433, Peoples R China
[3] Shanghai Normal Univ, Dept Chem, Shanghai 200234, Peoples R China
基金
中国国家自然科学基金;
关键词
Cu/SiO2; ammonia-evaporation; copper phyllosilicate; dimethyl oxalate; ethylene glycol; hydrogenation;
D O I
10.1016/j.jcat.2008.04.021
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
CU/SiO2 catalysts prepared by the ammonia-evaporation (AE) method have been systematically characterized focusing on the effect of the AE temperature during catalyst preparation. It is found that the texture, composition, and structure of the calcined and reduced Cu/SiO2 catalysts were profoundly affected by the AE temperature. Based on characterizations and previous findings, the copper species on calcined Cu/SiO2 samples and reduced Cu/SiO2 catalysts were assigned. In gas-phase hydrogenation of dimethyl oxalate (DMO) to ethylene glycol (EG), the evolution of the catalytic activity with the Cu-0 and Cu+ surface areas suggested that Cu+ also participated in the hydrogenation process. The cooperative effect between Cu-0 and Cu+ is proposed to be responsible for the highest hydrogenation activity of the Cu/SiO2 catalyst prepared at the AE temperature of 363 K, on which an EG yield of 98% was obtained under the optimized hydrogenation conditions. (c) 2008 Elsevier Inc. All rights reserved.
引用
收藏
页码:172 / 180
页数:9
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