The Nature of Active Copper Species in Cu-HMS Catalyst for Hydrogenation of Dimethyl Oxalate to Ethylene Glycol: New Insights on the Synergetic Effect between Cu0 and Cu+

被引:271
|
作者
Yin, Anyuan
Guo, Xiuying
Dai, Wei-Lin [1 ]
Fan, Kangnian
机构
[1] Fudan Univ, Dept Chem, Shanghai 200433, Peoples R China
来源
JOURNAL OF PHYSICAL CHEMISTRY C | 2009年 / 113卷 / 25期
基金
上海市自然科学基金;
关键词
MESOPOROUS MOLECULAR-SIEVES; RUTHENIUM CARBONYL CARBOXYLATES; SELECTIVE REDUCTION; METHANOL SYNTHESIS; CU/SIO2; CATALYST; PARTICLE-SIZE; DEHYDROGENATION; HYDROGENOLYSIS; NANOPARTICLES; PHASE;
D O I
10.1021/jp902688b
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
Copper-containing mesoporous HMS catalysts prepared via a one-pot synthesis method based on sol-gel chemistry have been systematically characterized focusing on the effect of copper loading. Structural characterization of a series of different copper loading samples was performed by means of N-2 adsorption, X-ray diffraction, Fourier transform infrared spectroscopy, transmission electron microscopy, temperature programmed reduction, N2O titration, and X-ray photoelectron spectroscopy. It is concluded that the copper loading has a great influence on the pore structure of the catalyst. On the basis of the characterizations, the copper species on calcined CuO/HMS samples and reduced Cu/HMS samples were assigned. The synergetic effect between the Cu-0 and Cu+ is considered to be responsible for the enhanced catalytic performance in the hydrogenation of dimethyl oxalate (DMO) to ethylene glycol (EG). The maximum ratio of Cu-0/Cu+ obtained via tuning the copper loading can result in the highest DMO hydrogenation activity and EG selectivity.
引用
收藏
页码:11003 / 11013
页数:11
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