Effect of boric oxide doping on the stability and activity of a Cu-SiO2 catalyst for vapor-phase hydrogenation of dimethyl oxalate to ethylene glycol

被引:345
|
作者
He, Zhe
Lin, Haiqiang
He, Ping
Yuan, Youzhu [1 ]
机构
[1] Xiamen Univ, Coll Chem & Chem Engn, State Key Lab Phys Chem Solid Surfaces, Xiamen 361005, Peoples R China
基金
中国国家自然科学基金;
关键词
Silica-supported copper; Boric oxide; Ethylene glycol; Hydrogenation; Stability; SUPPORTED COPPER-CATALYSTS; ION-EXCHANGE METHOD; CU/SIO2; CATALYSTS; HMS CATALYST; CU CATALYSTS; HYDROGENOLYSIS; OXIDATION; CO; METHANOL; SURFACE;
D O I
10.1016/j.jcat.2010.10.010
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
Stable and efficient B-Cu-SiO2 catalysts for the hydrogenation of dimethyl oxalate (DMO) to ethylene glycol were prepared through urea-assisted gelation followed by postimpregnation with boric acid. Auger electron spectroscopy and CO adsorption by in situ Fourier transform infrared spectroscopy revealed that the Cu+ species on the catalyst surface increased together with an increase in the amount of boric oxide dopant. X-ray diffraction and N2O chemisorption indicated that a suitable amount of boric oxide doping tended to improve copper dispersion and retard the growth of copper particles during DMO hydrogenation. Catalytic stability was greatly enhanced in the B-Cu-SiO2 catalyst with an optimized Cu/B atomic ratio of 6.6, because of the formation and preservation of appropriate distributions of Cu+ and Cu-0 species on the catalyst surfaces. The effect of boric oxide was attributed to its relatively high affinity for electrons, which tended to lower the reducibility of the Cu+ species. (C) 2010 Elsevier Inc. All rights reserved.
引用
收藏
页码:54 / 63
页数:10
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