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:351
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
相关论文
共 49 条
[1]  
Bartley W. J., 1987, US Pat, Patent No. 4677234
[2]   FTIR study of carbon monoxide oxidation and scrambling at room temperature over copper supported on ZnO and TiO2 .1. [J].
Boccuzzi, F ;
Chiorino, A .
JOURNAL OF PHYSICAL CHEMISTRY, 1996, 100 (09) :3617-3624
[3]   Ester hydrogenolysis over promoted Cu/SiO2 catalysts [J].
Brands, DS ;
Poels, EK ;
Bliek, A .
APPLIED CATALYSIS A-GENERAL, 1999, 184 (02) :279-289
[4]   FT-IR STUDY OF THE SURFACE OF COPPER-OXIDE [J].
BUSCA, G .
JOURNAL OF MOLECULAR CATALYSIS, 1987, 43 (02) :225-236
[5]   Selective synthesis of isobutanol by means of the Guerbet reaction Part 2.: Reaction of methanol/ethanol and methanol/ethanol/n-propanol mixtures over copper based/MeONa catalytic systems [J].
Carlini, C ;
Di Girolamo, M ;
Macinai, A ;
Marchionna, M ;
Noviello, M ;
Galletti, AMR ;
Sbrana, G .
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 2003, 200 (1-2) :137-146
[6]  
Chen G.S., 1992, CHIN J CATAL, V13, P291
[7]   Catalytic partial oxidation of methane to syngas over Ca-decorated-Al2O3-supported Ni and NiB catalysts [J].
Chen, L ;
Lu, Y ;
Hong, Q ;
Lin, J ;
Dautzenberg, FM .
APPLIED CATALYSIS A-GENERAL, 2005, 292 :295-304
[8]   CU/SiO2 catalysts prepared by the ammonia-evaporation method:: Texture, structure, and catalytic performance in hydrogenation of dimethyl oxalate to ethylene glycol [J].
Chen, Liang-Feng ;
Guo, Ping-Jun ;
Qiao, Ming-Hua ;
Yan, Shi-Run ;
Li, He-Xing ;
Shen, Wei ;
Xu, Hua-Long ;
Fan, Kang-Nian .
JOURNAL OF CATALYSIS, 2008, 257 (01) :172-180
[9]   CO OXIDATION OVER PD AND CU CATALYSTS .4. PREREDUCED AL2O3-SUPPORTED COPPER [J].
CHOI, KI ;
VANNICE, MA .
JOURNAL OF CATALYSIS, 1991, 131 (01) :22-35
[10]   SELECTIVE HYDROGENOLYSIS OF METHYL AND ETHYL-ACETATE IN THE GAS-PHASE ON COPPER AND SUPPORTED GROUP-VIII METAL-CATALYSTS [J].
CLAUS, P ;
LUCAS, M ;
LUCKE, B ;
BERNDT, T ;
BIRKE, P .
APPLIED CATALYSIS, 1991, 79 (01) :1-18