Surface synergistic effect in well-dispersed Cu/MgO catalysts for highly efficient vapor-phase hydrogenation of carbonyl compounds

被引:64
作者
Liu, Hanwen [1 ]
Hu, Qi [1 ]
Fan, Guoli [1 ]
Yang, Lan [1 ]
Li, Feng [1 ]
机构
[1] Beijing Univ Chem Technol, State Key Lab Chem Resources Engn, Beijing 100029, Peoples R China
基金
中国国家自然科学基金;
关键词
SELECTIVE HYDROGENATION; FURFURYL ALCOHOL; DIMETHYL OXALATE; GAMMA-BUTYROLACTONE; HMS CATALYST; COPPER; OXIDE; DEHYDROGENATION; TEMPERATURE; PERFORMANCE;
D O I
10.1039/c5cy00437c
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
The highly efficient vapor-phase selective hydrogenation of carbonyl compounds (e.g. furfural (FAL) and dimethyl 1,4-cyclohexane dicarboxylate (DMCD)) to corresponding alcohols was achieved excellently over well-dispersed MgO-supported copper catalysts (Cu/MgO), which were prepared by an alternative separate nucleation and aging step method. The characterization results revealed that the structure and catalytic performance of the as-formed Cu/MgO catalysts were profoundly affected by Cu loading. Especially, the results confirmed that the decrease in the Cu loading could lead to the improvement of metal dispersion and the formation of more surface strong Lewis basic sites. In the vapor-phase selective hydrogenation of FAL to furfuryl alcohol (FOL) and DMCD to 1,4-cyclohexane dimethanol (CHDM), two Cu/MgO catalysts with Cu loadings of 27.6 wt% and 70.9 wt% exhibited superior catalytic performance with higher conversions (>97.3%) and selectivities to alcohols (>96.0%) compared to the other supported ones. The high efficiency of the as-formed Cu/MgO catalysts was mainly attributed to the surface synergistic catalytic effect between the catalytically active metallic copper species and the Lewis basic sites, which held the key to the hydrogenation reaction related to the hydrogen dissociation and the activation of the carbonyl groups.
引用
收藏
页码:3960 / 3969
页数:10
相关论文
共 58 条
[31]  
Richard T. S., 2004, J POLYM SCI A, V42, P5847
[32]   Highly active and stable Ni/Ce-ZrO2 catalyst for H2 production from methane [J].
Roh, HS ;
Jun, KW ;
Dong, WS ;
Chang, JS ;
Park, SE ;
Joe, YI .
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 2002, 181 (1-2) :137-142
[33]   Gas-phase hydrogenolysis of dimethyl maleate to 1,4-butanediol and γ-butyrolactone over copper/zinc oxide catalysts [J].
Schlander, JH ;
Turek, T .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 1999, 38 (04) :1264-1270
[34]  
Schlossman M. L., 1981, U. S. Patent No, Patent No. [4301046, 4,301,046]
[35]   Study on the preparation of Cu/ZnO catalyst by sol-gel auto-combustion method and its application for low-temperature methanol synthesis [J].
Shi, Lei ;
Tao, Kai ;
Yang, Ruigin ;
Meng, Fanzhi ;
Xing, Chuang ;
Tsubaki, Noritatsu .
APPLIED CATALYSIS A-GENERAL, 2011, 401 (1-2) :46-55
[36]   A highly efficient Cu/La2O3 catalyst for transfer dehydrogenation of primary aliphatic alcohols [J].
Shi, Ruijuan ;
Wang, Fei ;
Tana ;
Li, Yong ;
Huang, Xiumin ;
Shen, Wenjie .
GREEN CHEMISTRY, 2010, 12 (01) :108-113
[37]   Hydrodeoxygenation of Furfural Over Supported Metal Catalysts: A Comparative Study of Cu, Pd and Ni [J].
Sitthisa, Surapas ;
Resasco, Daniel E. .
CATALYSIS LETTERS, 2011, 141 (06) :784-791
[38]   Kinetics and mechanism of hydrogenation of furfural on Cu/SiO2 catalysts [J].
Sitthisa, Surapas ;
Sooknoi, Tawan ;
Ma, Yuguang ;
Balbuena, Perla B. ;
Resasco, Daniel E. .
JOURNAL OF CATALYSIS, 2011, 277 (01) :1-13
[39]   Real-Time Product Switching Using a Twin Catalyst System for the Hydrogenation of Furfural in Supercritical CO2 [J].
Stevens, James G. ;
Bourne, Richard A. ;
Twigg, Martyn V. ;
Poliakoff, Martyn .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2010, 49 (47) :8856-8859
[40]   Biodiesel production from hempseed oil using alkaline earth metal oxides supporting copper oxide as bi-functional catalysts for transesterification and selective hydrogenation [J].
Su, Mengxing ;
Yang, Ru ;
Li, Min .
FUEL, 2013, 103 :398-407