Highly active and selective copper-containing HMS catalyst in the hydrogenation of dimethyl oxalate to ethylene glycol
Highly active and selective copper-containing HMS catalyst in the hydrogenation of dimethyl oxalate to ethylene glycol
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DOI：
10.1016/j.apcata.2008.07.020
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发表时间：
2008-10
影响因子：
5.5
通讯作者：
A. Yin;Xiuying Guo;W. Dai;Hexing Li;Kangnian Fan
中科院分区：
文献类型：
--
作者：
A. Yin;Xiuying Guo;W. Dai;Hexing Li;Kangnian Fan
采用浸渍法制备了含铜介孔氧化硅HMS催化剂。采用N2物理吸附、X射线衍射、透射电镜、H2程序升温还原、傅里叶变换红外光谱、N2 O滴定和X射线光电子能谱等手段对催化剂的表面结构进行了表征。结果表明，含铜HMS催化剂在草酸二甲酯选择加氢制乙二醇反应中表现出上级的催化性能。在473 K、2.5MPa氢气压力、草酸二甲酯液时空速为0.2h-1的条件下，草酸二甲酯的转化率可达100%，乙二醇的选择性可达92 Cu-HMS催化剂。铜-HMS催化剂的增强的催化性能可归因于活性铜物种的均匀分散和均匀性以及在具有大孔径和表面积的HMS载体上获得的较大的铜表面积。
Copper-containing mesoporous silica HMS catalysts were prepared by an impregnation method. The surface structures of these catalysts were characterized by N2-physisorption, X-ray diffraction, transmission electron microscopy, H2temperature-programmed reduction, Fourier transform infrared spectroscopy, N2O titration and X-ray photoelectron spectroscopy. The results show that the copper-containing HMS catalysts exhibit superior catalytic performance in the selective hydrogenation of dimethyl oxalate to ethylene glycol compared to the commercial silica-supported ones obtained by the same method. The dimethyl oxalate conversion can reach 100% and the ethylene glycol selectivity can reach 92% at 473K with 2.5MPa H2pressure and 0.2h−1liquid hour space velocity of dimethyl oxalate over the 5wt.% Cu-HMS catalyst. The enhanced catalytic performance of copper-HMS catalysts may be attributed to the homogeneous dispersion and uniformity of the active copper species and to the larger copper surface areas attained on the HMS supports with large pore diameters and surface areas.