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Highly selective hydrogenation of diesters to ethylene glycol and ethanol on aluminum-promoted CuAl/SiO2 catalysts
Catalysis Today ( IF 5.2 ) Pub Date : 2019-12-27 , DOI: 10.1016/j.cattod.2019.12.034
Guoqiang Shu , Kui Ma , Siyang Tang , Changjun Liu , Hairong Yue , Bin Liang

A highly selective CuAl/SiO2 catalyst was prepared for the hydrogenation of dimethyl oxalate (DMO) and ethylene carbonate (EC) to ethanol and ethylene glycol (EG), respectively. Aluminum modified silica sol was used to prepare CuAl/SiO2 catalysts by a hydrothermal method. The catalytic performance of the CuAl/SiO2 catalysts with varying aluminum content was investigated at the conditions of 553 K and 2.5 MPa for DMO hydrogenation, while 453 K and 3 MPa for EC hydrogenation. The results showed that the Cu1.0Al/SiO2 catalyst exhibited the highest selectivity of ethanol (∼94 %) in the DMO hydrogenation, while the Cu0.5Al/SiO2 catalyst exhibited the highest selectivity of EG (∼95 %) and methanol (65 %) in the EC hydrogenation. Characterizations (e.g., TPD, TPR and XANES) indicated that the moderate aluminum modification on SiO2 in the form of triple bondSisingle bondOHsingle bondAl bond could not only tune the support acidity to polarize the Cdouble bondO bond of esters, but also intrinsically facilitate the dispersion of Cu active species to activate H2, which thus facilitated the selective hydrogenation reaction to EG, ethanol and methanol.



中文翻译:

在铝促进的CuAl / SiO 2催化剂上将二酯高度选择性加氢为乙二醇和乙醇

制备了高选择性的CuAl / SiO 2催化剂,用于分别将草酸二甲酯(DMO)和碳酸亚乙酯(EC)加氢为乙醇和乙二醇(EG)。用铝改性的硅溶胶通过水热法制备CuAl / SiO 2催化剂。研究了不同铝含量的CuAl / SiO 2催化剂在DMO加氢条件下的553 K和2.5 MPa,EC加氢条件下的453 K和3 MPa的催化性能。结果表明,Cu1.0Al / SiO 2催化剂在DMO加氢中表现出最高的乙醇选择性(〜94%),而Cu0.5Al / SiO 2催化剂催化剂在EC加氢中表现出最高的EG(〜95%)和甲醇(65%)选择性。表征(例如,TPD,TPR和XANES)表明,SiO 2上呈三键Si 单键OH 单键Al键形式的适度铝修饰不仅可以调节载体的酸度,使双键酯的C O键极化,而且本质上有利于分散。 Cu活性物质可激活H 2,从而促进了对EG,乙醇和甲醇的选择性加氢反应。

更新日期:2019-12-27
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