Selective hydrogenation of ethylene carbonate to methanol and ethylene glycol over Cu/SiO2 catalysts prepared by ammonia evaporation method
Selective hydrogenation of ethylene carbonate to methanol and ethylene glycol over Cu/SiO2 catalysts prepared by ammonia evaporation method
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氨蒸发法制备的Cu/SiO2催化剂上碳酸乙烯酯选择性加氢制甲醇和乙二醇
DOI：
10.1016/j.ijhydene.2016.09.064
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发表时间：
2017-01-26
影响因子：
7.2
通讯作者：
Li, Huiquan
中科院分区：
文献类型：
--
作者：
Li, Fengjiao;Wang, Liguo;Li, Huiquan
以硅溶胶为硅源，采用蒸氨法制备了一系列不同铜负载量的Cu/SiO2-AE催化剂。系统的催化剂表征表明，不同比例的Cu度和Cu+物种共存的Cu/SiO2-AE催化剂，这来自CuO和层状硅酸铜的还原，分别。将所制备的催化剂用于碳酸乙烯酯（EC）加氢联产甲醇（MeOH）和乙二醇（EG）的反应。在所考察的催化剂中，Cu负载量适中的10%Cu/SiO2-AE催化剂表现出较好的催化活性和产物选择性，这主要归因于Cu度和Cu+物种的协同作用以及Cu+/（Cu++Cu度）的合适比例。结果表明，Cu ~（2+）物种吸附在EC的羰基上，而Cu ~（2+）物种则促进了H ~-2的解离。在优化的反应条件下，10%Cu/SiO2-AE催化剂上EC转化率为100%，甲醇选择性为70.8%，乙二醇选择性为98.0%。催化剂的重复使用性能表明，Cu和Cu 2 O颗粒的团聚是导致10%Cu/SiO2-AE催化剂活性沿着循环次数的增加而逐渐降低的主要原因。(C)2016年氢能出版有限责任公司。由爱思唯尔有限公司出版。保留所有权利。
A series of Cu/SiO2-AE catalysts with different copper loadings were prepared by ammonia evaporation method with silica sol as the silica source. The systematic catalyst characterization revealed that different proportions of Cu degrees and Cu+ species co-existed in the Cu/SiO2-AE catalysts, which derived from the reduction of CuO and copper phyllosilicate, respectively. The as-prepared catalysts were employed in the hydrogenation of ethylene carbonate (EC) to co-produce methanol (MeOH) and ethylene glycol (EG). Among the catalysts investigated, the 10%Cu/SiO2-AE catalyst with a moderate copper loading exhibited better catalytic activity and product selectivities, which was mainly ascribed to the synergetic effect of Cu degrees and Cu+ species and the suitable proportion of Cu+/(Cu++Cu degrees). It was proposed that the Cu degrees species promoted the dissociation of H-2, while Cu+ species adsorbed on the carbonyl group of EC. Under the optimized conditions, EC conversion of 100%, MeOH selectivity of 70.8% and EG selectivity of 98.0% were obtained over the 10%Cu/SiO2-AE catalyst. The catalyst reusability results showed that the agglomeration of Cu and Cu2O particles was responsible for the gradually decreasing activity of 10%Cu/SiO2-AE catalyst along with recycling runs. (C) 2016 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.