Citation: Jiaju Liu, Peng He, Liguo Wang, Hui Liu, Yan Cao, Huiquan Li. An efficient and stable Cu/SiO₂ catalyst for the syntheses of ethylene glycol and methanol via chemoselective hydrogenation of ethylene carbonate[J]. Chinese Journal of Catalysis, ;2018, 39(8): 1283-1293. doi: 10.1016/S1872-2067(18)63032-3 shu

An efficient and stable Cu/SiO₂ catalyst for the syntheses of ethylene glycol and methanol via chemoselective hydrogenation of ethylene carbonate

Jiaju Liu ^a,c, ,
Peng He ^a ,
Liguo Wang ^a,b,d ,
Hui Liu ^c ,
Yan Cao ^a ,
Huiquan Li ^a,d

a National Engineering Laboratory for Hydrometallurgical Cleaner Production Technology, Key Laboratory of Green Process and Engineering, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China;
b Jiangsu Collaborative Innovation Center for Ecological Building Materials and Environmental Protection Equipments, Yancheng Institute of Technology, Key Laboratory for Advanced Technology in Environmental Protection of Jiangsu Province, Yancheng 224051, Jiangsu, China;
c Beijing University of Chemical Technology, Beijing 100029, China;
d Sino-Danish College, University of Chinese Academy of Sciences, Beijing 100049, China

Received Date: 15 November 2017
Revised Date: 11 January 2018

Fund Project: This work was supported by the National Natural Science Foundation of China (21576272, 21406245), the project from Jiangsu Collaborative Innovation Center for Ecological Building Materials and Environmental Protection Equipments (YCXT201607), and the "Transformational Technologies for Clean Energy and Demonstration", Strategic Priority Research Program of the Chinese Academy of Sciences (XDA21030600).

The efficient synthesis of methanol and ethylene glycol via the chemoselective hydrogenation of ethylene carbonate (EC) is important for the sustainable utilization of CO₂ to produce commodity chemicals and fuels. In this work, a series of β-cyclodextrin-modified Cu/SiO₂ catalysts were prepared by ammonia evaporation method for the selective hydrogenation of EC to co-produce methanol and ethylene glycol. The structure and physicochemical properties of the catalysts were characterized in detail by N₂ physisorption, XRD, N₂O titration, H₂-TPR, TEM, and XPS/XAES. Compared with the unmodified 25Cu/SiO₂catalyst, the involvement of β-cyclodextrin in 5β-25Cu/SiO₂ could remarkably increase the catalytic activity-excellent activity of 1178 mg_EC g_cat^-1 h^-1 with 98.8% ethylene glycol selectivity, and 71.6% methanol selectivity could be achieved at 453 K. The remarkably improved recyclability was primarily attributed to the remaining proportion of Cu⁺/(Cu⁰+Cu⁺). Furthermore, the DFT calculation results demonstrated that metallic Cu⁰ dissociated adsorbed H₂, while Cu⁺ activated the carbonyl group of EC and stabilized the intermediates. This study is a facile and efficient method to prepare highly dispersed Cu catalysts-this is also an effective and stable heterogeneous catalyst system for the sustainable synthesis of ethylene glycol and methanol via indirect chemical utilization of CO₂.
- Ethylene carbonate,
- Hydrogenation,
- β-Cyclodextrin,
- Cu/SiO₂,
- Methanol,
- Ethylene glycol
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An efficient and stable Cu/SiO2 catalyst for the syntheses of ethylene glycol and methanol via chemoselective hydrogenation of ethylene carbonate

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通讯作者: 陈斌, bchen63@163.com

An efficient and stable Cu/SiO₂ catalyst for the syntheses of ethylene glycol and methanol via chemoselective hydrogenation of ethylene carbonate