The effective and stable Cu-C@SiO2 catalyst for the syntheses of methanol and ethylene glycol via selective hydrogenation of ethylene carbonate

doi:10.1016/j.ijhydene.2021.02.166

	The effective and stable Cu-C@SiO2 catalyst for the syntheses of methanol and ethylene glycol via selective hydrogenation of ethylene carbonate
	Chen, Xinwei 4,5; Wang, Liguo 1,2,4; Zhang, Chanjuan 2,4; Tu, Weixia 5; Cao, Yan 4; He, Peng 4; Li, Jiachen 2,4; Li, Huiquan 2,3,4
刊名	INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
	2021-05-13
卷号	46 期号:33 页码:17209-17220
关键词	Ethylene carbonate Hydrogenation Methanol Ethylene glycol Cu-C@SiO2, stable
ISSN号	0360-3199
DOI	10.1016/j.ijhydene.2021.02.166
英文摘要	The co-production of ethylene glycol and methanol via ethylene carbonate hydrogenation derived from CO2 has attracted great concerns because of the promising chemical utilization of CO2 in large-scale. Copper-based catalysts are widely concerned in hydrogenation of ester due to the high catalytic efficiency and low cost, but the stability of copper-based catalyst is poor and needs to be further improved. In this study, the modification Cu-C@SiO2-R catalyst with graphite oxide was prepared by using Cu-3(BTC)(2) as the precursor and ammonia evaporation method, and was applied in ethylene carbonate hydrogenation to synthesis ethylene glycol and methanol. Furthermore, the catalysts were characterized in detail. The results showed that the Cu-C@SiO2-R catalyst was modified with graphite oxide, the average size of Cu particles was 2.9 nm and Cu particles had good dispersion. In addition, both Cu-C@SiO2-R and Cu@SiO2-R catalysts had similar ratio of Cu+/(Cu-0+Cu+). In a batch reactor, under 453 K, 5 MPa, 4 h, the catalytic efficiency was 80.0% EC conversion 92.2% EG and 70.8% MeOH selectivity showing excellent catalytic performance capability of Cu-C@SiO2-R catalyst. In long-term experiment, the Cu-C@SiO2-R catalyst showed excellent stability after using for 264 h. The activity was 0.63 gEC g(cat)(-1) h(-1), and 100.0% EC conversion 99.9% EG and 85.8% MeOH selectivity could be achieved in a fixed bed. After the long-term experiment, the Cu+ /(Cu++Cu-0) ratio in Cu-C@SiO2-R catalyst kept at around 0.48. In contrast, the Cu+/(Cu++Cu-0) ratio in Cu@SiO2-R catalyst decreased sharply from 0.48 to 0.38. The stability of the structure and the balance of valence of Cu were considered to be responsible to the stability of Cu-C@SiO2-R catalyst, because the graphite oxide not only kept the Cu+/(Cu-0+Cu+) ratio stability, but also restrained the aggregation of Cu particles and loss of copper. This work provides an in-depth understanding of the stabilization mechanism of Cu and can be a reference for the industrial application of ethylene carbonate hydrogenation. (C) 2021 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.
资助项目	National Natural Science Foundation of China[21576272] ; Science and Technology Service Network Initiative, Chinese Academy of Sciences[KFJSTSQYZD138] ; Strategic Priority Research Program of Chinese Academy of Sciences[XDA 21030600]
WOS关键词	ONE-POT SYNTHESIS ; DIMETHYL OXALATE ; CU/SIO2 CATALYST ; CHEMOSELECTIVE HYDROGENATION ; EFFICIENT HYDROGENATION ; CU-SIO2 CATALYSTS ; COPPER-CATALYSTS ; FACILE SYNTHESIS ; CO2 ; OXIDATION
WOS研究方向	Chemistry ; Electrochemistry ; Energy & Fuels
语种	英语
出版者	PERGAMON-ELSEVIER SCIENCE LTD
WOS记录号	WOS:000646140200015
资助机构	National Natural Science Foundation of China ; Science and Technology Service Network Initiative, Chinese Academy of Sciences ; Strategic Priority Research Program of Chinese Academy of Sciences
内容类型	期刊论文
源URL	[http://ir.ipe.ac.cn/handle/122111/48767]
专题	中国科学院过程工程研究所
通讯作者	Wang, Liguo; Tu, Weixia
作者单位	1.Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China 2.Univ Chinese Acad Sci, Sino Danish Coll, Beijing 100049, Peoples R China 3.Univ Chinese Acad Sci, Sch Chem Engn, Beijing 100049, Peoples R China 4.Chinese Acad Sci, Inst Proc Engn, CAS Key Lab Green Proc & Engn, Natl Engn Lab Hydromet Cleaner Prod Technol, Beijing 100190, Peoples R China 5.Beijing Univ Chem Technol, Coll Chem Engn, Beijing 100029, Peoples R China
推荐引用方式 GB/T 7714	Chen, Xinwei,Wang, Liguo,Zhang, Chanjuan,et al. The effective and stable Cu-C@SiO2 catalyst for the syntheses of methanol and ethylene glycol via selective hydrogenation of ethylene carbonate[J]. INTERNATIONAL JOURNAL OF HYDROGEN ENERGY,2021,46(33):17209-17220.
APA	Chen, Xinwei.,Wang, Liguo.,Zhang, Chanjuan.,Tu, Weixia.,Cao, Yan.,...&Li, Huiquan.(2021).The effective and stable Cu-C@SiO2 catalyst for the syntheses of methanol and ethylene glycol via selective hydrogenation of ethylene carbonate.INTERNATIONAL JOURNAL OF HYDROGEN ENERGY,46(33),17209-17220.
MLA	Chen, Xinwei,et al."The effective and stable Cu-C@SiO2 catalyst for the syntheses of methanol and ethylene glycol via selective hydrogenation of ethylene carbonate".INTERNATIONAL JOURNAL OF HYDROGEN ENERGY 46.33(2021):17209-17220.