Importance of the Initial Oxidation State of Copper for the Catalytic Hydrogenation of Dimethyl Oxalate to Ethylene Glycol

doi:10.1002/open.201800225

	Importance of the Initial Oxidation State of Copper for the Catalytic Hydrogenation of Dimethyl Oxalate to Ethylene Glycol
	Ge, Qingjie 1; Sun, Jian 1; Sun, Yannan 1,2; Meng, Fanqiong 1
刊名	CHEMISTRYOPEN
	2018-12-01
卷号	7 期号:12 页码:969-976
关键词	copper esters hydrogenation oxidation state reduction
ISSN号	2191-1363
DOI	10.1002/open.201800225
通讯作者	Sun, Jian(sunj@dicp.ac.cn)
英文摘要	Exposing a Cu-based catalyst to a suitable temperature is of great importance to optimize its hydrogenation performance, as copper is sensitive to temperature. Herein, we investigated the effect of the initial oxidation state of copper, tuned by the reduction temperature, on its catalytic performance in the hydrogenation of dimethyl oxalate (DMO) to ethylene glycol (EG) through designing a series of catalysts with different reduction temperatures (200-350 degrees C). Among these catalysts, the Cu/SiO2 catalyst prepared by ammonia evaporation with a hydrogen reduction process at 250 degrees C showed the best performance in the hydrogenation of DMO with a conversion of 100 % and a selectivity to EG higher than 95 %. The relationship between the initial oxidation state of copper and catalytic performance was well established by characterizing the physicochemical properties of the Cu/SiO2 catalysts by XRD, TEM, H-2 temperature-programmed reduction, N2O adsorption, and in situ reduction Auger electron spectroscopy. The initial oxidation state of copper determined the conversion of DMO and the distribution of the products, and it could be balanced by reducing the temperature to improve the activity of the catalyst. This work provides a reference for further exploration of the mechanism and guidance for the design of catalysts for the hydrogenation of esters.
资助项目	Hundred-Talent Program of Dalian Institute of Chemical Physics ; Youth Innovation Promotion Association of Chinese Academy of Sciences[2018214] ; National Natural Science Foundation of China[21466030]
WOS关键词	VAPOR-PHASE HYDROGENATION ; CU/SIO2 CATALYST ; STRUCTURAL EVOLUTION ; CHEMOSELECTIVE HYDROGENATION ; SELECTIVE HYDROGENATION ; PERFORMANCE ; TEMPERATURE ; STABILITY ; ETHANOL ; SYNGAS
WOS研究方向	Chemistry
语种	英语
出版者	WILEY-V C H VERLAG GMBH
WOS记录号	WOS:000454525600004
资助机构	Hundred-Talent Program of Dalian Institute of Chemical Physics ; Hundred-Talent Program of Dalian Institute of Chemical Physics ; Youth Innovation Promotion Association of Chinese Academy of Sciences ; Youth Innovation Promotion Association of Chinese Academy of Sciences ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Hundred-Talent Program of Dalian Institute of Chemical Physics ; Hundred-Talent Program of Dalian Institute of Chemical Physics ; Youth Innovation Promotion Association of Chinese Academy of Sciences ; Youth Innovation Promotion Association of Chinese Academy of Sciences ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Hundred-Talent Program of Dalian Institute of Chemical Physics ; Hundred-Talent Program of Dalian Institute of Chemical Physics ; Youth Innovation Promotion Association of Chinese Academy of Sciences ; Youth Innovation Promotion Association of Chinese Academy of Sciences ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Hundred-Talent Program of Dalian Institute of Chemical Physics ; Hundred-Talent Program of Dalian Institute of Chemical Physics ; Youth Innovation Promotion Association of Chinese Academy of Sciences ; Youth Innovation Promotion Association of Chinese Academy of Sciences ; National Natural Science Foundation of China ; National Natural Science Foundation of China
内容类型	期刊论文
源URL	[http://cas-ir.dicp.ac.cn/handle/321008/166374]
专题	大连化学物理研究所_中国科学院大连化学物理研究所
通讯作者	Sun, Jian
作者单位	1.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, 457 Zhongshan Rd, Dalian 116023, Peoples R China 2.Univ Chinese Acad Sci, Sch Chem Engn, 380 Huaibeizhuang, Beijing 101408, Peoples R China
推荐引用方式 GB/T 7714	Ge, Qingjie,Sun, Jian,Sun, Yannan,et al. Importance of the Initial Oxidation State of Copper for the Catalytic Hydrogenation of Dimethyl Oxalate to Ethylene Glycol[J]. CHEMISTRYOPEN,2018,7(12):969-976.
APA	Ge, Qingjie,Sun, Jian,Sun, Yannan,&Meng, Fanqiong.(2018).Importance of the Initial Oxidation State of Copper for the Catalytic Hydrogenation of Dimethyl Oxalate to Ethylene Glycol.CHEMISTRYOPEN,7(12),969-976.
MLA	Ge, Qingjie,et al."Importance of the Initial Oxidation State of Copper for the Catalytic Hydrogenation of Dimethyl Oxalate to Ethylene Glycol".CHEMISTRYOPEN 7.12(2018):969-976.