Surface Amine Species Promoted Cu/SiO2 Catalysts for the Hydrogenation of Dimethyl Oxalate to Ethylene Glycol

被引:2
作者
Wang, Meilin [1 ]
Hou, Shixin [1 ]
Yang, Youwei [1 ]
Zhen, Ziheng [1 ]
Lv, Jing [1 ]
Huang, Shouying [1 ,2 ]
Wang, Yue [1 ,2 ,3 ]
Ma, Xinbin [1 ,2 ]
机构
[1] Tianjin Univ, Collaborat Innovat Ctr Chem Sci & Engn, Sch Chem Engn & Technol, Key Lab Green Chem Technol,Minist Educ, Tianjin 300072, Peoples R China
[2] Haihe Lab Sustainable Chem Transformat, Tianjin 300192, Peoples R China
[3] Tianjin Univ, Joint Sch Natl Univ Singapore & Tianjin Univ, Int Campus, Fuzhou 350207, Peoples R China
基金
中国国家自然科学基金;
关键词
VAPOR-PHASE HYDROGENATION; SELECTIVE HYDROGENATION; STRUCTURAL EVOLUTION; PERFORMANCE; CU; OXIDE; TEMPERATURE; ADSORPTION; BEHAVIOR; TEXTURE;
D O I
10.1021/acs.iecr.3c01162
中图分类号
TQ [化学工业];
学科分类号
0817 ;
摘要
Hydrogenation of dimethyl oxalate (DMO) to ethylene glycol(EG)is a critical step in the syngas-to-EG route. Cu/SiO2 catalystsprepared by ammonia-evaporation method exhibited stable and highlydispersed copper species during the DMO hydrogenation which has beenused in the industry. However, the catalytic activity and the selectivityof EG require further enhancement. Herein, we prepared a series ofsurface modified Cu/SiO2 catalysts with amine species bypostgrafting method using organic silane coupling agents. Detailedcharacterizations indicated that the introduced amine species couldreduce the amounts and intensity of basic sites, contributing to thereduction of byproducts (C-3-C4OH) selectivity,and consequently improve the EG selectivity. The amine species alsoshowed an electron-donating effect and significantly increased theproportion of Cu-0 species. Meanwhile, it is demonstratedthat there was a linear correlation between the TOFCu andmedium-strong basic sites induced by amine species, indicating thesynergistic catalysis between copper species and medium-strong basicsites accounted for the superior catalytic activity in DMO hydrogenation.These insights into the effects of the introduction of amine speciescould lead to new possibilities for the improvement of Cu/SiO2 catalysts for ester hydrogenations toward industrial applications.
引用
收藏
页码:10399 / 10408
页数:10
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