The role of CO2 dissociation in CO2 hydrogenation to ethanol on CoCu/silica catalysts

被引:21
|
作者
Wang, Zhongyan [1 ]
Yang, Chengsheng [1 ]
Li, Xianghong [1 ]
Song, Xiwen [1 ]
Pei, Chunlei [1 ]
Zhao, Zhi-Jian [1 ]
Gong, Jinlong [1 ,2 ,3 ]
机构
[1] Tianjin Univ, Collaborat Innovat Ctr Chem Sci & Engn, Key Lab Green Chem Technol, Minist Educ,Sch Chem Engn & Technol, Tianjin 300072, Peoples R China
[2] Tianjin Univ, Joint Sch Natl Univ Singapore & Tianjin Univ, Int Campus, Fuzhou 350207, Peoples R China
[3] Haihe Lab Sustainable Chem Transformat, Tianjin 300192, Peoples R China
基金
国家重点研发计划; 中国国家自然科学基金;
关键词
CO2; hydrogenation; bimetallic catalysts; cobalt catalysts; dissociation; ethanol synthesis; HIGHER ALCOHOL SYNTHESIS; FISCHER-TROPSCH SYNTHESIS; CARBON-DIOXIDE; SYNGAS; MCM-41; METHANOL; SURFACE; ACTIVATION; CONVERSION; REDUCTION;
D O I
10.1007/s12274-022-5092-x
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
CoCu-based catalysts are widely used in COx hydrogenation reactions to produce higher alcohols due to the C-C coupling ability of Co and the ability of Cu to produce alcohols. This work describes the role of easily happened CO2 dissociation on the CoCu surface during the reaction, using different silica support to tune the metal-support interaction, and reaches different selectivity to ethanol. CoCu supported on mesoporous silica MCM-41 shows ethanol selectivity as high as 85.3%, and the ethanol space-time yield (STY) is 0.229 mmol/(g(metal).h), however, poor selectivity to ethanol as low as 28.8% is observed on CoCu supported on amorphous silica. The different selectivity is due to the different intensities of CO2 dissociation on the catalysts. The adsorbed O produced via CO2 dissociation can occupy the cobalt hollow sites on CoCu surfaces, which are also the adsorption sites of C-1 intermediates for further C-C coupling.
引用
收藏
页码:6128 / 6133
页数:6
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