Carbon template synthesis of CeO2 catalyst for direct conversion of methanol and carbon dioxide to dimethyl carbonate

被引:7
|
作者
Chen, Shiping [1 ]
Li, Xin [1 ]
Lin, Liqin [1 ]
Jing, Xiaolian [1 ]
Weng, Wenting [1 ]
机构
[1] Quanzhou Normal Univ, Coll Chem Engn & Mat Sci, Dept Chem Engn & Technol, Quanzhou 362000, Fujian, Peoples R China
关键词
CO2; utilization; Dimethyl carbonate; Methanol; CeO2; Coconut shell activated carbon; DIRECT CARBOXYLATION; OXYGEN-VACANCY; CO2; SURFACE; PERFORMANCE; COMPOSITES; DMC;
D O I
10.1016/j.joei.2023.101190
中图分类号
TE [石油、天然气工业]; TK [能源与动力工程];
学科分类号
0807 ; 0820 ;
摘要
Dimethyl carbonate (DMC) is an interesting, value added chemical and a high energy additive to fuels. In this study, several CeO2 catalysts were successfully synthesized through carbon template method using two renew-able sources of activated carbon. The structure of catalysts was fully resolved by XRD, SEM, N-2-adsorption, NH3- TPD, CO2-TPD and XPS. CeO2 catalysts prepared using coconut shell activated carbon (CAC) template exhibit better surface morphology and improved catalytic performance compared to walnut shell activated carbon (WAC)-supported catalysts. We demonstrated a correlation between the efficiency of DMC synthesis and the abundance of moderately acidic and moderately basic active sites on the catalyst. It was found that the presence of oxygen vacancies (Vo) facilitates carbonyl bond cleavage of CO2. The best-performing catalyst was 4% CeO2/CAC owing to the richest Vo and the optimum acid/base properties. Moreover, a plausible catalytic mechanism of DMC formation was proposed, and includes the interaction between methoxy carbonate (CH3OCO2-) formed with the aid of Vo and moderately basic sites and methyl cation (CH3+) formed on the moderately acidic sites.
引用
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页数:7
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