Study of Direct Synthesis of DMC from CO 2 and Methanol on CeO 2 : Theoretical Calculation and Experiment

作者：Daoyun Zhu, Haiou Liu, Yangqiang Huang, Xiao Luo, Yu Mao, Zhiwu Liang · 发表于：Industrial & Engineering Chemistry Research · 年份：2022 · DOI：10.1021/acs.iecr.2c01522 · 被引用次数：34 · 研究领域：Carbon dioxide utilization in catalysis、Catalysts for Methane Reforming、Catalytic Processes in Materials Science

Rare earth metal oxides are known to have good catalytic effectiveness in the direct synthesis of dimethyl carbonate (DMC) from CO 2 and methanol. In this work, we screened ceria (CeO 2 ) catalysts by analyzing their capacity for CO 2 adsorption. The effects of the crystal surface morphology and oxygen vacancy on the catalytic performance of the ceria catalyst were studied by using density functional theory (DFT). The results show that the (110) surface and higher oxygen vacancy content can better promote the synthesis of DMC and that the rod-shaped CeO 2 catalyst has a better catalytic effect. The oxygen vacancy content on the catalyst was improved by freeze-drying and confirmed by thermogravimetric analysis, Raman spectroscopy, and electron paramagnetic resonance. The freeze-dried CeO 2 (CeO 2 -FD) then showed a higher catalytic performance. The conversion rate of methanol and the yield of DMC were 33.95% and 584 mmol g –1 cat, respectively, under mild conditions (140 °C and 1 MPa).