Efficient ceria-manganese oxide for the direct conversion of CO2 and methanol to dimethyl carbonate

IF 1.7 4区化学 Q4 CHEMISTRY, PHYSICAL

Reaction Kinetics, Mechanisms and Catalysis Pub Date : 2024-08-29 DOI:10.1007/s11144-024-02722-x

Yue Yu, Xiaolu Chen, Ping He, Zhiwen Xu, Xiao Wu, Hong Chen, Songlin Yang, Jia Yu, Shuang Gao

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Abstract

A number of Ce_1-xMn_x catalysts with different Mn contents were prepared by resol-assisted cationic coordinative co-assembly approach and used for the synthesis of dimethyl carbonate (DMC) from CO₂ and methanol. Multiple characterizations of XRD, FT-IR, TEM, BET, CO₂-TPD, NH₃-TPD, H₂-TPR, XPS analyses were applied to investigate the surface properties of the Ce_1-xMn_x catalysts. It turned out that adjusting the proper concentration of Mn ions not only increased the pore volumes, but also improved the content of medium acidic and medium basic sites. When a small amount of Mn was added, the presence of Mn²⁺ on the catalyst surface enhanced, facilitating the conversion of Ce⁴⁺ to Ce³⁺, and leading to higher oxygen vacancy concentration. Consequently, the adsorption and activation of CO₂ and methanol were promoted, and the catalytic efficiency of the reaction was improved. It was found that Ce_0.95Mn_0.05 catalyst exhibited the best catalytic activity, achieving a high DMC yield of 6.44 mmol/g (120 °C, 6.5 MPa, 4 h).

Graphical Abstract

Abstract Image

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将二氧化碳和甲醇直接转化为碳酸二甲酯的高效氧化铈-氧化锰技术

通过解析辅助阳离子配位共组装方法制备了多种不同锰含量的 Ce1-xMnx 催化剂，并将其用于以二氧化碳和甲醇为原料合成碳酸二甲酯（DMC）。采用 XRD、FT-IR、TEM、BET、CO2-TPD、NH3-TPD、H2-TPR、XPS 等多种表征方法研究了 Ce1-xMnx 催化剂的表面性质。结果表明，调整适当的锰离子浓度不仅能增加孔隙体积，还能提高中酸性位点和中碱性位点的含量。当添加少量 Mn 时，催化剂表面 Mn2+ 的存在增强，促进了 Ce4+ 向 Ce3+ 的转化，导致氧空位浓度升高。因此，促进了 CO2 和甲醇的吸附和活化，提高了反应的催化效率。研究发现，Ce0.95Mn0.05 催化剂的催化活性最好，DMC 产率高达 6.44 mmol/g（120 °C，6.5 MPa，4 h）。

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来源期刊

Reaction Kinetics, Mechanisms and Catalysis CHEMISTRY, PHYSICAL-

CiteScore

3.30

自引率

5.60%

发文量

201

审稿时长

2.8 months

期刊介绍： Reaction Kinetics, Mechanisms and Catalysis is a medium for original contributions in the following fields: -kinetics of homogeneous reactions in gas, liquid and solid phase; -Homogeneous catalysis; -Heterogeneous catalysis; -Adsorption in heterogeneous catalysis; -Transport processes related to reaction kinetics and catalysis; -Preparation and study of catalysts; -Reactors and apparatus. Reaction Kinetics, Mechanisms and Catalysis was formerly published under the title Reaction Kinetics and Catalysis Letters.