CeO2/Beta composite catalysts in dimethyl carbonate synthesis from CO2: effect of preparation method on surface oxygen species

IF 1.7 4区化学 Q4 CHEMISTRY, PHYSICAL

Reaction Kinetics, Mechanisms and Catalysis Pub Date : 2024-11-03 DOI:10.1007/s11144-024-02755-2

Fei Wang, Biao Da, Tiantian Wan, Yue Zhang, Na Liu, Qingxiang Ma, Jie Xu, Bing Xue, Xuejiao Wei

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引用次数: 0

Abstract

Two kinds of CeO₂/Beta composite catalysts were prepared by precipitation method (CeB-p) and hydrothermal method (CeB-h), respectively. The physicochemical properties of all samples were studied in detail by combining XRD, XPS, SEM, TEM, N₂ sorption, NH₃-TPD and CO₂-TPD techniques. CeB-p catalyst exhibited a higher dimethyl carbonate (DMC) yield than the CeB-h catalyst at the similar conditions for DMC synthesis from CO₂ and methanol. This enhanced activity of CeB-p catalyst was attributed to enhanced acid–base properties modulated by abundant surface lattice oxygen species rather than oxygen vacancies. Compared with the inertly adsorbed methoxy induced by the oxygen vacancy enriched CeB-h, abundant surface lattices oxygen species in CeB-p catalyst facilitated the formation of weakly absorbed methoxy species, which resulted in the shift of the rate-determining step and the reduction of reaction energy barrier. This study offered guidance for the rational design and fabrication of high-performance DMC synthesis catalysts based on CeO₂/Beta composite.

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CO2合成碳酸二甲酯中CeO2/Beta复合催化剂制备方法对表面氧的影响

采用沉淀法（CeB-p）和水热法（CeB-h）制备了两种CeO2/Beta复合催化剂。采用XRD、XPS、SEM、TEM、N2吸附、NH3-TPD、CO2-TPD等技术对样品的理化性质进行了详细研究。在相同条件下，CeB-p催化剂的碳酸二甲酯（DMC）产率高于CeB-h催化剂。CeB-p催化剂活性的增强归因于丰富的表面晶格氧而不是氧空位所调节的酸碱性质的增强。与富氧空位的CeB-h诱导的惰性吸附甲氧基相比，CeB-p催化剂中丰富的表面晶格氧促进了弱吸附甲氧基的形成，导致了决定速率步骤的移动和反应能垒的降低。该研究为合理设计和制备基于CeO2/Beta复合材料的高性能DMC合成催化剂提供了指导。

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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.