燃料化学学报2025,Vol.53Issue(11):1590-1602,13.DOI:10.1016/S1872-5813(25)60577-9
CeO2晶格畸变对CO2和甲醇直接合成碳酸二甲酯的影响
Effect of lattice distortion of CeO2 on direct synthesis of dimethyl carbonate from CO2 and methanol
摘要
Abstract
The conversion of CO2 to dimethyl carbonate(DMC)offers a promising route for CO2 utilization.In this study,four CeO2 catalysts with distinct nanostructures were synthesized via a template-free hydrothermal method by systematically varying the types and concentrations of precipitants as well as the hydrothermal reaction conditions,and they were employed for DMC synthesis from CO2 and methanol.The atomic arrangements of CeO2 varied significantly with its morphology,leading to differences in lattice distortion,which directly influenced the concentration of oxygen vacancies.Notably,the CeO2 nanospheres,which exhibited the highest lattice distortion and oxygen vacancy concentration,achieved a DMC yield(11.12 mmol/g)48 times greater than that of the nanocubes(0.23 mmol/g).The results indicated that oxygen vacancies played a pivotal role in the catalytic process by facilitating the adsorption and activation of CO2 to form bidentate carbonates,as well as activating methanol to generate methoxy species.These processes collectively promoted the formation of the key intermediate(*CH3OCOO).This study proposes a strategy to enhance the oxygen vacancy concentration by increasing lattice distortion,providing valuable insights for designing high-performance CeO2 catalysts for DMC synthesis.关键词
二氧化铈/晶格畸变/氧空位Key words
cerium dioxide/lattice distortion/oxygen vacancy分类
化学工程引用本文复制引用
赵江涛,艾培培,张旭妍,邵旭浩,谭明慧,黄伟..CeO2晶格畸变对CO2和甲醇直接合成碳酸二甲酯的影响[J].燃料化学学报,2025,53(11):1590-1602,13.基金项目
The project was supported by National Natural Science Foundation of China(22008166),Fundamental Research Program of Shanxi Province(202403021211029,201901D211047). (22008166)