The conversion of CO_(2)to dimethyl carbonate(DMC)offers a promising route for CO_(2)utilization.In this study,four CeO2 catalysts with distinct nanostructures were synthesized via a template-free hydrothermal method ...The conversion of CO_(2)to dimethyl carbonate(DMC)offers a promising route for CO_(2)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 CO_(2)and methanol.The atomic arrangements of CeO_(2)varied significantly with its morphology,leading to differences in lattice distortion,which directly influenced the concentration of oxygen vacancies.Notably,the CeO_(2)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 CO_(2)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 CeO_(2)catalysts for DMC synthesis.展开更多
基金National Natural Science Foundation of China(22008166)Fundamental Research Program of Shanxi Province(202403021211029,201901D211047).
文摘The conversion of CO_(2)to dimethyl carbonate(DMC)offers a promising route for CO_(2)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 CO_(2)and methanol.The atomic arrangements of CeO_(2)varied significantly with its morphology,leading to differences in lattice distortion,which directly influenced the concentration of oxygen vacancies.Notably,the CeO_(2)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 CO_(2)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 CeO_(2)catalysts for DMC synthesis.
