The catalytic direct synthesis of dimethyl carbonate(DMC)from CO_(2)and methanol is a crucial approach to utilizing CO_(2)and producing high-value chemicals.However,the high stability of the CO_(2)molecule imposes the...The catalytic direct synthesis of dimethyl carbonate(DMC)from CO_(2)and methanol is a crucial approach to utilizing CO_(2)and producing high-value chemicals.However,the high stability of the CO_(2)molecule imposes thermodynamic limitations on this reaction pathway,along with challenges related to insufficient catalyst activity and stability.Currently,solutions primarily focus on developing efficient catalyst.Herein,La-doped CeO_(2)nanoflower catalysts(La_(x)CeO_(2))were synthesized via hydrothermal method.Characterization reveals that La doping optimizes the pore structure and enriched oxygen vacancies,thereby enhancing catalytic performance.Notably,La_(0.1)CeO_(2)exhibits the largest pore size and highest oxygen vacancy content,achieving a remarkable DMC productivity of 9.42 mmol/g under 140℃,4 MPa of CO_(2),and 3 h of reactio n,surpassing pure CeO_(2)nano flowers.Based on experimental findings and in-situ diffuse infrared Fourier transform analysis,a plausible reaction pathway was proposed.This work underscores the potential of La_(x)CeO_(2)nano flowers as efficient catalysts for sustainable CO_(2)conversion to DMC.展开更多
基金supported by Jiangsu Province Science and Technology Plan Special Fund(BZ2022053)National Natural Science Foundation of China(42476239)+1 种基金Natural Science Research Projects of Universities in Jiangsu Province(24KJD530004)the Dean/Opening Project of Guangxi Key Laboratory of Petrochemical Resource Processing and Process Intensification Technology(2021K008)。
文摘The catalytic direct synthesis of dimethyl carbonate(DMC)from CO_(2)and methanol is a crucial approach to utilizing CO_(2)and producing high-value chemicals.However,the high stability of the CO_(2)molecule imposes thermodynamic limitations on this reaction pathway,along with challenges related to insufficient catalyst activity and stability.Currently,solutions primarily focus on developing efficient catalyst.Herein,La-doped CeO_(2)nanoflower catalysts(La_(x)CeO_(2))were synthesized via hydrothermal method.Characterization reveals that La doping optimizes the pore structure and enriched oxygen vacancies,thereby enhancing catalytic performance.Notably,La_(0.1)CeO_(2)exhibits the largest pore size and highest oxygen vacancy content,achieving a remarkable DMC productivity of 9.42 mmol/g under 140℃,4 MPa of CO_(2),and 3 h of reactio n,surpassing pure CeO_(2)nano flowers.Based on experimental findings and in-situ diffuse infrared Fourier transform analysis,a plausible reaction pathway was proposed.This work underscores the potential of La_(x)CeO_(2)nano flowers as efficient catalysts for sustainable CO_(2)conversion to DMC.
