Plasma-assisted Ru/Zr-MOF catalyst for hydrogenation of CO₂ to methane

【摘要】 As an important type of metal-organic framework（MOF）, Zr-MOF shows excellent CO₂ adsorption performance.In this work, a Zr-MOF was synthesized by a solvothermal method and adopted to support Ru through simple incipient-wetness impregnation.Then the Ru/Zr-MOF was applied for CO₂ hydrogenation（V :V= 4: 1）H CO₂ 2 with the assistance of dielectric barrier discharge（DBD） plasma.The hydrogenation of CO₂ results showed that methane was produced selectively under the synergistic effect between plasma and the Ru/Zr-MOF catalyst, and the selectivity and yield of methane reached 94.6% and 39.1%, respectively.The XRD and SEM analyses indicate that the basic crystalline phase structure and morphology of the Zr-MOF and Ru/Zr-MOF remained the same after DBD plasma treatment, suggesting that the catalysts are stable in plasma.The guest molecules in the pores of the Zr-MOF are removed and the Ru³⁺ions are reduced to metallic Ru⁰ in the reduction atmosphere according to the BET and XPS results, which are responsible for the high performance of plasma with the Ru/Zr-MOF catalyst.In situ optical emission spectra of pure plasma, plasma with Zr-MOF, and plasma with Ru/Zr-MOF were measured, and the active species of C, H and CH for CO₂ hydrogenation were detected.The plasma-assisted Ru/Zr-MOF exhibited high catalytic activity and stability in CO₂ hydrogenation to methane, and it has great guiding significance for CO₂ hydrogenation by using plasma and MOF materials.更多还原

【Abstract】 As an important type of metal-organic framework（MOF）, Zr-MOF shows excellent CO₂ adsorption performance.In this work, a Zr-MOF was synthesized by a solvothermal method and adopted to support Ru through simple incipient-wetness impregnation.Then the Ru/Zr-MOF was applied for CO₂ hydrogenation（V :V= 4: 1）H CO₂ 2 with the assistance of dielectric barrier discharge（DBD） plasma.The hydrogenation of CO₂ results showed that methane was produced selectively under the synergistic effect between plasma and the Ru/Zr-MOF catalyst, and the selectivity and yield of methane reached 94.6% and 39.1%, respectively.The XRD and SEM analyses indicate that the basic crystalline phase structure and morphology of the Zr-MOF and Ru/Zr-MOF remained the same after DBD plasma treatment, suggesting that the catalysts are stable in plasma.The guest molecules in the pores of the Zr-MOF are removed and the Ru³⁺ions are reduced to metallic Ru⁰ in the reduction atmosphere according to the BET and XPS results, which are responsible for the high performance of plasma with the Ru/Zr-MOF catalyst.In situ optical emission spectra of pure plasma, plasma with Zr-MOF, and plasma with Ru/Zr-MOF were measured, and the active species of C, H and CH for CO₂ hydrogenation were detected.The plasma-assisted Ru/Zr-MOF exhibited high catalytic activity and stability in CO₂ hydrogenation to methane, and it has great guiding significance for CO₂ hydrogenation by using plasma and MOF materials.更多还原