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The fundamental insights of the reaction mechanism, especially the synergistic effect between oxygen vacancies and basic sites, are highly promising yet challenging for Ru-based catalysts during carbon dioxide (CO2) methanation. Herein, a series of Ru-based catalysts were employed to study the mechanism of CO2 methanation. It is found that Ru/CeO2 catalyst exhibits a much higher CO2 conversion (86%) and CH4 selectivity (100%), as well as excellent stability of 30 h due to the existence of abundant oxygen vacancies and weak basic sites. Additionally, the in-situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and density functional theory (DFT) calculations reveal that the formate formation step dominated the hydrogenation route on Ru/CeO2 catalyst, and the b-HCOO* could be the key intermediate due to b-HCOO* is more easily hydrogenated to methane than m-HCOO*. The systematic study marks the significance of precise tailoring of the synergistic relationship between oxygen vacancies and basic sites for achieving the desired performance in CO2 methanation.
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