Journal
NANO RESEARCH
Volume -, Issue -, Pages -Publisher
TSINGHUA UNIV PRESS
DOI: 10.1007/s12274-023-5592-3
Keywords
Ru-based catalysts; oxygen vacancies; basic sites; CO2 methanation; mechanism study
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In this study, it was found that the Ru/CeO2 catalyst exhibited high CO2 conversion (86%) and CH4 selectivity (100%) with excellent stability of 30 hours, due to the presence of abundant oxygen vacancies and weak basic sites. The in-situ DRIFTS and DFT calculations revealed that b-HCOO* was the key intermediate in the hydrogenation route on the Ru/CeO2 catalyst, being more easily hydrogenated to methane than m-HCOO*. This systematic study highlights the importance of precise tailoring of the synergistic relationship between oxygen vacancies and basic sites for achieving desired performance in CO2 methanation.
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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