Oxygen vacancies in Ru/TiO2 - drivers of low-temperature CO2 methanation assessed by multimodal operando spectroscopy

[摘要] Summary: Hydrogenation of CO2 is very attractive for transforming this greenhouse gas into valuable high energy density compounds. In this work, we developed a highly active and stable Ru/TiO2 catalyst for CO2 methanation prepared by a solgel method that revealed much higher activity in methanation of CO2 (ca. 4–14 times higher turnover frequencies at 140–210°C) than state-of-the-art Ru/TiO2 catalysts and a control sample prepared by wetness impregnation. This is attributed to a high concentration of O-vacancies, inherent to the solgel methodology, which play a dual role for 1) activation of CO2 and 2) transfer of electrons to interfacial Ru sites as evident from operando DRIFTS and in situ EPR investigations. These results suggest that charge transfer from O-vacancies to interfacial Ru sites and subsequent electron donation from filled metal d-orbitals to antibonding orbitals of adsorbed CO are decisive factors in boosting the CO2 methanation activity.

[关键词] Chemistry;Inorganic chemistry;Catalysis