Affiliation: | 1. Xiamen Key Laboratory of Materials for Gaseous Pollutant Control, Institute of Urban Environment, Chinese Academy of Sciences, 361021 Xiamen, China CAS Center for Excellence in Regional Atmospheric Environment, Key Laboratory of Urban Pollutant Conversion, Institute of Urban Environment, Chinese Academy of Sciences, 361021 Xiamen, China University of Chinese Academy of Sciences, 100049 Beijing, China;2. Fujian Institute of Research on The Structure of Matter, Chinese Academy of Sciences, 350002 Fuzhou, China Xiamen Institute of Rare-earth Materials, Haixi Institutes, Chinese Academy of Sciences, 361021 Xiamen, China University of Chinese Academy of Sciences, 100049 Beijing, China;3. Xiamen Key Laboratory of Materials for Gaseous Pollutant Control, Institute of Urban Environment, Chinese Academy of Sciences, 361021 Xiamen, China |
Abstract: | Strong metal-support interactions (SMSI) have gained great attention in the heterogeneous catalysis field, but its negative role in regulating light-induced electron transfer is rarely explored. Herein, we describe how SMSI significantly restrains the activity of Ru/TiO2 in light-driven CO2 reduction by CH4 due to the photo-induced transfer of electrons from TiO2 to Ru. In contrast, on suppression of SMSI Ru/TiO2−H2 achieves a 46-fold CO2 conversion rate compared to Ru/TiO2. For Ru/TiO2−H2, a considerable number of photo-excited hot electrons from Ru nanoparticles (NPs) migrate to oxygen vacancies (OVs) and facilitate CO2 activation under illumination, simultaneously rendering Ruδ+ electron deficient and better able to accelerate CH4 decomposition. Consequently, photothermal catalysis over Ru/TiO2−H2 lowers the activation energy and overcomes the limitations of a purely thermal system. This work offers a novel strategy for designing efficient photothermal catalysts by regulating two-phase interactions. |