Suppressive Strong Metal‐Support Interactions on Ruthenium/TiO2 Promote Light‐Driven Photothermal CO2 Reduction with Methane

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/TiO 2 in light‐driven CO 2 reduction by CH 4 due to the photo‐induced transfer of electrons from TiO 2 to Ru. In contrast, on suppression of SMSI Ru/TiO 2 −H 2 achieves a 46‐fold CO 2 conversion rate compared to Ru/TiO 2 . For Ru/TiO 2 −H 2 , a considerable number of photo‐excited hot electrons from Ru nanoparticles (NPs) migrate to oxygen vacancies (OVs) and facilitate CO 2 activation under illumination, simultaneously rendering Ru δ+ electron deficient and better able to accelerate CH 4 decomposition. Consequently, photothermal catalysis over Ru/TiO 2 −H 2 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.