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

Suppressive strong metal–support interactions (SMSI) enable hot electrons excited on Ru to transfer to a TiO2−H2 support, thereby reducing the electron density on Ru to accelerate light-driven CO2 reduction with methane. The optimized Ru/TiO2−H2 composite exhibits an enhanced CO2 conversion rate of 400 mmol gcat −1 h−1.


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.

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