Suppressive Strong Metal‐Support Interactions on Ruthenium/TiO2 Promote Light‐Driven Photothermal CO2 Reduction with Methane. Issue 19 (29th March 2023)

• Record Type: Journal Article
• Authors: Li, Qiang; Wang, Huiling; Zhang, Meng; Li, Guanghui; Chen, Jing; Jia, Hongpeng
• Is Part Of: Angewandte Chemie international edition. Volume 62:Issue 19(2023)
• Page Start: n/a
• Page End: n/a
• Publication Date: 2023-03-29
• Subjects: CO2 Reduction -- Electronic Transfer Modulations -- Photothermal Catalysis -- Suppressed Strong Metal-Support Interactions; Chemistry -- Periodicals; 540
• DOI: 10.1002/anie.202300129
• Languages: English
• ISSNs: 1433-7851

Abstract

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 Ru δ+ 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. Abstract : 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 and accelerating 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 .