Constructing matched active sites for robust photocatalytic dry reforming of methane

Photocatalytic dry reforming of methane (DRM) is a promising green process for converting two greenhouse gases into syngas. Nonetheless, achieving photocatalytic DRM with both high activity and stoichiometric products ratio remains a grand challenge. We report here a Ru single-atom-modified hierarchical porous TiO2-SiO2 (Ru-TS) as a photocatalyst for DRM, achieving a remarkable syngas generation rate of 98.52 mmol gRu−1 h−1 for CO and 96.50 mmol gRu−1 h−1 for H2 with extraordinary durability under mild conditions. The local microstructure of Ru-Ov-Ti on catalyst provides matched active sites for CH4 and CO2 adsorption and activation through charge redistribution and electronic localization and optimizes CH4-CO2 reaction route for inhibiting side reaction and promoting effective C–O coupling. This work provides guidance in the active site construction of robust catalysts for photocatalytic DRM and other multi-molecule synergetic reactions.