Photoinduced Lattice Oxygen Spillover on Ru/BaTiO 3 for Efficient and Stable Photothermal Dry Reforming of Methane

Lattice oxygen (Ol)-mediated photothermal dry reforming of methane (DRM) offers a promising approach to converting two greenhouse gases (CH4 and CO2) into syngas. However, the intrinsic stability of metal–oxygen bonds often restricts the Ol mobility. Herein, we developed a Ru/BaTiO3 with a well-defined metal–support interface that enables a photoinduced lattice oxygen spillover effect for efficient and stable photothermal DRM. Under light irradiation, the photoexcited electrons transfer to Ruδ+ sites, greatly improving its electron density, while the photogenerated holes move to the lattice oxygen of BaTiO3, which weakens the Ba–O–Ti bonds for facilitating lattice oxygen migration. In situ characterizations and theoretical calculations confirm that this photoinduced lattice oxygen spillover effect promotes reactant activation and shifts the DRM pathway from the carbon-forming CH3* route as observed in thermal catalysis to a carbon-free CH3O* route, thereby effectively suppressing coke formation. As a result, the Ru/BaTiO3 catalyst exhibits excellent catalytic stability (>120 h) and superior catalytic activity (10.1/11.4 mol gRu–1 h–1 for H2/CO production) under simulated sunlight irradiation. This work motivates the design of efficient and stable DRM catalysts under mild conditions.