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

作者：Delong Duan, Cenfeng Fu, Xiaomin Ji, Zehui Dai, Aobo Chen, Canyu Hu, M-Y Ge, Hailong Xiong, Min Zhou, Ran Long, Yujie Xiong · 发表于：Journal of the American Chemical Society · 年份：2025 · DOI：10.1021/jacs.5c17614 · 被引用次数：15 · 研究领域：Catalysts for Methane Reforming、Advanced Photocatalysis Techniques、CO2 Reduction Techniques and Catalysts

Lattice oxygen (O l )-mediated photothermal dry reforming of methane (DRM) offers a promising approach to converting two greenhouse gases (CH 4 and CO 2 ) into syngas. However, the intrinsic stability of metal–oxygen bonds often restricts the O l mobility. Herein, we developed a Ru/BaTiO 3 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 Ru δ + sites, greatly improving its electron density, while the photogenerated holes move to the lattice oxygen of BaTiO 3, 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 CH 3 * route as observed in thermal catalysis to a carbon-free CH 3 O* route, thereby effectively suppressing coke formation. As a result, the Ru/BaTiO 3 catalyst exhibits excellent catalytic stability (>120 h) and superior catalytic activity (10.1/11.4 mol g Ru –1 h –1 for H 2 /CO production) under simulated sunlight irradiation. This work motivates the design of efficient and stable DRM catalysts under mild conditions.