Regulating Atomically‐Precise Pt Sites for Boosting Light‐Driven Dry Reforming of Methane

Abstract Light‐driven dry reforming of methane is a promising and mild route to convert two greenhouse gas into valuable syngas. However, developing facile strategy to atomically‐precise regulate the active sites and realize balanced and stable syngas production is still challenging. Herein, we developed a spatial confinement approach to precisely control over platinum species on TiO 2 surfaces, from single atoms to nanoclusters. The configuration comprising single atoms and sub‐nanoclusters engenders pronounced electronic metal‐support interactions, with resultant interfacial states prompting surface charge rearrangement. The unique geometric and electronic properties of these atom‐cluster assemblies facilitate effective activation of CH 4 and CO 2 , accelerating intermediate coupling and minimizing side reactions. Our catalyst exhibits an outstanding syngas generation rate of 34.41 mol g Pt −1 h −1 with superior durability, displaying high apparent quantum yield of 9.1 % at 365 nm and turnover frequency of 1289 h −1 . This work provides insightful understanding for exploring more multi‐molecule systems at an atomic scale.