This research demonstrates how asymmetric vacancies enhance ROS evolution in photocatalytic methane conversion, suggesting new pathways for efficient chemical transformations.
Photocatalytic oxidation mediated by reactive oxygen species (ROS) provides an effective platform for a wide range of important chemical transformations. However, conventional oxygen-vacancy engineering strategy, while enhancing O₂ activation, often hampers subsequent ROS evolution due to overly strong adsorption, thereby limiting oxidation kinetics. Here, we demonstrate that asymmetric vacancies in ZnGa₂O₄, characterized by a ZnTd-Ov-GaOh configuration, can overcome this intrinsic limitation by synergistically coupling O₂ activation with efficient ROS evolution. Specifically, the dynamic GaOh site preferentially promotes O₂ adsorption and activation, whereas the ZnTd site interacts weakly with oxygen-derived species, facilitating ROS release and vacancy replenishment, thereby achieving an optimal balance between these critical steps. Consequently, Ag/ZnGa₂O₄ delivers the highest turnover number (TON) reported to date among Ag-based catalysts for the photocatalytic oxidative coupling of methane via a ROS-mediated pathway. The general effectiveness of this asymmetric-vacancy strategy is further validated in other representative photocatalytic reactions, including hydrogen peroxide production and the oxidative coupling of benzyl alcohol.
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Zhang et al. (2026) studied this question.
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