Planar hexanuclear uranium cluster enables efficient photocatalytic hydrogen peroxide production via dual hydrogen abstraction-oxygen reduction pathways

Solar-driven hydrogen peroxide (H 2 O 2 ) production is a highly promising approach for addressing environmental and energy challenges. The photocatalytic H 2 O 2 production efficiency is predominantly governed by visible light harvesting efficiency, surface active site accessibility, and charge-migration efficiency. In this study, a distinct planar hexanuclear uranyl cluster is formed through chelating and bridging benzoate ligands and terminally coordinated water molecules. Its distinctive structural features offer new possibilities for addressing the challenges of rapid carrier recombination and insufficient active sites in photocatalysis. The ordered periodic arrangement of uranyl units enhances carrier migration and charge utilization, facilitating the two-step single-electron oxygen reduction to generate H 2 O 2 . Meanwhile, the planar molecular configuration promotes the efficient desorption of products from the metal centers, thereby reducing H 2 O 2 decomposition. In addition, the discrete structure of U 6 -BA increases the exposure of the uranyl-oxo active sites, enabling more comprehensive substrate binding and promoting H 2 O 2 production through strong oxidation and hydrogen abstraction. As a result, U 6 -BA exhibits significantly improved photocatalytic performance, achieving an H 2 O 2 production rate of 2160 μmol h −1  g −1 . This study proposes an effective strategy for optimizing photocatalytic H 2 O 2 production using uranyl cluster, offering new insights into the design and application of photocatalytic materials.