Universal pseudo-fluctuation engineering induces local free radical surface confinement effect to enhance photocatalytic oxidation of toluene

作者：Yuhui Liu, Zhe Wang, Peng Chen, Lang Chen, Shuang‐Feng Yin · 发表于：Applied Catalysis B: Environmental · 年份：2025 · DOI：10.1016/j.apcatb.2025.125806 · 被引用次数：3 · 研究领域：Catalysis and Oxidation Reactions、Advanced Chemical Physics Studies、Catalytic Processes in Materials Science

Breaking the trade-off between activity and selectivity has always been a long-standing challenge in the field of catalysis. In this study, we introduce an innovative universal pseudo-fluctuation strategy utilizing surface-uncoordinated In(OH) 3-x -ZnIn 2 S 4 heterojunctions (ZIO) to achieve local free radical confinement. Notably, the low-coordination and contraction of In−O bonds generate disordered and loosely hydrogen-bonded chains, which enhances the adsorption and activation of toluene. Meanwhile, the dynamic transformation of In−O bonds regulates the d‐band center while restructuring a dense hydrogen bonding network. This process locally confines highly reactive oxygen species and facilitates the desorption of benzaldehyde, effectively inhibiting the over-oxidation of the product. Ultimately, after 48 h of irradiation, the photocatalytic toluene oxidation rate of ZIO-2 reached 100.59 mmol g −1 without generating excessive oxidation by-products. Our work delineates a clear surface reaction pathway and introduces a novel design paradigm for atomic-scale photocatalysis in multi-state interfaces, paving the way for advanced catalysts that harness interfacial microenvironments to achieve enhanced performance. • A water-mediated free radical surface confinement strategy to enhance photocatalytic toluene oxidation. • The low-coordination structure modulates the d‐band center of ZIO-2. • The dynamic transformation of In−O bonds reorganizing the chain hydrogen bonding into a hy...