Nanoconfined Cu─O─Mo Asymmetric Sites Enable Ambient Spontaneous O <sub>2</sub> ‐to‐ <sup>1</sup> O <sub>2</sub> Conversion for Sustainable Water Purification
Jian Ye, Chenxiao Yu, Jiangdong Dai, Lili Li, Ruilong Zhang, Jianming Pan, Wenhua Xue, Yuehan Jiang, Jun Zhao
Abstract
Abstract The selective activation of molecular oxygen (O 2 ) to singlet oxygen ( 1 O 2 ) represents a sustainable route for green oxidation yet remains fundamentally challenged by spin‐forbidden transitions and kinetic trapping of superoxide intermediates. Here, an asymmetric Cu + ─O─Mo 6+ dual‐site embedded within a nanoconfined membrane is constructed that drives spontaneous O 2 ‐to‐ 1 O 2 conversion under ambient conditions, achieving 95.2% selectivity without additional energy inputs. Experimental and theoretical analyses reveal that electron‐rich Cu + sites facilitate spin‐selective electron transfer to adsorbed O 2 while adjacent Mo 6+ sites stabilize Cu + species and facilitate the direct formation of 1 O 2 , bypassing the conventional superoxide desorption bottleneck. The nanoconfined environment further concentrates local reactants, yielding a 0.053 ms −1 degradation rate constant, exceeding most Fenton‐like systems. The system maintains operational stability for 146 h in continuous‐flow filtration with ultralow metal leaching (<0.02 mg L −1 ) and operational cost (0.01 USD L −1 ), enabling over 95% removal of diverse micropollutants in complex water matrices. This work establishes a new catalytic paradigm merging atomic‐scale asymmetric site design with nanoconfinement engineering for sustainable and selective O 2 activation, providing an efficient and environmentally benign strategy for advanced water purification.