Dual‐Path Singlet Oxygen Generation by Sulfur Vacancy Tailored Atomic Iron Assembly for Sustainable Decontamination

Abstract

Abstract Singlet oxygen ( 1 O 2 ) generation via single‐atom catalysis remains challenging in achieving both high efficiency and yield. Herein, S vacancies on MoS 2 are rationally engineered via a topochemical oxidation strategy, achieving Fe assembly from nanoparticles to nanoclusters and single atoms. Atomic Fe sites situated atop of Mo and isolated S vacancies primarily facilitated the SO 5 •− and O 2 •− pathways, respectively. This dual‐path generation of 1 O 2 achieved a high yield (0.36 m m ) with exceptional peroxymonosulfate utilization (73%). Isolated S vacancies allowed universal fabrication of high‐loading SA with stable M−S 3 coordination (M = Mn, Fe, Co, Ni, and Cu). This unique platform further elucidated modulation of dual‐path 1 O 2 generation by the inherent electronic structure of metals, depending on the 3 d orbital unoccupancy, d ‐band center spin, and magnetic moment of metallic SA. The optimized catalyst (Fe SA ‐MoS V2 ) demonstrated exceptional performance toward a broad spectrum of contaminant types and wastewater matrices, along with scalable treatment capacity (30 L) and long‐term operation (40 days, equivalent to 960 batch cycles). This study unveils a trade‐off relationship between the topological defective vacancy in structuring metal sites, catalytic activity, and long‐term stability in Fenton‐like catalysis, offering an innovative material design strategy for sustainable wastewater treatment.

Affiliated Institutions

• Zhejiang University CN

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