Precision Engineering of Single‐Atom Catalysts to Enhance the Peroxymonosulfate Activation in Fenton‐Like Reactions

ABSTRACT The Fenton reaction represents an effective advanced oxidation processes (AOPs) for degrading organic pollutants. However, the conventional homogeneous Fenton reaction suffers from several limitations, including the narrow pH range, iron sludge generation, and low H ₂ O ₂ utilization efficiency. To overcome these bottlenecks, the heterogeneous Fenton‐like reaction has emerged. Recently, single‐atom catalysts (SACs) have been widely used in Fenton‐like reactions due to their high atomic utilization rate and abundant active sites, showing great application prospects. Therefore, a systematic review of single‐atom catalysts is critical for advancing Fenton‐like systems. This review first explores the mechanisms underlying the activation of peroxymonosulfate (PMS) by SACs. It then systematically categorizes the structure–activity relationships of SACs, including coordination environment engineering, reaction pathway regulation, spatially confined architectures, and multi‐metal synergistic systems. Finally, the review critically examines the current challenges and future application prospects of SACs in Fenton‐like catalysis, with emphasis placed on the imperative integration of mechanistic insights and rational design for to achieve sustainable and high‐efficiency performance.