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Abstract High-entropy alloy nanoparticles (HEA-NPs) exhibit favorable properties in catalytic processes, as their multi-metallic sites ensure both high intrinsic activity and atomic efficiency. However, controlled synthesis of uniform multi-metallic ensembles at the atomic level remains challenging. This study successfully loads HEA-NPs onto a nitrogen-doped carbon carrier (HEAs) and pioneers the application in peroxymonosulfate (PMS) activation to drive Fenton-like oxidation. The HEAs-PMS system achieves ultrafast pollutant removal across a wide pH range with strong resistance to real-world water interferences. Furthermore, the nonradical HEAs-PMS system selectively transforms phenolics into high-molecular-weight products via a polymerization pathway. The unique non-mineralization regime remarkably reduces PMS consumption and achieves a high electron utilization efficiency of up to 213.4%. Further DFT calculations and experimental analysis reveal that Fe and Co in HEA-NPs act as the primary catalytic sites to complex with PMS for activation, while Ni, Cu, and Pd serve as charge mediators to facilitate electron transfer. The resulting PMS* complexes on HEAs possess a high redox potential, which drives spatially separated phenol oxidation on nitrogen-doped graphene support to form phenoxyl radicals, subsequently triggering the formation of high-molecule polymeric products via polymerization reactions. This study offers engineered HEAs catalysts for water treatment with low oxidant consumption and emissions.

Abstract Microplastic pollution, an emerging environmental issue, poses significant threats to aquatic ecosystems and human health. In tackling microplastic pollution and advancing green hydrogen production, this study reveals a tandem catalytic microplastic degradation-hydrogen evolution reaction (MPD-HER) process using hierarchical porous carbon nitride-supported single-atom iron catalysts (FeSA-hCN). Through hydrothermal-assisted Fenton-like reactions, we accomplish near-total ultrahigh-molecular-weight-polyethylene degradation into C3-C20 organics with 64% selectivity of carboxylic acid under neutral pH, a leap beyond current capabilities in efficiency, selectivity, eco-friendliness, and stability over six cycles. The system demonstrates versatility by degrading various daily-use plastics across different aquatic settings. The mixture of FeSA-hCN and plastic degradation products further achieves a hydrogen evolution of 42 μmol h‒1 under illumination, outperforming most existing plastic photoreforming methods. This tandem MPD-HER process not only provides a scalable and economically feasible strategy to combat plastic pollution but also contributes to the hydrogen economy, with far-reaching implications for global sustainability initiatives.