Sustainable Water Decontamination: Advanced High-Valent Iron Active Species-Driven Peroxymonosulfate Activation for Global Challenges

Abstract

High-valent iron active species (HVIAS)-driven peroxymonosulfate (PMS) activation has emerged as a transformative approach in environmental remediation. This review systematically deciphers the mechanistic evolution and characterization advances of HVIAS generation: non-radical-dominated electron transfer pathways have been rigorously elucidated through in situ X-ray absorption spectroscopy (XAS) and Mössbauer spectroscopy. In contaminant elimination, the HVIAS-PMS system achieves 1-2 orders of magnitude higher degradation kinetics than conventional radical-based routes via targeted oxidation of electron-rich moieties in antibiotics. To address real-world wastewater complexity, 3D-structured and 3D-printed catalytic materials enhance HVIAS generation efficiency and stability through confinement effects and mass transport optimization. Nevertheless, critical challenges—including C-F bond cleavage in PFAS, co-existing matrix interference, and byproduct toxicity—demand urgent re-evaluation for practical implementation. Future endeavors should prioritize smart-responsive catalyst design, multi-omics-driven toxicity profiling, global byproduct database establishment, and cross-scale integration of HVIAS-PMS with renewable energy technologies. This perspective presents cutting-edge advancements in HVIAS-PMS systems, provides a multidimensional framework bridging fundamental research and applications for sustainable water decontamination, and discusses the limitations as well as prospects.