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<p>Over the past two decades, the integration of Fenton chemistry with metal–organic frameworks (MOFs) have revolutionized the landscape of advanced oxidation processes (AOPs) for wastewater treatment. The classical homogeneous Fenton reaction, while renowned for its powerful oxidative capacity, is constrained by a narrow pH range (typically 2.8–3.5), production of iron sludge, and difficulty in catalyst recovery. These limitations have driven the development of heterogeneous Fenton systems that immobilize Fe species on solid support, aiming to enhance catalyst stability and recyclability. Metal–organic frameworks (MOFs) have emerged as tunable platforms for Fenton and Fenton-like catalysis, offering modular control over redox behavior, light absorption, and active site accessibility. Their highly ordered architecture enables spatial confinement of Fe, Cu, or Co nodes within organic linkers that mediate charge separation and radical transfer. This review critically examines the structure–function–pathway nexus of MOF-driven Fenton systems from framework composition and defect engineering to the generation of reactive oxygen species (ROS) under solar and visible irradiation. The discussion integrates recent advances in ligand functionalization, hetero-metal doping, and hybridization with carbonaceous or semiconductor supports to enhance stability and recyclability under near-neutral pH. Mechanistic pathways are mapped across homogeneous, heterogeneous, and interface-confined regimes, highlighting electron-transfer kinetics, Fe²⁺/Fe³⁺ regeneration, and ROS selectivity. Comparative kinetic benchmarks and thermodynamic correlations are provided to guide catalyst rationalization and scale-up. This review goes beyond conventional performance summaries by correlating MOF structural design parameters with radical generation mechanisms, establishing a unified framework linking crystal chemistry, band energetics, and catalytic dynamics. It formulates design rules and reaction descriptors that bridge molecular architecture to applied water treatment performance, thereby defining the roadmap for next-generation, stable, and recyclable photo-Fenton catalysts.</p> Graphical Abstract <p></p>

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From Framework to Radical Pathways: A Critical Review on MOF-Driven Fenton and Fenton-Like Catalysis

  • 期刊论文

  • 发表日期：

    2026年3月9日

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  • Shehab A. Mansour,
  • Abdullah Alshehab,
  • Mai K. Fouad,
  • Maha A. Tony

摘要

Over the past two decades, the integration of Fenton chemistry with metal–organic frameworks (MOFs) have revolutionized the landscape of advanced oxidation processes (AOPs) for wastewater treatment. The classical homogeneous Fenton reaction, while renowned for its powerful oxidative capacity, is constrained by a narrow pH range (typically 2.8–3.5), production of iron sludge, and difficulty in catalyst recovery. These limitations have driven the development of heterogeneous Fenton systems that immobilize Fe species on solid support, aiming to enhance catalyst stability and recyclability. Metal–organic frameworks (MOFs) have emerged as tunable platforms for Fenton and Fenton-like catalysis, offering modular control over redox behavior, light absorption, and active site accessibility. Their highly ordered architecture enables spatial confinement of Fe, Cu, or Co nodes within organic linkers that mediate charge separation and radical transfer. This review critically examines the structure–function–pathway nexus of MOF-driven Fenton systems from framework composition and defect engineering to the generation of reactive oxygen species (ROS) under solar and visible irradiation. The discussion integrates recent advances in ligand functionalization, hetero-metal doping, and hybridization with carbonaceous or semiconductor supports to enhance stability and recyclability under near-neutral pH. Mechanistic pathways are mapped across homogeneous, heterogeneous, and interface-confined regimes, highlighting electron-transfer kinetics, Fe²⁺/Fe³⁺ regeneration, and ROS selectivity. Comparative kinetic benchmarks and thermodynamic correlations are provided to guide catalyst rationalization and scale-up. This review goes beyond conventional performance summaries by correlating MOF structural design parameters with radical generation mechanisms, establishing a unified framework linking crystal chemistry, band energetics, and catalytic dynamics. It formulates design rules and reaction descriptors that bridge molecular architecture to applied water treatment performance, thereby defining the roadmap for next-generation, stable, and recyclable photo-Fenton catalysts.

Graphical Abstract