Recently, the research team led by Prof. J. Paul Chen at the College of Chemistry and Environmental Engineering, Shenzhen University, published a review titled “Metal–Organic Frameworks-Driven Atomic Precision in Advanced Oxidation for Pollution Control” in Advanced Materials (impact factor 26.8; CAS JCR Q1, TOP journal). Assistant Professor Wei Qu is the sole first author, and Prof. J. Paul Chen is the sole corresponding author. Shenzhen University is the first corresponding affiliation.

Persistent organic pollutants (POPs) and emerging contaminants pose escalating challenges to global sustainability. Owing to their high thermodynamic stability and strongly electron-withdrawing functional groups, these contaminants often resist conventional biological and physicochemical treatments, while their toxicity, persistence, and bioaccumulation amplify long-term ecological risks. In traditional treatment systems, the combination of continuous discharge and incomplete removal underscores the urgent need for more efficient and reliable remediation strategies. Advanced oxidation processes (AOPs), which generate reactive oxygen species in situ, can achieve both selective and nonselective oxidation of recalcitrant pollutants and thus hold great promise. However, practical deployment remains constrained by intrinsic limitations of conventional heterogeneous catalysts, including suboptimal atomic utilization, limited accessibility of active sites, sluggish electron-transfer kinetics, and vulnerability to oxidative deactivation under harsh conditions—factors that collectively restrict catalytic lifetime, scalability, and cost-effectiveness. These bottlenecks are driving a paradigm shift in environmental catalysis toward atomic-scale engineering, where precision exposure and regulation of active sites, tailored electronic structures, and robust interfacial architectures are pivotal to overall efficiency and stability. In this context, atomically dispersed catalysts—particularly those derived from metal–organic frameworks (MOFs)—offer a transformative pathway to next-generation oxidation catalysts with high atom economy, structural robustness, and multifunctionality.

This review provides a systematic overview of recent advances enabling atomic-precision catalysis for AOPs using MOFs as programmable platforms. Centered on three technical thrusts—(i) constructing unsaturated metal sites, (ii) precisely tuning functional organic linkers, and (iii) coupling hierarchical confinement with mass-transport regulation—it elucidates structure–electron–activity relationships for single- and dual-atom sites across radical and nonradical pathways, and proposes a unified framework linking materials design to engineering practice along with key research challenges. The article further integrates density functional theory and molecular dynamics to clarify active-site electronic structures, adsorption/activation barriers, and confined transport mechanisms, thereby informing pathway identification and rate-determining steps. By introducing machine learning and high-throughput strategies—using coordination fingerprints such as M–N₄—the review demonstrates data-driven catalyst screening and inverse design that markedly reduce experimental trial-and-error. To advance engineering translation, it advocates incorporating life-cycle assessment (LCA) and techno-economic analysis (TEA) early in materials development, using quantitative metrics (environmental burden, energy consumption, and cost) to guide scale-up and application scenario selection, and it emphasizes that enhancing redox stability, anti-deactivation capability, scalable manufacturing, and environmental adaptability is critical for the next generation of water-treatment technologies.

Looking ahead, MOF-derived atomic catalysts must move beyond “proof-of-concept” toward deployment by closing the loop from mechanism and design to manufacturing, evaluation, and application. This entails accelerating identification of optimal metal–ligand architectures via machine learning and high-throughput computation; capturing transient active states, charge redistribution, and electron-transfer pathways at atomic resolution through in situ/operando characterization; and establishing dynamic structure–activity relationships that account for coordination fluctuations and reaction microenvironments to jointly optimize activity and durability. In parallel, green synthesis using renewable precursors, combined with rigorous LCA/TEA benchmarks, should serve as gatekeepers for scale-up. Leveraging MOFs as programmable platforms will enable multifunctional catalytic systems that integrate pollutant degradation with membrane separation, energy conversion, and pathogen inactivation, ultimately achieving robust, durable, and sustainable field deployment through long-term stability, environmental robustness, manufacturing consistency, and standardized testing.

This work was supported by the National Natural Science Foundation of China, the High-Level Talent Research Start-up Fund of Shenzhen University, and the Youth Research Fund of Shenzhen University.

Original article: https://doi.org/10.1002/adma.202512877