Interlayer-limited single-atom sub-nanoreactor facilitates efficient H2O2 activation

Fenton reaction is an effective and widespread means of water purification, with the efficient generation of hydroxyl radicals (•OH) and harsh operating environments limiting their application to the total environment. The coordinated coordination environment of the active site is crucial for the Fenton catalytic process. This study reports the rational design and application of a domain-limited single-atom sub-nanoreactor (C-Fe-MoS₂). The results show that carbon intercalation improves the interlayer confinement microenvironment of MoS₂, and the dual coordination structure plays a key role in optimizing the electronic structure of the monoatomic iron sites, accelerating the H₂O₂ mass transfer adsorption and subsequent peroxy bond cleavage reactions. The acid modulation mechanism of MoS₂ breaks the pH limitation and thus exhibits highly efficient degradation of various organic pollutants over a wide range of pH. This study provides a molecular mechanism for the effect of the coordination environment on the catalytic performance of active-site Fenton catalysts, which may shed light on the understanding of H₂O₂ activation mechanisms and the rational design of efficient catalysts.