Pore modulation of single atomic Fe sites for ultrafast Fenton-like chemistry with amplified electron migration oxidation.

ABSTRACT

The limited interaction between pollutants, oxidants, and the surface catalytic sites of single atom catalysts (SACs) restricts the water decontamination effectiveness. Confining catalytic sites within porous structures enables the localized enrichment of reactants for optimized reaction kinetics, while the specific regulatory mechanisms remain unclear. Herein, SACs with porous modification significantly improves the utilization of peroxymonosulfate (PMS) and pollutant degradation activity. Confining catalytic sites in porous structure effectively reduces the mass transfer distance between radicals (SO4•- and •OH) and pollutants, thereby improving reaction performance. Pore modulation changes the surface electronic structure, leading to a significant improvement in the electron migration process. The system shows significant potential in effectively oxidizing various common emerging pollutants, and exhibits robust resistance to interference from environmental matrices. Moreover, a quantitative evaluation using life cycle assessment (LCA) indicates that the pFe-SAC/PMS system showcases superior environmental importance and practicality.