Unraveling the Single-Atom Fe–N4 Catalytic Site Selectivity Generate Singlet Oxygen Via Activation of Persulfate: Polarizing Electric Fields Changes the Electron Transfer Pathway

Single-atom catalysts have been proved to be an effective material for the removal of organic pollutants from water and wastewater, and yet, the relationship between their internal structures and their roles still remains elusive. In this work, a catalyst Fe (MIL)-SAC with single-atom Fe-N4 active site was prepared. Fe (MIL)-SAC/Peroxydisulfate (PDS) system was able to achieve complete degrade of the Sulfamethoxazole (SMX) with kobs at 0.466 min-1, which was faster than the Fenton system under the same conditions (kobs = 0.422 min-1) and 16 times faster than Fe (MIL) (kobs = 0.029 min-1). Density functional calculations reveal that the Fe-N4 structure will affect the electron transport path and lead to selective generation of 1O2 by triggering S-O breakage and O-O polarization in PDS. Furthermore, Fe (MIL)-SAC/PDS system exhibits strong resistance to common influencing factors and has good application prospects. This work provides a new approach for the selectively generation of 1O2 for the efficient treatment of organic pollutants in aqueous environment.