Regulating electron distribution of Fe/Ni-N₄P₂ single sites for efficient photo-Fenton process

Regulating local electron density by introducing single-atom is an effective strategy to improve the activity of heterogeneous photo-Fenton processes. Here N, P coordinated Fe and Ni single-atom catalysts on carbon nitrides (CN-FeNi-P) were prepared to activate H₂O₂ for contaminant mineralization under visible light irradiation. The as-prepared CN-FeNi-P presented a higher moxifloxacin degradation activity in photo-Fenton system, which was up to 3.7 times that of pristine CN, meanwhile, its TOC removal reached to 95.9 % in 60 min. Based on density functional theory calculations, the Ni single-atoms serve as the optimal reactive sites to produce •OH. The strong interaction between Fe and Ni single-atoms by P-bridging and the modulated local electron structure after introducing P into coordination environment can lower •OH formation energy. This study provides new doping strategies to design single-atom catalysts and expands the family of the Fenton-like system for advanced oxidation technologies.