Efficient Single-Atom Fe-Catalyzed Fenton-like Reaction Involving Peroxymonosulfate for BPA Degradation by High-Valent Fe(IV)=O

Catalytic activation of peroxymonosulfate is one of the most promising advanced oxidation processes for water treatment. The development of advanced functional catalysts is essential to efficient and selective elimination of the emerging organic pollutants in water. Via a facile one-step method using the naturally abundant tannic acid and low-cost melamine as precursors, the atomically dispersed Fe was anchored on a nitrogen-doped carbon matrix, and the configuration of Fe-N4 was confirmed by synchrotron X-ray absorption spectroscopy. The single-atom Fe catalyst was efficient in catalytic degradation of various organic pollutants, e.g., removal of 100 μM BPA within 40 s under mild reaction conditions. The essential role of high-valent iron-oxo species in selective degradation of pollutants was identified by systematic mechanistic investigations. This work demonstrates the unique advantages of high-valent FeIV=O in selective elimination of emerging organic pollutants and sheds light on the design of an efficient and durable single-atom catalyst for a variety of applications.