Carbon-based peroxymonosulfate (PMS)-based Fenton-like reaction emerges as a promising technology for the organic micro-pollutants elimination. However, the organic micro-pollutants degradation via traditional radical dominated pathway is severely limited by the side reactions between radicals and water quality matrix, such as coexisting inorganic ions and natural organic matter (NOM). To this end, a catalyst, protonation Fe-O co-doped carbon nitride (PFeOCN), was successfully synthesized to activate peroxymonosulfate toward nonradical oxidation for organics such as bisphenol A (BPA). In comparison with the intrinsic carbon nitride (CN), PFeOCN showed a 1950-folds enhancement in BPA degradation rate constant. The degradation rate of BPA in PFeOCN/PMS system was not obviously inhibited in the present of coexisting inorganic ions and NOM (<b>Figure 1)</b>. The quenching tests, chronopotentiometry and electron paramagnetic resonance (EPR) suggest that an improved reactivity of PFeOCN was attributed to the reinforced electron-transfer regime without generation of free radicals. First, protonation would change the electronic structure of catalyst and induce positive charge into the material surfaces, which enhance the adsorption ability of PFeOCN for PMS or BPA because of electrostatic repulsion. Then the PFeOCN−PMS* complex was formed and selectively abstracted electrons from the co-adsorbed BPA to initiate the oxidation. Excellent reusability with a wide pH range and negligible effect of water quality matrix confirmed the practical application prospects of the PFeOCN/PMS system. This study would provide a new way for effective PMS activation by heterogeneous catalysts to efficiently degrade organic micro-pollutants in actual wastewater system via electron transfer.

Protonation carbon nitride-based materials improved catalytic activity in Fenton-like reaction: Electron transfer mechanism

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