Broad-spectrum degradation of emerging contaminants and industrial dyes by a robust CuCo_(1:2)@N catalyst activating...

To broaden the application scope of peroxymonosulfate advanced oxidation processes (PMS-AOPs) in water purification, we developed a catalyst rich in oxygen vacancies (O_Vs) (CuCo_(1:2)@N) for activating peroxymonosulfate (PMS) to purify water. Research indicates that at an ultra-low dosage (0.01 g/L catalyst, 0.5 mM PMS), the system achieves >99 % degradation of tetracycline (20 mg/L) within 20 min. It exhibits broad-spectrum efficacy, removing various antibiotics (e.g., 90 % removal of 30 mg/L levofloxacin) and synthetic dyes (>99 % removal). Quenching experiments, electron paramagnetic resonance (EPR) analysis, and probe experiments collectively indicate that the reaction proceeds via a synergistic combination of radical pathways (SO₄^・-, ・OH, O₂^・-) and non-radical pathways (¹O₂). Notably, density functional theory (DFT) calculations reveal that nitrogen-induced O_Vs serve as primary active sites, favoring PMS adsorption (ΔE = 1.692 eV) and thereby promoting organic degradation. Furthermore, using tetracycline (TC) as a model contaminant, the attack sites on CuCo_(1:2)@N were investigated, and a degradation pathway for TC was proposed. This study introduces O_Vs to synergize with metal redox cycles, offering a novel strategy for optimizing heterogeneous Fenton-like catalytic oxidation to achieve water purification.