Heterogeneous activation of peroxydisulfate by sulfur-doped g-C3N4 under visible-light irradiation: Implications for the degradation of spiramycin and an assessment of N-nitrosodimethylamine formation potential

Highlights: • PDS/SCN catalytic system was used for spiramycin degradation for the first time. • SCN has good stability and excellent reuse photocatalytic activity. • Spiramycin removal mechanism was investigated and degradation pathway was proposed. • NDMA FP was significantly reduced after PDS/SCN catalytic photolysis of spiramycin. In this study, peroxydisulfate (PDS) was activated by synthesized sulfur-doped g-C₃N₄ (SCN) under visible-light irradiation and was adopted to enhance the removal of spiramycin, which is an important precursor of N-nitrosodimethylamine (NDMA). Specifically, 95.4% of spiramycin (≤10 mg/L) was removed in 60 min under the conditions of an initial value of pH of 7.0, an SCN dose of 1.0 g/L, and a PDS dose of 200 mg/L, and its degradation fitted well with the pseudo first-order kinetics. Electron paramagnetic resonance analysis and trapping experiments confirmed that ·O₂⁻ and h⁺ were the main oxidizers for the degradation of spiramycin, and ·SO₄⁻ and ·OH also participated in the removal of spiramycin. The removal of spiramycin in the PDS/SCN visible-light catalytic system occurred through three different pathways: aldehyde oxidation, cleavage of C-O bond and demethylation. Notably, 61.4% of NDMA formation potential (FP) was reduced after the reaction. The SCN catalyst was stable and its catalytic performance was excellent in the PDS/SCN system, as the spiramycin removal efficiency decreased only slightly from 95.4% to 87.3% after being reused three times. Therefore, our study not only provides an alternative method for removing spiramycin but can also can significantly reduce NDMA FP.