N, S co-doped magnetic mesoporous carbon nanosheets for activating peroxymonosulfate to rapidly degrade tetracycline: Synergistic effect and mechanism

Abstract

Heteroatoms doped carbon materials are widely used in the advanced oxidation process (AOPs) to remove organic pollutants in water due to the synergies effect between different heteroatoms. In this study, a novel kind of N, S co-doped magnetic mesoporous carbon nanosheets (Fe@NS-C) was prepared by simple one-step pyrolysis. Further, the influence of doping amount of S (L-methionine) and N (melamine) on catalytic activity was studied, the optimized sample Fe@NS-C-2-12/PMS showed a satisfying degradation ( 91.07%) for high concentrations of tetracycline (80 mg/L TC) in 10 min, which was attributed to the proper ratio of S content to N content (S(at.%)/ N(at.%)= 0.2097) in the sample could better play its synergistic effect by XPS analysis. The Fe@NS-C-2-12/ PMS system also exhibited satisfactory degradation effects in a wide pH range (3-10) and the existence of inorganic ions and humic acid. Then, the degradation mechanisms were mainly through the non-radical pathway (¹O₂ and electron transfer) and the major active sites were pyridinic N compared to thiophene S, CO, and Fe-N_x. This study could inspire the design of high-performance active and low-cost heteroatomic doping nano-magnetic catalysts for PMS-based waste treatment.

Keywords: N, S co-doping; Peroxymonosulfate; Singlet oxygen and electron transfer; Tetracycline.