Heterogeneous degradation of chloramphenicol antibiotic by peroxymonosulfate activated by FeS and FeS2: Mechanism and effects of catalysts dosage and pH

Abstract

Antibiotics in the environmental waters pose long-term threat to ecological safety because of their persistent and potential toxic nature. FeS and FeS2 were proved to be efficient catalysts for the activation of peroxymonosulfate (PMS) and the generation of sulfate radical generation for refractory pollutant degradation. However, their performance for antibiotic degradation has not yet been comparatively and comprehensively investigated. Herein, the FeS/PMS and FeS2/PMS systems were developed to explore chloramphenicol (CAP) degradation under equal conditions. The results show that CAP was efficiently degraded in both two systems, with a removal efficiency exceeding 90 % within 120 min using 6 mM PMS and 0.6 g/L catalysts.Acceleration in degradation rate was observed in the FeS2/PMS system when the catalyst dosage ranged from 0.1 g/L to 1.0 g/L (constant PMS concentration) with a reaction rate constant (kobs) of 2.1-fold higher than that in the FeS/PMS system. However, the kobs were comparable with the PMS concentration range (constant catalyst dosage) in the two systems, suggesting that the catalysts were the rate-limiting step in CAP degradation process. The initial pH strongly affected CAP degradation in the FeS/PMS system but had little effect on that in the FeS2/PMS system. Surface Fe2+ played a dominant role in PMS activation, and S22−/S2− facilitated Fe2+ regeneration. Further, both FeS and FeS2 had stable activity for PMS activation during long-term use. This study proves the effectiveness of FeS and FeS2 for PMS activation for antibiotic degradation and differentiates their catalytic qualities, which will provide alternative heterogeneous catalysts for practical application.