Activation of peroxymonosulfate by Fe doped g-C3N4 /graphene under visible light irradiation for Trimethoprim degradation

Abstract

Fe-doped g-C3N4 / graphene (rGO) composites were investigated as catalysts for the activation of peroxymonosulfate (PMS) to degrade Trimethoprim (TMP) under visible light irradiation. The rapid recombination of photogenerated electron-hole pairs in g-C3N4 may be suppressed by doping with Fe and incorporating rGO. The TMP degradation efficiency using 0.2% Fe-g-C3N4/2 wt% rGO/PMS was 3.8 times than that of g-C3N4/PMS. The degradation efficiency of TMP increased with higher catalyst dosages and PMS concentrations. Acidic condition (pH = 3) was observed to significantly enhance the TMP degradation efficiency from 61.4% at pH = 6 to nearly 100%. By quenching experiments and electron spin resonance (ESR), O2− was found to play an important role for the activation of PMS to accelerate the generation of reactive radicals for the TMP degradation. A total of 8 intermediates derived from hydroxylation, demethoxylation and carbonylation were identified through theoretical calculations and the HRAM/LC–MS-MS technique, and transformation pathways of TMP oxidation were proposed. TOC removal rate of TMP increased as reaction time was prolonged. Acute toxicity estimation by quantitative structure-active relationship analysis indicated that most of the less toxic intermediates were generated. The aim of this study was to elucidate and validate the functionality of a promising polymeric catalyst for the environmental remediation of organic contaminants.