Effective Degradation of Metronidazole through Electrochemical Activation of Peroxymonosulfate: Mechanistic Insights and Implications

Abstract

The investigation into the degradation of metronidazole (MNZ), a frequently employed antibiotic, through the electrochemical activation of peroxymonosulfate (PMS) utilizing either boron-doped diamond (BDD) or dimensional stable anode (DSA) as the anode, was conducted in a systematic manner. The enhancement of MNZ removal was observed with increasing current density, PMS dosage, and initial pH. Response surface methodology (RSM), based on a Box–Benken design, was utilized to evaluate the efficiency of MNZ elimination concerning current density (ranging from 11.1 to 33.3 mA/cm2), initial pH (ranging from 3 to 9), PMS dosage (ranging from 1 to 5 mmol·L−1), and reaction time (ranging from 25 to 45 min). The optimal operational conditions for MNZ removal were determined as follows: a current density of 13.3 mA/cm2, a pH of 3.7, a PMS dosage of 2.4 mmol·L−1, and a reaction time of 40 min. Electron paramagnetic resonance (EPR), quenching experiments, and chemical probe experiments confirmed the involvement of •OH, SO4•− and 1O2 radicals as the primary reactive species in MNZ degradation. The presence of HCO3− and H2PO4− hindered MNZ removal, whereas the presence of Cl− accelerated it. The degradation pathways of MNZ were elucidated by identifying intermediates and assessing their toxicity. Additionally, the removal efficiencies of other organic pollutants, such as sulfamethoxazole (SMX), carbamazepine (CBZ), and nitrobenzene (NB), were compared. This study contributes to a comprehensive understanding of MNZ degradation efficiency, mechanisms, and pathways through electrochemical activation of PMS employing BDD or DSA anodes, thereby offering valuable insights for the selection of wastewater treatment systems.