Electrochemical oxidation of sulfamethoxazole in BDD anode system: Degradation kinetics, mechanisms and toxicity evaluation

Abstract

In the present study, electrochemical oxidation of sulfamethoxazole (SMX) with Boron-doped Diamond (BDD) anode and Stainless Steel (SS) cathode was investigated systematically. The effects of current density, initial pH, supporting electrolyte and natural organic matter (NOM) on SMX degradation were explored. Under the conditions of current density 30 mA cm−2, 0.1 M Na2SO4 used as supporting electrolyte, pH of 7 and without NOM affect, SMX was completely removed after 3 h electrolysis. COD removal efficiency, current efficiency and energy consumption were 65.6%, 40.1%, 72 kWh kg COD−1, respectively. Degradation mechanism was analyzed based on the active sites of SMX identified by density functional theory (DFT) calculation and intermediates analysis by HPLC-Q-TOF-MS/MS. Three possible degradation pathways were proposed, with the replacement of -NH2 at aromatic ring by -OH, the oxidation of -NH2 to -NO2 and the addition of -OH on isoxazole ring observed. The active sites detected in reaction matched the DFT calculation results exactly. The toxicity of intermediates produced during electrolysis process was evaluated by Escherichia coli experiment. Results showed that, after 2 h electrolysis, the inhibition ratio was decreased from the initial value of 22.8% to 10%, which has already achieved the safety boundary. After 4 h electrolysis, the toxicity was almost zero even with still 60% COD remained in the solution. This phenomenon demonstrated that the toxicity of SMX and its intermediate products was reduced significantly during electrolysis process.