Degradation of the antibiotic trimethoprim by electrochemical advanced oxidation processes using a carbon-PTFE air-diffusion cathode and a boron-doped diamond or platinum anode

摘要

The degradation of 20.0 mg L~(-1) of trimethoprim (TMP), an antibiotic commonly detected in wastewaters, in an aqueous solution with 7.0gL~(-1) Na2S04 was accomplished by electrochemical advanced oxidation processes (EAOPs) such as anodic oxidation with electrogenerated H2O2 (AO-H2O2), electro-Fenton (EF), photoelectro-Fenton (PEF) and solar photoelectro-Fenton (SPEF), as well as by the classical Fenton and photo-Fenton processes. All experiments were performed in a novel 2.2 L lab-scale flow plant equipped with compound parabolic collectors (CPCs) and an electrochemical filter-press cell with a BDD or Pt anode and a carbon-PTFE air-diffusion cathode to electrogenerate H2O2. The effect of initial Fe~(2+) concentration, current density and pH on the PEF method with the BDD anode (PEF-BDD) was firstly assessed by means of TMP and dissolved organic carbon (DOC) decays, aiming to establish a treatment process using minimal iron concentration, adequate current density/H2O2 production and maximal pH. This treatment was efficiently performed using a low Fe~(2+) dose of 2.0 mg L~(-1), a low current density of 5 mA cm~(-2) and pH of 3.5 without iron precipitation. The relative oxidation ability of EAOPs using the BDD/air-diffusion cell increased in the order: AO-H2O2 < EF < PEF < SPEF. The EF-BDD and PEF-BDD processes were more effective than the comparable Fenton and photo-Fenton ones. The PEF-BDD process exhibited slightly faster TMP degradation than the PEF-Pt one, whereas in SPEF the influence of the anode was almost negligible. After ca. 37 kJ L~(-1) UV energy, 77 and 73% mineralization with 30 and 26% current efficiency and 1.2 and 0.9 kWh m~(-30 energy cost were obtained, respectively. It was found a slow and partial TMP mineralization mainly linked to the formation of a high content of hardly oxidizable N-derivatives, containing the major part of N. Up to 18 aromatic products and 19 hydroxylated derivatives were detected by LC-MS during TMP degradation by PEF-Pt. An additional SPEF-Pt experiment using a real wastewater matrix spiked with TMP attained slower TMP and DOC decays.