The contamination of surface and ground water by antibiotics is of significant importance due to their potential chronic toxic effects to the aquatic and human lives. Thus, in this work, the electrochemical oxidation of cephalexin (CEX) was carried out in a one compartment filter-press flow cell using a boron-doped diamond (BDD) electrode as anode. During the electrolysis, the investigated variables were: supporting electrolyte (NaSO, NaCl, NaNO, and NaCO) at constant ionic strength (0.1 M), pH (3, 7, 10, and without control), and current density (5, 10 and 20 mA cm). The oxidation and mineralization of CEX were assessed by high performance liquid chromatography, coupled to mass spectrometry and total organic carbon. The oxidation process of CEX was dependent on the type of electrolyte and on pH of the solution due to the distinct oxidant species electrogenerated; however, the conversion of CEX and its hydroxylated intermediates to CO depends only on their diffusion to the surface of the BDD. In the final stages of electrolysis, an accumulation of recalcitrant oxamic and oxalic carboxylic acids, was detected. Finally, the growth inhibition assay with Escherichia coli cells showed that the toxicity of CEX solution decreased along the electrochemical treatment due to the rupture of the β-lactam ring of the antibiotic.
Highlights
Both fluoroquinolones are totally removed regardless of supporting electrolyte (SE)
Use of NaCl leads to a significantly faster removal of the fluoroquinolones (FQs)
The SE nature affects the TOC removal rate, much more markedly for NaCl
Solution antimicrobial activity
vs.
electrolysis time is affected by SE and FQ nature
LC-MS/MS analyses show that both SE and FQ nature determine occurring oxidation steps
The electrochemical degradation of ciprofloxacin-CIP (50 mg L in 0.10 mol L NaSO) was investigated using a double-sided Ti-Pt/β-PbO anode in a filter-press flow reactor, with identification of oxidation intermediates and follow-up of antimicrobial activity against Escherichia coli. The effect of solution pH, flow rate, current density, and temperature on the CIP removal rate was evaluated. All of these parameters did affect the CIP removal performance; thus, optimized electrolysis conditions were further explored: pH = 10, q = 6.5 L min, j = 30 mA cm, and θ = 25 °C. Therefore, CIP was removed within 2 h, whereas ~75% of the total organic carbon concentration (TOC) was removed after 5 h and then, the solution no longer presented antimicrobial activity. When the electrochemical degradation of CIP was investigated using a single-sided boron-doped diamond (BDD) anode, its performance in TOC removal was similar to that of the Ti-Pt/β-PbO anode; considering the higher oxidation power of BDD, the surprisingly good comparative performance of the Ti-Pt/β-PbO anode was ascribed to significantly better hydrodynamic conditions attained in the filter-press reactor used with this electrode. Five initial oxidation intermediates were identified by LC-MS/MS and completely removed after 4 h of electrolysis; since they have also been determined in other degradation processes, there must be similarities in the involved oxidation mechanisms. Five terminal oxidation intermediates (acetic, formic, oxamic, propionic, and succinic acids) were identified by LC-UV and all of them (except acetic acid) were removed after 10 h of electrolysis.
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