g-C3N4 as Photocatalyst for the Removal of Metronidazole Antibiotic from Aqueous Matrices under Lab and Pilot Scale Conditions

Abstract

The presence of pharmaceuticals in water is a problem of utmost importance due to the various adverse effects that these compounds may have on aquatic organisms and also humans. Since conventional wastewater treatment plants fail to efficiently remove many of these compounds, new techniques such as heterogeneous photocatalysis have been developed that are capable of degrading them. In this study, graphitic carbon nitride (g-C3N4) was used as photocatalyst to remove metronidazole (MTZ), which is a widely prescribed antibiotic that has been reported as a potential carcinogen. The experiments were performed under lab and pilot scale conditions. During the lab scale experiments, 90.6% of the initial pharmaceutical concentration was removed after 360 min of irradiation and its removal followed a pseudo first order kinetic model with a degradation rate constant of k = 0.00618 min−1. Moreover, scavenging studies indicated that the indirectly produced hydroxy radicals contribute very little to the degradation mechanism. Through high precision mass spectrometry techniques, eight transformation products (TPs) were identified, and possible transformation pathways were suggested. Similarly, in the case of pilot scale experiments, 100 and 200 mg L−1 of g-C3N4 were used and the antibiotic’s removal also followed pseudo first order kinetics with k = 0.00827 min−1 and k = 0.00942 min−1, respectively. However, starting from low level inherent concentrations, only two TPs were identified. By using in silico tools (ECOSAR and T.E.S.T.), various ecotoxicological values were predicted for the TPs, which were generally found to be less toxic than the parent compound and with lower mutagenic and bioaccumulative potential. Moreover, the monitoring of the ecotoxicity with the in vitro Microtox bioassay showed that at the end of all the photocatalytic processes, the toxicity was reduced. In conclusion, this technique could have the potential to remove MTZ and other similar pharmaceuticals in full-scale applications. However, for this to happen with the highest possible efficiency, further studies must be conducted, focusing on improving the catalyst’s performance and reusability, improving the separation of catalyst as well as finding the optimum conditions for this process.