Fe3+ enhanced degradation of oxytetracycline in water by pseudomonas

Abstract

The application and fate of antibiotics are closely related to human health and the ecological balance, which has gradually aroused the widespread global concerns. Long-term antibiotic residues can easily induce antibiotic resistance and antibiotic resistance genes (ARGs) in the environment. Although many studies have investigated the metabolic pathways of biosynthesis or degradation of oxytetracycline (OTC) and its influencing factors under laboratory or controlled conditions, the understanding of OTC degradation pathways and influencing factors in the environment is still poor. In the present study, the role of Pseudomonas (T4) in OTC biodegradation were investigated with different carbon sources, metal ions, substrate concentrations, temperatures, and pH values, as well as the temporal changes in the relative abundance of OTC ARGs. It was found that OTC could be degraded by T4 as a sole carbon source. Comparison with Cu2+, the addition of Fe3+ could significantly promote the growth of T4, and then increased the OTC degradation percentage to 65.3%. The initial concentration of OTC, temperature, and pH had significant impacts on OTC degradation. At the initial OTC concentration of 50 mg L−1, the percentage degradation of OTC by T4 could reach 81.0% at the presence of Fe3+, and at 40 °C and pH = 7. Common tetracycline ARGs were not found during the OTC degradation by T4 in the present study. The eight main putative OTC degradation byproducts were identified by ultra-high definition accurate-mass quadrupole time-of-flight tandem mass spectrometry (QTOF/MS). Six different reaction types and seven possible degradation pathways were proposed, including enol-ketone conversion, hydroxylation, dehydration, deamination, demethylation and decarbonylation. Under optimal conditions, the OTC degradation percentages by T4 could reach to 88.2%, 91.6% and 92.0% in pond water, fish wastewater and industrial wastewater, respectively. These results demonstrate the high effectiveness of T4 at the presence of Fe3+ for the enhanced biodegradation of OTC in water environment, without resulting in the occurrence of ARGs. This has important implications for the removal of OTC from aquatic environments by the technology proposed from this study.