A comprehensive insight into plasma-catalytic removal of antibiotic oxytetracycline based on graphene-TiO2-Fe3O4 nanocomposites

Non-thermal plasma coupled with graphene-TiO2-Fe3O4 nanocomposites was applied to promote oxytetracycline (OTC) degradation in water. Graphene-TiO2-Fe3O4 nanocomposites were systematically characterized and calculated based on the density functional theory (DFT). Graphene-TiO2-Fe3O4 nanocomposites exhibited higher specific surface area, carrier separation rate and magnetic intensity. More importantly, graphene-TiO2-Fe3O4 nanocomposites were very prone to separation from solution. Compared to Fe3O4 and graphene-TiO2, graphene-TiO2-Fe3O4 nanocomposites further enhanced the removal efficiency of OTC. The highest removal efficiency could reach 98.1% when the doping amount of Fe3O4 was 20 wt%. The optimal parameters of catalyst dosage, peak voltage, air flow rate and pH value were 0.24 g/L, 18 kV, 4 L/min and 3.2, respectively. Compared with graphene-TiO2, the addition of graphene-TiO2-Fe3O4 nanocomposites decreased the concentration of O-3 and H2O2, but increased the production of center dot OH. center dot OH, O-3 and H2O2 played certain role for OTC elimination. The degradation process was explored by UV-Vis spectrum, three dimensional fluorescence, liquid chromatographymass spectrometry (LC-MS), ion chromatography (IC) and discrete Fourier transform (DFT) analysis. Reactive molecular dynamical (MD) simulation was also performed to further investigate the reaction mechanisms, and the simulation show a good agreement with the experimental observation by analyzing the bond breaking and formation. The actual toxicity of OTC was alleviated after plasma-catalytic treatment.