Antibiotics oxytetracycline removal by photocatalyst titanium dioxide and graphitic carbon nitride in aquaculture wastewater

Abstract

The surge in the use of antibiotics, especially in aquaculture, has led to development of antibiotic resistance genes, which will harm environmental and public health. One of the most commonly used antibiotics in aquaculture is oxytetracycline (OTC). Employing photocatalysis, this study compared OTC degradation efficiency of two different types of common photocatalysts, TiO2 and graphitic carbon nitride (GCN) in terms of their photochemical properties and underlying photocatalytic mechanism. For reference purpose, self-synthesized GCN from urea precursor (GCN-Urea) and commercial GCN (GCN-Commercial) were both examined. OTC adsorption-photocatalysis removal rates in pure OTC solution by TiO2, GCN-Urea and GCN-Commercial were attained at 95%, 60% and 40% respectively. Photochemical properties evaluated included light absorption, band gap, valence and conduction band positions, photoluminescence, cyclic voltammetry, BET surface area and adsorption capability of the photocatalysts. Through the evaluations, this study provides novel insights towards current state-of-the-art heterogeneous photocatalytic processes. The electron-hole recombination examined by photoluminescence is not the key factor influencing the photocatalytic efficacies as commonly discussed. On the contrary, the dominating factors governing the higher OTC degradation efficiency of TiO2 compared to GCN are the high mobility of electrons that leads to high redox capability and the high pollutant-photocatalyst affinity. These claims are proven by 86% and 40% more intense anodic and cathodic cyclic voltammetry curve peaks of TiO2 as compared to both GCNs. OTC also demonstrated 1.7 and 2.3 times higher affinity towards TiO2 than GCN-Urea and GCN-Commercial. OTC removal by TiO2 in real aquaculture wastewater only achieved 50%, due to significant inhibition effect by dissolved solids, dissolved organic matters and high ionic contents in the wastewater.