Abstract
The removal of tetracycline antibiotics from water is currently an important environmental issue. Here we prepared an iron-loaded granular activated carbon catalyst (GAC-Fe) through a one-step calcination method to remove tetracycline antibiotics from aqueous solution. The GAC-Fe was characterized by Fourier transform infrared absorption spectroscopy, X-ray photoelectron spectroscopy, and X-ray diffraction analysis. The effect of different influencing factors on the removal behavior of tetracycline antibiotics was studied, such as the solid-to-liquid ratio, H2O2 dosage, environmental temperature, initial pH, and contact time. The removal mechanism was explored through Fe ion dissolution and a free radical quenching experiment. The results show that the optimum solid-to-liquid ratio was 3.0 g∙L−1 and the suitable H2O2 dosage was 1.0 mL (3%). The applicable environmental temperature was 25 °C and the appropriate pH value was 2.0. The removal rate of tetracycline antibiotics tended to be stable in a contact time of 600 min. The main mechanism of tetracycline antibiotic removal by GAC-Fe was heterogeneous catalytic reaction through iron ion leaching and free radical inhibition experiment. The hydroxyl radical played a major role during the removal process. The partially dissolved iron ions initiated a homogeneous catalytic reaction. However, heterogeneous catalytic degradation was the main reaction. The GAC-Fe could still remove tetracycline antibiotics after five cycles, especially for methacycline and minocycline. Our work suggests that the GAC-Fe catalyst has potential as a remediation agent for tetracycline antibiotics in aqueous solution.
Highlights
Tetracycline antibiotics are among the most used antibiotic group for human and animal health [1,2].Due to their low cost and high antimicrobial activity, tetracycline antibiotics are marketable in developing countries [1]
An Fe ion loaded granular activated carbon (GAC-Fe) catalyst was prepared by one-step calcination with ferrous ions supported by GAC as a carrier, and the effects of solid–liquid ratio, H2 O2 dosage, ambient temperature, initial pH, and contact time on antibiotic removal were investigated
As shown in the spectrum, the peak shape of GAC in the range of 20–30 (2θ) is not sharp, indicating that amorphous carbon dominated in the GAC
Summary
Tetracycline antibiotics are among the most used antibiotic group for human and animal health [1,2]. The above studies showed that an iron-loaded carbon-based catalyst had a better removal effect than a pollutant in aqueous solution. Ma et al [35] synthesized heterogeneous carbon nanotubes/FeS Fenton-like catalyst and used it for the removal of antibiotics from aqueous solution. The preparation of heterogeneous catalysts on granular activated carbon (GAC) through loading iron ions and the simultaneous degradation of multiple tetracycline antibiotics have rarely been reported. An Fe ion loaded granular activated carbon (GAC-Fe) catalyst was prepared by one-step calcination with ferrous ions supported by GAC as a carrier, and the effects of solid–liquid ratio, H2 O2 dosage, ambient temperature, initial pH, and contact time on antibiotic removal were investigated. This research can provide a theoretical basis and technical reference for the resource utilization of GAC and the control of antibiotic wastewater pollution
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