Abstract

Tetracycline antibiotics are widely used in human and veterinary medicine; however, their gradual increase in the aquatic environment poses a serious threat to human health and ecosystems. The reactivity of peroxydisulfate (PDS) in the degradation of chlortetracycline (CTC) in aqueous solution using a zero-valent iron/activated carbon (AC) microelectrolysis method (Fe0–AC/PDS) was investigated by batch experiments. The results showed that the effects of different systems were as follows: Fe0–AC/PDS > Fe0/PDS > AC/PDS > Fe0–AC > AC > Fe0 > PDS. In the Fe0–AC/PDS system, the degradation efficiency of CTC could reach 88% under the following optimal experimental conditions: Fe0 dose of 0.4 g L−1, PDS dose of 2 g L−1, pH of 3 and initial CTC concentration of 50 mg L−1. The presence of Cl−, HCO3− and H2PO4− inhibited the degradation of CTC, while humic acid accelerated the degradation rate of CTC. The mineralization of CTC was evaluated from the TOC, with a value of 31.44% in 7 h. Free radical identification experiments showed that SO4−˙ and O2−˙ were involved in the degradation of CTC. The iron and carbon materials had good reusability, and the degradation rate of CTC was still approximately 70% after four cycles. Finally, the possible mechanism for the degradation of CTC by the Fe0–AC/PDS systems was discussed. Based on the above conclusions, Fe0–AC microelectrolysis is a new heterogeneous catalytic method for green and efficient activation of PDS and demonstrates potential applicability in the treatment of wastewater.

Highlights

  • Tetracyclines (TCs) are broad-spectrum antibiotics.[1]

  • In the Fe0–activated carbon (AC) system, the removal rate of CTC was 20.24%, which showed that the oxidation ability of the active groups produced by Fe0–AC microelectrolysis was limited

  • The results showed that the Fe0–AC microelectrolysis system could generate more oxidation radicals by activating PDS, which was more conducive to the removal of CTC

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Summary

Introduction

Tetracyclines (TCs) are broad-spectrum antibiotics.[1] Because of their advantages of high quality and low price,[2] TCs have been widely used to improve human health, treat and prevent animal infection, and promote growth in animal husbandry.[3] due to the essential characteristics of antibiotics, people and animals can only absorb and metabolize some of the TCs, and a considerable percentage (70%–90%) is released into the environment through wastewater effluent and animal manure.[4] In addition, the excessive use of TCs will result in them entering the environment through municipal effluent, sewage sludge, solid wastes and manure applications,[5] causing significant toxicity and serious contamination. It is crucial to study and promote the technology of removing TCs for maintaining a healthy environment. Excessive Fe2+ consumes the sulfate radical generated in the system, as shown in eqn (1):[23]

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