期刊
CHEMICAL ENGINEERING JOURNAL
卷 298, 期 -, 页码 225-233出版社
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2016.04.028
关键词
Antibiotics; Persulfate; Sulfate radical; Tetracycline; Thermo activation
资金
- China Postdoctoral Research Funds [2015M570454]
- National Science Foundation of China [51578294]
- Jiangsu Planned Projects for Postdoctoral Research Funds [1402013A]
- Fundamental Research Funds for the Central Universities [KYZ201407]
- Priority Academic Program Development (PAPD) of Jiangsu Higher Education Institute
Tetracyclines (TCs), including tetracycline (TTC), oxytetracycline (OTC), and chlorotetracycline (CTC), are frequently detected in natural waters, soils, and sediments, which raised great concerns about the proliferation of antibiotic resistant genes. This study investigated the degradation of TCs by sulfate radical produced by thermo-activated persulfate in aqueous solution. Increasing the temperature significantly enhanced the degradation of TTC, and the relationship between pseudo-first-order rate constant (k(obs)) and temperature obeyed Arrhenius equation. The degradation of TTC showed pH dependence, and k(obs) increased markedly with increasing pH. Seven intermediate products of TTC were temporarily identified by solid phase extraction and liquid chromatography-tandem mass spectrometry (SPE-LC-MS/MS). The transformation pathways of TTC included N-demethylation, hydroxylation-oxidation and dehydration. Detailed mechanisms for sulfate radical-induced N-demethylation and hydroxylation-oxidation were proposed. The degradation of the three TCs followed the order of OTC > CTC > TTC, highlighting the structure-specific reactivity. Interestingly, TTC was degraded extremely fast in artificial surface water (ASW), implying sulfate radical-based oxidation of TCs may be efficient in environmentally relevant conditions. The antimicrobial potency and ecotoxicological effects of the degradation products warrant further studies. (C) 2016 Elsevier B.V. All rights reserved.
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