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Oxidation of tetracycline and oxytetracycline for the photo-Fenton process: Their transformation products and toxicity assessment

土霉素 四环素 毒性 核化学 降级(电信) 过氧化氢 环境化学 化学 脱质子化 紫外线 生物化学 抗生素 有机化学 材料科学 光电子学 电信 离子 计算机科学
作者
Chee-Hun Han,Hee‐Deung Park,Song-Bae Kim,Viviane Yargeau,Jae‐Woo Choi,Sang-Hyup Lee,Jeong-Ann Park
出处
期刊:Water Research [Elsevier BV]
卷期号:172: 115514-115514 被引量:268
标识
DOI:10.1016/j.watres.2020.115514
摘要

Advanced oxidation processes have gained significant attention for treating tetracycline (TC) and oxytetracycline (OTC), however, their oxidation using the photo-Fenton process has not been sufficiently studied. Although degradations of TC and OTC were enhanced by increasing H2O2 and Fe2+ within the ranges investigated (H2O2 = 20-50 mg/L and Fe = 1-10 mg/L) under UV irradiation, further experiments for the photo-Fenton process were conducted with 20 mg/L of H2O2 and 5 mg/L of Fe2+ to balance efficiency and cost. The photo-Fenton process (UV/H2O2/Fe2+) was shown to be more effective to remove TC and OTC than H2O2, ultraviolet (UV), and UV/H2O2 at the same doses of oxidants. Inorganic anions and cations were shown to inhibit the degradation of TC and OTC during the photo-Fenton process, in the following order: HPO42- > HCO3- ≫ SO42- > Cl- and Cu2+ ≫ Ca2+ > Na+. The TC and OTC degradation are generally improved by increasing pH, which is opposite to the kpCBA,obs values, caused by increasing the deprotonation degree of TC and OTC. Four and nine transformation products of TC and OTC, respectively, were detected over the treatment period. Among the transformation products, m/z 443.14 (C22H22N2O8) formed during TC degradation, and m/z 433.16 (C20H20N2O9) and m/z 415.15 (C20H18N2O8) formed during OTC degradation, were reported for the first time. Vibrio fischeri toxicity assessment indicated that the inhibition ratio was decreased with a decreasing TC concentration, while, OTC transformation lead to higher toxicity. The product (m/z 477.15b) was determined to be the compound causing toxicity during degradation of OTC by using the quantitative structure activity relationship (QSAR). This toxic transformation product caused higher inhibition ratios than its parental compound (OTC), but its further oxidization resulted in decreasing the inhibition ratios.
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