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典型大环内酯类抗生素罗红霉素被羟基自由基降解:动力学、产物及毒性评估。

Degradation of typical macrolide antibiotic roxithromycin by hydroxyl radical: kinetics, products, and toxicity assessment.

机构信息

Co-Innovation center for sustainable Forestry in Southern China, College of Biology and the Environment, Nanjing Forestry University, Longpan Road 159, Nanjing, 210037, China.

Advanced Analysis and Testing Center, Nanjing Forestry University, Longpan Road 159, Nanjing, 210037, China.

出版信息

Environ Sci Pollut Res Int. 2019 May;26(14):14570-14582. doi: 10.1007/s11356-019-04713-1. Epub 2019 Mar 14.

Abstract

The degradation of roxithromycin (ROX) by hydroxyl radical (·OH) generated by UV/HO was systematically investigated in terms of degradation kinetics, effects of water chemistry parameters, oxidation products, as well as toxicity evaluation. The degradation of ROX by UV/HO with varying light irradiation intensity, initial ROX concentration, and HO concentration in pure water and wastewater all followed pseudo-first-order kinetics. The second-order rate constant for reaction between ROX and ·OH is 5.68 ± 0.34 × 10/M/s. The degradation rate of ROX increased with the pH; for instance, the apparent degradation rates were 0.0162 and 0.0309/min for pH 4 and pH 9, respectively. The presence of natural organic matter (NOM) at its concentrations up to 10 mg C/L did not significantly affect the removal of ROX. NO and NO anions inhibited the degradation of ROX due to the consumption of ·OH in reactions with these ions. Fe, Cu, and Mg cations inhibited the degradation of ROX, probably because of the formation of ROX-metal chelates. A total of ten degradation products were tentatively identified by HPLC/LTQ-Orbitrap XL MS, which mainly derived from the attack on the oxygen linking the lactone ring and the cladinose moiety, tertiary amine and oxime side chain moiety by ·OH. The toxicity evaluation revealed that UV/HO treatment of ROX induced the toxicity to bioluminescent bacteria increased.

摘要

羟基自由基(·OH)引发的 UV/HO 降解罗红霉素(ROX)的动力学、水化学参数影响、氧化产物以及毒性评价。ROX 在纯水中和废水中的 UV/HO 降解,随着光照强度、初始 ROX 浓度和 HO 浓度的变化,降解动力学均遵循准一级动力学。ROX 与·OH 的二级反应速率常数为 5.68 ± 0.34 × 10/M/s。ROX 的降解速率随 pH 值的增加而增加;例如,pH 值为 4 和 9 时的表观降解速率分别为 0.0162 和 0.0309/min。在高达 10 mg C/L 的天然有机物(NOM)浓度下,其存在并没有显著影响 ROX 的去除。由于这些离子与·OH 的反应消耗了·OH,NO 和 NO 阴离子抑制了 ROX 的降解。Fe、Cu 和 Mg 阳离子抑制了 ROX 的降解,可能是因为形成了 ROX-金属配合物。通过 HPLC/LTQ-Orbitrap XL MS 共鉴定出 10 种降解产物,主要源于·OH 对内酯环和克拉定糖部分、叔胺和肟侧链部分的攻击。毒性评价表明,UV/HO 处理 ROX 导致发光细菌的毒性增加。

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