Oxidation of indometacin by ferrate (VI): kinetics, degradation pathways, and toxicity assessment
Oxidation of indometacin by ferrate (VI): kinetics, degradation pathways, and toxicity assessment
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高铁酸盐 (VI) 氧化吲哚美辛：动力学、降解途径和毒性评估
DOI：
10.1007/s11356-017-8750-x
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发表时间：
2017-04-01
影响因子：
5.8
通讯作者：
Lv, Wenying
中科院分区：
文献类型：
--
作者：
Huang, Junlei;Wang, Yahui;Lv, Wenying
研究了高铁酸盐（Fe(VI)）氧化吲哚美辛（IDM）的反应动力学、转化产物和毒性变化。IDM和Fe（VI）之间的反应对每种反应物都遵循一级动力学。当溶液pH从7.0增加到10.0时，表观二阶速率常数kapp从9.35减小到6.52 M−1s−1。考虑到IDM与Fe（VI）反应的物种特异性速率常数，可以很好地解释kapp的pH依赖性。利用液相色谱-串联质谱（LC-MS/MS）对产物进行详细的研究表明，氧化产物主要来源于酰胺键的水解、羟基的加成和亲电氧化。利用Microtox试验对氧化产物的毒性进行了评价，结果表明转化产物对费氏弧菌的毒性较低。通过生态构效关系（ECOSAR）计算的定量构效关系（QSAR）分析表明，所有鉴定产物对鱼、水蚤和绿藻的急性和慢性毒性均低于母体药物。此外，Fe（VI）对含碳酸盐离子、富里酸（FA）的水体和湖泊水样中的IDM有较好的降解效果；然而，与去离子水相比，要完全去除湖水中的IDM，需要更高的铁（VI）剂量。
The oxidation of indometacin (IDM) by ferrate(VI) (Fe(VI)) was investigated to determine the reaction kinetics, transformation products, and changes in toxicity. The reaction between IDM and Fe(VI) followed first-order kinetics with respect to each reactant. The apparent second-order rate constants (kapp) decreased from 9.35 to 6.52 M−1s−1, as the pH of the solution increased from 7.0 to 10.0. The pH dependence ofkappmight be well explained by considering the species-specific rate constants of the reactions of IDM with Fe(VI). Detailed product studies using liquid chromatography-tandem mass spectrometry (LC-MS/MS) indicated that the oxidation products were primarily derived from the hydrolysis of amide linkages, the addition of hydroxyl groups, and electrophilic oxidation. The toxicity of the oxidation products was evaluated using the Microtox test, which indicated that transformation products exhibited less toxicity to theVibrio fischeribacteria. Quantitative structure-activity relationship (QSAR) analysis calculated by the ecological structure activity relationship (ECOSAR) revealed that all of the identified products exhibited lower acute and chronic toxicity than the parent pharmaceutical for fish, daphnid, and green algae. Furthermore, Fe(VI) was effective in the degradation IDM in water containing carbonate ions or fulvic acid (FA), and in lake water samples; however, higher Fe(VI) dosages would be required to completely remove IDM in lake water in contrast to deionized water.