Oxidation of Pharmaceuticals by Ferrate(VI)–Amino Acid Systems: Enhancement by Proline
Oxidation of Pharmaceuticals by Ferrate(VI)–Amino Acid Systems: Enhancement by Proline
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DOI：
10.1021/acs.jpca.3c00134
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发表时间：
2023-03
期刊：
影响因子：
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通讯作者：
V. Sharma;Junyue Wang;Mingbao Feng;Ching-Hua Huang
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文献类型：
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作者：
V. Sharma;Junyue Wang;Mingbao Feng;Ching-Hua Huang
水中微污染物的存在威胁着公众的健康和生态。通过一种绿色氧化剂高铁酸盐(VI)(FeVIO42-，Fe(VI))可以实现对药物等微污染物的去除。然而，缺乏电子的药物，如卡马西平(CBZ)，对Fe(VI)的去除效率很低。在弱碱性条件下，通过添加9种不同官能度的氨基酸(AA)来加速去除水中的CBZ，研究了Fe(VI)的活化作用。在所研究的氨基酸中，环状氨基酸Pro对CBZ的降解率最高。通过证实Fe(VI)与Pro反应产生的高活性中间体Fe(V)物种(即Fe(VI)+Proline→Fe(V)+Proline·)参与了Pro的加速作用。对Fe(VI)-Pro体系降解CBZ的动力学进行了动力学模拟，得到Fe(V)与CBZ的反应速率为(1.03±0.21)×106M~(-1)·S~(-1)，比Fe(VI)的2.25M~(-1)·S~(-1)高几个数量级。
The occurrence of micropollutants in water threatens public health and ecology. Removal of micropollutants such as pharmaceuticals by a green oxidant, ferrate(VI) (FeVIO42–, Fe(VI)) can be accomplished. However, electron-deficient pharmaceuticals, such as carbamazepine (CBZ) showed a low removal rate by Fe(VI). This work investigates the activation of Fe(VI) by adding nine amino acids (AA) of different functionalities to accelerate the removal of CBZ in water under mild alkaline conditions. Among the studied amino acids, proline, a cyclic AA, had the highest removal of CBZ. The accelerated effect of proline was ascribed by demonstrating the involvement of highly reactive intermediate Fe(V) species, generated by one-electron transfer by the reaction of Fe(VI) with proline (i.e., Fe(VI) + proline → Fe(V) + proline•). The degradation kinetics of CBZ by a Fe(VI)–proline system was interpreted by kinetic modeling of the reactions involved that estimated the rate of the reaction of Fe(V) with CBZ as (1.03 ± 0.21) × 106 M–1 s–1, which was several orders of magnitude greater than that of Fe(VI) of 2.25 M–1 s–1. Overall, natural compounds such as amino acids may be applied to increase the removal efficiency of recalcitrant micropollutants by Fe(VI).