Accelerated Oxidation of Organic Contaminants by Ferrate(VI): The Overlooked Role of Reducing Additives.

Accelerated Oxidation of Organic Contaminants by Ferrate(VI): The Overlooked Role of Reducing Additives.
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DOI:
10.1021/acs.est.8b03770
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发表时间:
2018-10-02
影响因子:
11.4
通讯作者:
Sharma VK
Sharma VK
中科院分区:
环境科学与生态学1区
文献类型:
--
作者:
Feng M;Jinadatha C;McDonald TJ;Sharma VK

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本文报道了在30 S中加入单电子和双电子转移还原剂(R(1)和R(2))加速高铁酸盐(FeVIO42−,FeVI)氧化污染物的方法。添加R(2)(例如,NH2OH、AsIII、SeIV、PIII和NO2−,以及S2O32−)最初产生FeIV,而添加R(1)(例如,SO32−)生成FeV。R(2)添加剂,除S_2O_32−外,对20-40%的目标污染物甲氧苄氨嘧啶(TMP)有增强氧化作用。与之相比,在FeVI中加入R(1),TMP的氧化强度可达100%。有趣的是,添加S2O32−(即R(2))也可以使氧化增强到100%。TMP的去除效率取决于摩尔比([R(1)]:[FeVI]或[R(2)]:[FeVI])。当∼的摩尔比为0.125时,大多数还原剂的脱色率最高。FeVI-S2O32−系统还可以快速氧化水和真实水基质中的各种有机污染物(药物、杀虫剂、人工甜味剂和X射线造影剂)。通过测定含氧水和除氧水中污染物的去除量,使用探针剂,以及用FeVI-S2O32−系统鉴定−和磺胺二甲氧嘧啶的氧化产物,阐明了FeV和FeIV是FeVI-S2O32 TMP-污染物体系中的氧化物种。值得注意的是,首次观察到从磺胺(即SDM)中消除SO2。
This paper presents an accelerated ferrate(VI) (FeVIO42−, FeVI) oxidation of contaminants in 30 s by adding one-electron and two-electron transfer reductants (R(1) and R(2)). An addition of R(2) (e.g., NH2OH, AsIII, SeIV, PIII, and NO2−, and S2O32−) results in FeIV initially, while FeV is generated with the addition of R(1) (e.g., SO32−). R(2) additives, except S2O32−, show the enhanced oxidation of 20–40% of target contaminant, trimethoprim (TMP). Comparatively, enhanced oxidation of TMP was up to 100% with the addition of R(1) to FeVI. Interestingly, addition of S2O32− (i.e., R(2)) also achieves the enhanced oxidation to 100%. Removal efficiency of TMP depends on the molar ratio ([R(1)]:[FeVI] or [R(2)]:[FeVI]). Most of the reductants have the highest removal at molar ratio of ∼0.125. A FeVI–S2O32− system also oxidizes rapidly a wide range of organic contaminants (pharmaceuticals, pesticides, artificial sweetener, and X-ray contrast media) in water and real water matrices. FeV and FeIV as the oxidative species in the FeVI–S2O32−-contaminant system are elucidated by determining removal of contaminants in oxygenated and deoxygenated water, applying probing agent, and identifying oxidized products of TMP and sulfadimethoxine (SDM) by FeVI–S2O32− systems. Significantly, elimination of SO2 from sulfonamide (i.e., SDM) is observed for the first time.
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