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高铁酸盐(VI)加速氧化有机污染物:还原剂的被忽视作用。

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

机构信息

Program for the Environment and Sustainability, Department of Environmental and Occupational Health, School of Public Health , Texas A&M University , College Station , Texas 77843 , United States.

Central Texas Veterans Health Care System , 1901 Veterans Memorial Drive , Temple , Texas United States.

出版信息

Environ Sci Technol. 2018 Oct 2;52(19):11319-11327. doi: 10.1021/acs.est.8b03770. Epub 2018 Sep 18.

Abstract

This paper presents an accelerated ferrate(VI) (FeO, Fe) oxidation of contaminants in 30 s by adding one-electron and two-electron transfer reductants (R and R). An addition of R (e.g., NHOH, As, Se, P, and NO, and SO) results in Fe initially, while Fe is generated with the addition of R (e.g., SO). R additives, except SO, 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 to Fe. Interestingly, addition of SO (i.e., R) also achieves the enhanced oxidation to 100%. Removal efficiency of TMP depends on the molar ratio ([R]:[Fe] or [R]:[Fe]). Most of the reductants have the highest removal at molar ratio of ∼0.125. A Fe-SO 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. Fe and Fe as the oxidative species in the Fe-SO-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 Fe-SO systems. Significantly, elimination of SO from sulfonamide (i.e., SDM) is observed for the first time.

摘要

本文通过添加单电子和双电子转移还原剂(R 和 R),在 30 秒内实现了铁酸盐(VI)(FeO,Fe)对污染物的加速氧化。添加 R(例如,NHOH、As、Se、P 和 NO、SO)会导致 Fe 的初始生成,而添加 R(例如,SO)会生成 Fe。除 SO 外,R 添加剂对目标污染物甲氧苄啶(TMP)的氧化增强了 20-40%。相比之下,添加 R 到 Fe 中可使 TMP 的氧化增强高达 100%。有趣的是,添加 SO(即 R)也可实现 100%的氧化增强。TMP 的去除效率取决于摩尔比([R]:[Fe]或[R]:[Fe])。大多数还原剂在摩尔比约为 0.125 时具有最高的去除效率。Fe-SO 体系还可快速氧化水中和实际水基质中的多种有机污染物(药物、农药、人工甜味剂和 X 射线造影剂)。通过确定含氧和脱氧水中污染物的去除、应用探针剂以及通过 Fe-SO 体系鉴定 TMP 和磺胺二甲氧嘧啶(SDM)的氧化产物,阐明了 Fe-SO-污染物体系中的氧化物种为 Fe 和 Fe。值得注意的是,首次观察到从磺胺类药物(即 SDM)中消除 SO。

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