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Fe2+/HClO Reaction Produces FeIVO2+: An Enhanced Advanced Oxidation Process.
Environmental Science & Technology ( IF 10.8 ) Pub Date : 2020-03-23 , DOI: 10.1021/acs.est.0c00218
Sheng Liang,Liuyi Zhu,Jian Hua,Weijian Duan,Puu-Tai Yang,Shan-Li Wang,Chaohai Wei,Chengshuai Liu,Chunhua Feng

The reaction between Fe2+ and HClO constitutes a promising advanced oxidation process (AOP) for removing pollutants from wastewater, and •OH has been considered the dominant reactive oxidant despite limited evidence for this. Herein, we demonstrate that the Fe2+/HClO reaction enables the production of FeIVO2+ rather than •OH in acid medium, a finding that is strongly supported by multiple lines of evidence. Both X-ray absorption near-edge structure spectroscopic tests and Mössbauer spectroscopic tests confirmed the appearance of FeIVO2+ as the reactive intermediate in the reaction between Fe2+ and HClO. The determination of FeIVO2+ generation was also derived from the methyl phenyl sulfoxide (PMSO)-based probe experiments with respect to the formation of PMSO2 without •OH adducts and the density functional theory studies according to the lower energy barrier for producing FeIVO2+ compared with •OH. A dual-anode electrolytic system was established for the in situ generation of Fe2+ and HClO that allows the production of FeIVO2+. The system exhibits an enhanced capacity for oxidizing a model pollutant (e.g., phosphite) from industrial wastewater, making it an attractive and promising AOP for the abatement of aqueous contaminants.

中文翻译:

Fe2 + / HClO反应产生FeIVO2 +:一种增强的高级氧化工艺。

Fe2 +和HClO之间的反应构成了一种有前途的高级氧化工艺(AOP),用于去除废水中的污染物,尽管对此证据有限,但•OH被认为是主要的活性氧化剂。本文中,我们证明了Fe2 + / HClO反应能够在酸性介质中生成FeIVO2 +而不是•OH,这一发现得到了多条证据的有力支持。X射线吸收近边缘结构光谱测试和Mössbauer光谱测试均证实FeIVO2 +的出现是Fe2 +与HClO之间反应的反应中间体。FeIVO2 +生成的测定也来自基于甲基苯基亚砜(PMSO)的探针实验,涉及不带•OH加合物的PMSO2的形成以及根据与•OH相比产生FeIVO2 +的较低能垒的密度泛函理论研究。建立了双阳极电解系统,用于原位生成Fe2 +和HClO,从而生产F​​eIVO2 +。该系统具有增强的能力,可氧化工业废水中的模型污染物(例如亚磷酸盐),使其成为用于消除水性污染物的诱人且有前途的AOP。
更新日期:2020-03-11
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