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原位和异位过氧化氢在增强高铁酸盐(VI)氧化有机污染物中的作用的深入了解。

Insights into the role of in-situ and ex-situ hydrogen peroxide for enhanced ferrate(VI) towards oxidation of organic contaminants.

机构信息

State Key Laboratory of Hydraulics and Mountain River Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China; Sino-German Centre for Water and Health Research, Sichuan University, Chengdu 610065, China.

The Key Laboratory of Water and Sediment Sciences, Ministry of Education, College of Environmental Sciences and Engineering, Peking University, Beijing 100871, China.

出版信息

Water Res. 2021 Sep 15;203:117548. doi: 10.1016/j.watres.2021.117548. Epub 2021 Aug 13.

Abstract

Recently, several studies have been conscious of the promotion effect of hydrogen peroxide (HO), a self-decay product of ferrate (Fe(VI)), on Fe(VI) to oxidize contaminations, but the pivotal activation mechanism has not been thoroughly evaluated. This work aims to compare and reveal the promoting mechanism of HO in Fe(VI) and Fe(VI)-HO processes, and to illustrate the practical use potential of Fe(VI)-HO system. Many lines of evidence verified the involvement of OH and O in pollutant degradation were excluded in Fe(VI) and Fe(VI)-HO systems, meaning that high dosage of HO cannot trigger an activation pathway different from in-situ HO. The better oxidation performance of the Fe(VI)-HO system than Fe(VI) alone was ascribed to the catalytic role of in-situ and ex-situ HO, which can directly and/ or indirectly facilitate the formation of Fe(IV) and Fe(V). Considering the structural similarity of peroxymonosulfate (PMS) and peroxydisulfate (PDS) with HO as well as their universality in water pollutant remediation, the oxidation properties and reactive oxidants of Fe(VI)-PMS and Fe(VI)-PDS processes were also examined. Besides, the Fe(VI)-HO system suffered from less restriction by inorganic ions and natural organic matter, and exhibited satisfactory pollutant removal effects in real water. Overall, this work provides a further and comprehensive cognition about the role of HO in Fe(VI) and Fe(VI)-HO systems.

摘要

最近,一些研究已经意识到过氧化氢(HO)作为高铁酸盐(Fe(VI))的自分解产物对 Fe(VI)氧化污染物的促进作用,但关键的激活机制尚未得到彻底评估。本工作旨在比较和揭示 HO 在 Fe(VI)和 Fe(VI)-HO 过程中的促进机制,并阐明 Fe(VI)-HO 系统的实际应用潜力。大量证据排除了 OH 和 O 在 Fe(VI)和 Fe(VI)-HO 体系中参与污染物降解的可能性,这意味着高剂量的 HO 不能引发不同于原位 HO 的激活途径。Fe(VI)-HO 体系的氧化性能优于单独的 Fe(VI)归因于原位和异位 HO 的催化作用,它们可以直接和/或间接促进 Fe(IV)和 Fe(V)的形成。考虑到过一硫酸盐(PMS)和过二硫酸盐(PDS)与 HO 的结构相似性以及它们在水污染修复中的普遍性,还考察了 Fe(VI)-PMS 和 Fe(VI)-PDS 过程的氧化性质和反应性氧化剂。此外,Fe(VI)-HO 体系受无机离子和天然有机物的限制较小,在实际水中表现出令人满意的污染物去除效果。总的来说,这项工作提供了对 HO 在 Fe(VI)和 Fe(VI)-HO 体系中的作用的进一步和全面的认识。

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