水环境中ZVI/氧化剂体系及其电子迁移作用机制

杨世迎; 任腾飞; 张艺萱; 郑迪; 辛佳

doi:10.7536/PC170133

化学进展 ›› 2017, Vol. 29 ›› Issue (4) :388-399 DOI: 10.7536/PC170133

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水环境中ZVI/氧化剂体系及其电子迁移作用机制

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ZVI/Oxidant Systems Applied in Water Environment and Their Electron Transfer Mechanisms

Shiying Yang^1,2,3*, Tengfei Ren^1,3, Yixuan Zhang³, Di Zheng³, Jia Xin^1,3

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摘要

利用零价铁（Zero-Valent Iron，ZVI）去除水环境中的污染物成为近年来的研究热点。当O₂、H₂O₂等氧化剂存在时，ZVI、氧化剂与污染物之间的电子迁移机制非常复杂，ZVI和氧化剂之间的相互影响机制尚无定论。传统观点认为，O₂会促进ZVI钝化膜的形成并阻断电子传递从而降低ZVI的还原性能。然而O₂可在ZVI作用下通过双电子传输转化为H₂O₂，构成ZVI/O₂类Fenton体系；在此基础上，利用额外加入H₂O₂、HSO₅^-、S₂O₈^2-等氧化剂，发展出了基于·OH或SO₄^·-的ZVI/氧化剂高级氧化体系（ZVI-AOPs），从而氧化降解有机污染物。有学者认为H₂O₂、KMnO₄、S₂O₈^2-等强氧化剂的加入反而可以加快ZVI腐蚀和失电子的速率，从而提高ZVI去除重金属等污染物的还原性能，该研究结论对钝化膜机制提出了挑战。ZVI与氧化剂的联合作用还可以实现同时还原去除重金属和氧化降解有机物，也可以对卤代有机物等抗氧化污染物实现先还原后氧化去除。本文综述了基于ZVI/氧化剂的高级氧化或还原体系及其电子迁移机制，同时对ZVI与氧化剂的联合作用体系作一总结，并就值得深入研究的问题进行了展望。

Abstract

In recent years, the use of zero-valent iron (ZVI) for treatment of toxic contaminants in water system has been widely investigated. In the presence of oxidant, such as oxygen (O₂) or hydrogen peroxide (H₂O₂), the electron transfer processes among ZVI, oxidants and contaminants are extremely complex, and the interaction mechanisms between ZVI and oxidants are still inconclusive. Generally speaking, O₂ can promote the formation of iron oxide layer via corrosion of ZVI by water and oxygen, which may block the outward electron transfer and then decrease the reductive ability of ZVI. However, O₂ could be activated via two-electron reduction pathway to produce H₂O₂, thereby forming ZVI/O₂ Fenton-like system. Based on this, the extra addition of H₂O₂, peroxymonosulfate (HSO₅^-) or persulfate (S₂O₈^2-) can react with ZVI and the generated Fe²⁺ and then produce strong oxidizing hydroxyl radicals (·OH) and sulfate radicals (SO₄^·-), which can efficiently degrade organic contaminants through advanced oxidation processes (ZVI-AOPs). Otherwise, some researchers recently propose another critical role of common oxidants in accelerating ZVI corrosion and then hence in facilitating the electron transfer rate and promoting the reductive performance of ZVI. The combination of ZVI and oxidants can not only show significant synergistic degradation between heavy metals and organic contaminants, but also achieve the degradation and mineralization of refractory pollutants through reduction through ZVI firstly and then oxidation through AOPs. This review summarizes the ZVI-AOPs system and ZVI-reduction system based on the interaction between ZVI and oxidants and their electron transfer processes, as well as makes a summary of the associative effect of ZVI and oxidants. At last, the prospects of the research areas meriting further investigation are pointed out.

Contents
1 Introduction
2 Advanced oxidation processes
2.1 ZVI/oxidant advanced oxidation system
2.2 Physically enhanced ZVI/oxidant system
2.3 Chemically enhanced ZVI/oxidant system
3 Reduction processes
3.1 ZVI/O₂ reduction system
3.2 ZVI/H₂O₂ reduction system
3.3 ZVI/PS reduction system
3.4 ZVI/other oxidants reduction system
4 Associative mechanisms of ZVI and oxidants
4.1 Simultaneous removal of combined pollutants
4.2 Removal of refractory pollutants
5 Conclusion

Graphical abstract

关键词

零价铁 / 氧化剂 / 氧化还原 / 电子迁移 / 联合作用 / 水处理

Key words

zero-valent iron(ZVI) / oxidants / oxidation and reduction / electron transfer / combination mechanism / water treatment

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杨世迎, 任腾飞, 张艺萱, 郑迪, 辛佳. 水环境中ZVI/氧化剂体系及其电子迁移作用机制[J]. 化学进展, 2017, 29(4): 388-399 DOI:10.7536/PC170133

Shiying Yang, Tengfei Ren, Yixuan Zhang, Di Zheng, Jia Xin. ZVI/Oxidant Systems Applied in Water Environment and Their Electron Transfer Mechanisms[J]. Progress in Chemistry, 2017, 29(4): 388-399 DOI:10.7536/PC170133

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