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Effect of Structural Transformation of Nanoparticulate Zero-Valent Iron on Generation of Reactive Oxygen Species

机译:纳米零价铁的结构转变对活性氧生成的影响

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摘要

While it has been recognized for some time that addition of nanoparticlate zerovalent iron (nZVI) to oxygen-containing water results in both corrosion of Fe~0 and oxidation of contaminants, there is limited understanding of either the relationship between transformation of nZVI and oxidant formation or the factors controlling the lifetime and extent of oxidant production. Using Fe K-edge extended X-ray absorption fine structure (EXAFS) spectroscopy, we show that while nZVI particles are transformed to ferrihydrite then iepidocrocite in less than 2 h, oxidant generation continues for up to 10 h. The major products (Fe(Ⅱ) and H_2O_2) of the reaction of nZVI with oxygenated water are associated, for the most part, with the surface of particles present with these surface-associated Fenton reagents inducing oxidation of a target compound (in this study, ~(14)C-labeled formate). Effective oxidation of formate only occurred after formation of iron oxides on the nZVI surface with the initial formation of high surface area ferrihydrite facilitating rapid and extensive adsorption of formate with colocation of this target compound and surface-associated Fe(Ⅱ) and H_2O_2 apparently critical to formate oxidation. Ongoing formate oxidation long after nZVI is consumed combined with the relatively slow consumption of Fe(Ⅱ) and H_2O_2 suggest that these reactants are regenerated during the nZVI-initiated heterogeneous Fenton process.
机译:尽管人们已经认识到将纳米粒子零价铁(nZVI)添加到含氧水中会导致Fe〜0的腐蚀和污染物的氧化,但是对于nZVI的转化与氧化剂形成之间的关系的理解仍然有限。或控制氧化剂寿命和程度的因素。使用Fe K边缘扩展X射线吸收精细结构(EXAFS)光谱,我们显示,虽然nZVI粒子在不到2小时的时间内就转化为三水铁矿然后再成为异铁矿,但氧化剂的生成持续长达10小时。 nZVI与含氧水反应的主要产物(Fe(Ⅱ)和H_2O_2)在大多数情况下与这些与表面相关的Fenton试剂诱导目标化合物氧化的颗粒表面有关(在本研究中) ,〜(14)C标记的甲酸酯)。甲酸的有效氧化仅在nZVI表面形成铁氧化物后才发生,而高表面积亚铁水合物的初始形成则促进了甲酸的快速和广泛吸附,并且该目标化合物与表面相关的Fe(Ⅱ)和H_2O_2的共存对甲酸氧化。在nZVI被消耗很长时间之后,正在进行的甲酸盐氧化以及相对缓慢的Fe(Ⅱ)和H_2O_2消耗表明这些反应物是在nZVI引发的非均相Fenton过程中再生的。

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  • 来源
    《Environmental Science & Technology》 |2016年第7期|3820-3828|共9页
  • 作者单位

    School of Civil and Environmental Engineering, University of New South Wales, Sydney, New South Wales 2052, Australia;

    State Key Laboratory of Pollution Control and Resources Reuse, College of Environmental Science and Engineering, Tongji University, Shanghai 200092, People's Republic of China;

    School of Civil and Environmental Engineering, University of New South Wales, Sydney, New South Wales 2052, Australia;

    School of Civil and Environmental Engineering, University of New South Wales, Sydney, New South Wales 2052, Australia;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
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  • 正文语种 eng
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