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在有氧条件下,Fe(II)和多金属氧酸盐(POM)修饰的零价铝(ZVAl)对亚砷酸盐的氧化去除。

Oxidative removal of arsenite by Fe(II)- and polyoxometalate (POM)-amended zero-valent aluminum (ZVAl) under oxic conditions.

机构信息

Department of Soil & Environmental Sciences, National Chung Hsing University, 250 Kuo-Kuang Rd., Taichung 40227, Taiwan, ROC.

出版信息

Water Res. 2013 May 1;47(7):2583-91. doi: 10.1016/j.watres.2013.02.024. Epub 2013 Feb 26.

Abstract

Abiotic transformation of As(III) to As(V) is possible which would decrease As toxicity. This study investigated the potential applications of zero-valent Al (ZVAl) or Al wastes, such as Al beverage cans, for converting As(III) to As(V) in an acidic solution under aerobic conditions. Results showed that As(III) could not be oxidized by ZVAl within 150 min reaction at pH 1 because of the presence of an oxide layer on ZVAl. However, 85 μM As(III) could be completely oxidized with the addition of Fe(II) or POM due to the generation of a Fenton reaction or the enhancement of H2O2 production, respectively, on the ZVAl surfaces. Because Fe(II) or polyoxometalate (POM) exhibited more stable at low pH and scavenged rapidly the H2O2 produced on the aerated ZVAl surfaces, OH radical productions were more efficient and As(III) was rapidly oxidized in the ZVAl/O2 system with theses two catalysts. The catalytic oxidation kinetics of As(III) in the presence of Fe(II) or POM were best described by zero-order reaction, and the rate constants increased with a decrease of pH from 2 to 1. Following the oxidative conversion of As(III) to As(V) in the ZVAl/Fe/O2 system, As(V) was removed by the newly formed hydrous Al/Fe precipitates by increasing the solution pH to 6. Nonetheless, the As(V) removal was incomplete in the ZVAl/POM/O2 system because the hydrolyzed products of POM, e.g., PO4(3-), inhibited As(V) removal due to the competitive adsorption of the oxyanion on Al precipitates. Discarded Al-based beverage cans exhibit a higher efficiency for As(III) oxidation and final As removal compared with that of ZVAl, and thus, the potential application of Al beverage cans to scavenge As in solutions is feasible.

摘要

砷(III)可能会发生非生物转化为砷(V),从而降低砷的毒性。本研究探讨了零价铝(ZVAl)或铝废料(如铝饮料罐)在有氧条件下将砷(III)转化为砷(V)在酸性溶液中的潜在应用。结果表明,由于 ZVAl 表面存在氧化物层,在 pH 值为 1 时,ZVAl 在 150 分钟的反应内不能将砷(III)氧化。然而,由于 Fenton 反应或分别在 ZVAl 表面上增强了 H2O2 的产生,添加 Fe(II) 或 POM 可以将 85 μM 的砷(III)完全氧化。由于 Fe(II) 或多金属氧酸盐(POM)在低 pH 值下更稳定,并且迅速清除有氧 ZVAl 表面上产生的 H2O2,因此在这些两种催化剂存在下,OH 自由基的产生更有效,并且在 ZVAl/O2 体系中砷(III)被迅速氧化。在 Fe(II) 或 POM 存在下,As(III)的催化氧化动力学最好用零级反应来描述,并且随着 pH 值从 2 降至 1,速率常数增加。在 ZVAl/Fe/O2 体系中将 As(III)氧化为 As(V)之后,通过将溶液 pH 值提高到 6,新形成的水合 Al/Fe 沉淀物去除了 As(V)。然而,在 ZVAl/POM/O2 体系中,由于 POM 的水解产物(例如,PO4(3-))由于阴离子在 Al 沉淀物上的竞争吸附而抑制了 As(V)的去除,因此 As(V)的去除并不完全。废弃的含铝饮料罐与 ZVAl 相比,对 As(III)氧化和最终 As 去除具有更高的效率,因此,将含铝饮料罐应用于溶液中去除 As 是可行的。

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