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Fenton 降解法在 Al、Fe-柱撑黏土存在下对磺胺甲恶唑的降解:催化行为及中间产物的鉴定。

Fenton degradation of sulfanilamide in the presence of Al,Fe-pillared clay: Catalytic behavior and identification of the intermediates.

机构信息

Baikal Institute of Nature Management SB RAS, Str. Sakh'yanova 8, 670047 Ulan-Ude, Russian Federation; Buryat State University, Str. Smolina 24a, 670000 Ulan-Ude, Russian Federation.

Baikal Institute of Nature Management SB RAS, Str. Sakh'yanova 8, 670047 Ulan-Ude, Russian Federation.

出版信息

J Hazard Mater. 2015 Aug 15;293:21-9. doi: 10.1016/j.jhazmat.2015.03.038. Epub 2015 Mar 19.

Abstract

Liquid phase catalytic degradation of sulfanilamide with H2O2 was carried out in the presence of Fe,Al/M-pillared clay (Fe,Al/M-MM, M=Na(+), Ca(2+) and Ba(2+)) as heterogeneous Fenton type catalyst. Fe,Al/M-MMs were prepared by swelling of layered aluminosilicate (90-95 wt.% montmorillonite) from a bed located in Mukhortala (Buryatia, Russia) in Na(+), Ca(2+) and Ba(2+) forms by means of the exchange of these cations with bulky Fe,Al-polyoxocations prepared at Al/Fe=10/1 and OH/(Al+Fe)=2.0, and then calcinated at 500°C. XRD method and chemical analysis demonstrated that the rate of crystalline swelling was dependent on the interlayer cations and decreased in the order: Fe,Al-/Na-MM>Fe,Al/Ca-MM>Fe,Al/Ba-MM. It was found that the catalytic properties of Fe,Al/M-MMs depended on the type of exchangeable cations. The effect of the H2O2/sulfanilamide molar ratio, the catalyst content, the reaction temperature and the reaction pH on the removal rate of sulfanilamide has been studied in the presence of Fe,Al/Na-MM. The catalyst can be applied for degradation of sulfanilamide with H2O2 for at least three successive cycles without loss of activity. HPLC analyses pointed out that the main degradation intermediate products were sulfanilic acid, benzenesulfonic acid, p-benzoquinone and aliphatic carboxylic acids.

摘要

在 Fe、Al/M-柱撑粘土(Fe、Al/M-MM,M=Na(+)、Ca(2+)和 Ba(2+))存在下,用 H2O2 进行磺胺的液相催化降解,作为非均相 Fenton 型催化剂。Fe、Al/M-MMs 通过用大体积的 Fe、Al-聚氧阳离子交换来自 Mukhortala(俄罗斯布里亚特)床层的层状铝硅酸盐(90-95wt.%蒙脱石),在 Al/Fe=10/1 和 OH/(Al+Fe)=2.0 的条件下,得到 Na(+)、Ca(2+)和 Ba(2+)形式,然后在 500°C 下煅烧,制备得到。XRD 方法和化学分析表明,结晶膨胀率取决于层间阳离子,并按以下顺序降低:Fe、Al-/Na-MM>Fe、Al/Ca-MM>Fe、Al/Ba-MM。研究了在 Fe、Al/Na-MM 存在下,H2O2/磺胺摩尔比、催化剂含量、反应温度和反应 pH 对磺胺去除率的影响。该催化剂可用于至少三个连续循环的 H2O2 降解磺胺,活性无损失。HPLC 分析指出,主要的降解中间产物是磺胺、苯磺酸、对苯醌和脂肪族羧酸。

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