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从粉煤灰中合成纳米零价铁及其在芬顿反应中氧化降解甲基橙的应用。

Novel synthesis of nanoscale zerovalent iron from coal fly ash and its application in oxidative degradation of methyl orange by Fenton reaction.

机构信息

Department of Civil and Environmental Engineering, Konkuk University, 120 Neungdong-ro, Gwangjin-gu, Seoul 05029, Republic of Korea.

Department of Civil and Environmental Engineering, Konkuk University, 120 Neungdong-ro, Gwangjin-gu, Seoul 05029, Republic of Korea.

出版信息

J Hazard Mater. 2019 Mar 5;365:751-758. doi: 10.1016/j.jhazmat.2018.11.073. Epub 2018 Nov 17.

DOI:10.1016/j.jhazmat.2018.11.073
PMID:30476798
Abstract

We firstly developed a novel synthesis method of nanoscale zerovalent iron (NZVI) using Fe sources in coal fly ash (CFA) for the oxidative degradation of methyl orange by Fenton reaction. Hydrochloric acid (HCl) and methyl isobutyl ketone (MIBK) were used for Fe dissolution from CFA and selective Fe(III) chelation, respectively. Among varied HCl concentrations, 7 N HCl showed the best performance for the oxidation of aqueous Fe(II) to Fe(III) and efficient chelation of Fe(III) with MIBK. The NZVI-CFA was synthesized by adding NaBH to a solution of Fe(III)-chelated MIBK, yielding NZVI transformation >95% from Fe(III) in HCl. Various surface analyses were performed to characterize the NZVI-CFA, which was almost identical to typical NZVI-Bare. HCl and MIBK could be reused several times, indicating potential reusability of chemicals used in the synthesis. Remarkable >96% decolorization of methyl orange was obtained by the NZVI-CFA-induced Fenton reaction at pH 3, with a ∼22% decrease in total organic carbon in 7 min. The heterogeneous Fenton reaction initiated by NZVI-CFA with HO showed reactivity similar to that of the homogeneous Fenton reaction (i.e., aqueous Fe(II) with HO), indicating the importance of homogeneous reaction for the oxidative degradation of methyl orange.

摘要

我们首先开发了一种使用粉煤灰(CFA)中的铁源合成纳米零价铁(NZVI)的新方法,用于通过芬顿反应氧化降解甲基橙。盐酸(HCl)和甲基异丁基酮(MIBK)分别用于从 CFA 中溶解 Fe 和选择性螯合 Fe(III)。在各种 HCl 浓度中,7 N HCl 表现出最佳性能,可将水溶液中的 Fe(II)氧化为 Fe(III),并有效螯合 MIBK 中的 Fe(III)。通过向 Fe(III)-螯合 MIBK 的溶液中添加 NaBH,可合成 NZVI-CFA,从而使 HCl 中 Fe(III)转化为 NZVI 的转化率>95%。对 NZVI-CFA 进行了各种表面分析以进行表征,其几乎与典型的 NZVI-Bare 相同。HCl 和 MIBK 可以重复使用几次,表明合成中使用的化学品具有潜在的可重复使用性。在 pH 3 下,NZVI-CFA 引发的芬顿反应可使甲基橙的脱色率达到>96%,7 分钟内总有机碳的含量下降了约 22%。NZVI-CFA 与 HO 引发的非均相芬顿反应的反应性与均相芬顿反应(即水溶液中的 Fe(II)与 HO)相似,表明均相反应对于甲基橙的氧化降解非常重要。

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