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亚铁(III)在酸性和近中性 pH 条件下通过生物电能激活过硫酸盐:均相机制与非均相机制。

Persulfate activation by Fe(III) with bioelectricity at acidic and near-neutral pH regimes: Homogeneous versus heterogeneous mechanism.

机构信息

Department of Environmental Science and Engineering, Hubei Environmental Remediation Material Engineering Technology Research Center, Wuhan University, Wuhan 430079, China; Hubei Key Laboratory of Pollutant Analysis & Reuse Technology, Department of Environmental Engineering, Hubei Normal University, Huangshi 435002, China.

Hubei Key Laboratory of Pollutant Analysis & Reuse Technology, Department of Environmental Engineering, Hubei Normal University, Huangshi 435002, China.

出版信息

J Hazard Mater. 2019 Jul 15;374:92-100. doi: 10.1016/j.jhazmat.2019.03.068. Epub 2019 Apr 2.

DOI:10.1016/j.jhazmat.2019.03.068
PMID:30981017
Abstract

The combination of persulfate (PS) activation by iron ions with electrochemical process (electro/Fe/PS) is a promising advanced oxidation process. However, almost all these systems were performed in an unbuffered solution and actually under acidic pH condition, with the electricity being frequently supplied by external power. Considering the high buffering capacity of wastewater and energy saving, peroxydisulfate (PDS) activation by Fe(III) species with bioelectricity provided by microbial fuel cell (MFC) for bisphenol A (BPA) oxidation was investigated at fixed near-neutral pH as well as acidic pH. The results indicate that 90.8% of BPA could be removed at pH 2.5. Though the iron existed in the form of precipitate, BPA could still be efficiently removed at pH 6.0. The precipitate formed in the system at pH 6.0 was identified as the amorphous iron oxyhydroxides. Sulfate radicals in the bulk solution and that adsorbed on the precipitate were the dominant reactive species responsible for the oxidation of BPA in the homogeneous and heterogeneous MFC/Fe(III)/PDS processes, respectively. The mechanisms of BPA degradation at both pH values were proposed via EPR and quenching tests as well as XPS analysis. The effects of operating parameters, the mineralization, the mineralization current efficiency and energy consumption were also explored.

摘要

过硫酸盐(PS)与铁离子联合电化学法(电/Fenton/PS)是一种很有前途的高级氧化技术。然而,几乎所有这些系统都是在未缓冲溶液中进行的,实际上处于酸性 pH 条件下,并且经常通过外部电源供电。考虑到废水的高缓冲能力和节能,本研究利用微生物燃料电池(MFC)提供的生物电能,以固定的近中性 pH 和酸性 pH 条件下,研究了三价铁(Fe(III))激活过二硫酸盐(PDS)用于双酚 A(BPA)氧化的反应。结果表明,在 pH 值为 2.5 时,90.8%的 BPA 可以被去除。尽管铁以沉淀物的形式存在,但在 pH 值为 6.0 时,BPA 仍能被有效地去除。在 pH 值为 6.0 的系统中形成的沉淀物被确定为无定形铁氢氧化物。在均相和非均相 MFC/Fe(III)/PDS 过程中,溶液中的硫酸根自由基和吸附在沉淀物上的硫酸根自由基是氧化 BPA 的主要活性物质。通过 EPR 和猝灭实验以及 XPS 分析提出了在这两种 pH 值条件下 BPA 降解的机制。还探讨了操作参数、矿化度、矿化电流效率和能耗的影响。

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