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Fe-Mn 二元氧化物协同介导的自由基反应增强对磺胺甲恶唑的降解。

Enhanced degradation of sulfamethoxazole by Fe-Mn binary oxide synergetic mediated radical reactions.

机构信息

Anhui Province Key Laboratory of Farmland Ecological Conservation and Pollution Prevention, School of Resources and Environment, Anhui Agricultural University, Hefei, 230036, China.

出版信息

Environ Sci Pollut Res Int. 2019 May;26(14):14350-14361. doi: 10.1007/s11356-019-04710-4. Epub 2019 Mar 13.

Abstract

In this study, a novel Fe-Mn binary oxide (FMBO), which combined the oxidation capability of iron and manganese oxides, was constructed to remove sulfamethoxazole (SMX) effectively using the simultaneous co-precipitation and oxidation methods, and the reaction products were probed by liquid chromatography-mass spectrometry (LC/MS). Particularly, FMBO-mediated transformation mechanisms of SMX were explored using radical scavengers and electron paramagnetic resonance (EPR). Results indicated that the best removal efficiency was obtained at a pH of 4.0, with the HO of 6.0 mmol/L and the FMBO dosage of 2.0 g/L, giving 97.6% removal of 10 mg/L SMX within 60 min. More importantly, we found that the hydroxyl (•OH) radicals generated by FMBO through Fenton-like reaction were responsible for the SMX oxidation. EPR studies were confirmed that the peak intensities of hydroxyl adduct decreased remarkably with increasing pH values. Moreover, the four SMX degradation intermediate products were detected by LC/MS and a reaction pathway for the possible mineralization of SMX, with •OH radicals as the main oxidant, was proposed. These findings provide a novel insight into the removal of SMX by FMBO-mediated radical reactions in aquatic environments. Moreover, this research suggested that FMBO can act as an efficient catalyst to remove SMX in hospital wastewater.

摘要

在这项研究中,采用同时共沉淀和氧化法构建了一种新型的 Fe-Mn 二元氧化物(FMBO),该氧化物结合了氧化铁和氧化锰的氧化能力,有效地去除了磺胺甲恶唑(SMX),并通过液相色谱-质谱(LC/MS)对反应产物进行了探测。特别是,通过自由基清除剂和电子顺磁共振(EPR)探索了 FMBO 介导的 SMX 转化机制。结果表明,在 pH 值为 4.0、HO 为 6.0 mmol/L、FMBO 用量为 2.0 g/L 的条件下,去除 10 mg/L SMX 的最佳去除效率为 97.6%,在 60 min 内即可完成。更重要的是,我们发现 FMBO 通过类 Fenton 反应产生的羟基(•OH)自由基是 SMX 氧化的原因。EPR 研究证实,随着 pH 值的增加,羟基加合物的峰强度显著降低。此外,通过 LC/MS 检测到了四个 SMX 降解中间产物,并提出了一种可能的 SMX 矿化反应途径,其中•OH 自由基是主要氧化剂。这些发现为 FMBO 介导的自由基反应在水环境污染中去除 SMX 提供了新的见解。此外,本研究表明 FMBO 可以作为一种有效的催化剂,用于去除医院废水中的 SMX。

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