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锰(IV)氧化物在模型腐殖质成分存在下增强磺胺类抗生素的转化。

Enhanced transformation of sulfonamide antibiotics by manganese(IV) oxide in the presence of model humic constituents.

机构信息

Key Laboratory for Water Quality and Conservation of the Pearl River Delta, Ministry of Education, Institute of Environmental Research at Greater Bay, Guangzhou University, Guangzhou, 510006, China; School of Architecture, Civil and Environmental Engineering (ENAC), École Polytechnique Fédérale de Lausanne (EPFL), CH-1015, Lausanne, Switzerland.

Institute of Environmental and Ecological Engineering, Guangdong University of Technology, Guangzhou, Guangdong, 510006, China.

出版信息

Water Res. 2019 Apr 15;153:200-207. doi: 10.1016/j.watres.2019.01.011. Epub 2019 Jan 21.

DOI:10.1016/j.watres.2019.01.011
PMID:30716563
Abstract

In this study, a manganese(IV) oxide-mediator (MnO-mediator) system for the abatement of sulfonamide antibiotics was evaluated. Two simple model humic constituents, syringaldehyde (SA) and acetosyringone (AS), could promote the transformation of sulfonamides at pH 5-8. Two additional potential mediators, tannic acid and 2,2'-azino-bis(3-ethylbenzothiazoline)-6-sulfonate (ABTS), had negligible enhancement on the transformation of sulfonamides by MnO. The enhancing effect was attributed to the reaction of the oxidized mediator (i.e., phenoxy radical or benzoquinone-like compounds) produced from the oxidation of the mediators by MnO with SMX. Thereby cross-coupling products from sulfamethoxazole (SMX) with oxidized SA were formed in the MnO-SA system, which was confirmed by liquid chromatography/electrospray ionization-triple quadrupole mass spectrometry. Coexisting metal ions (i.e., Ca(II), Mg(II) and Mn(II)) showed inhibitory effects in the order of Mn(II)> Ca(II)> Mg(II). For repetitive runs of the MnO-SA-SMX system, MnO lost its oxidative capacity due to the sorption of Mn(II) on the reactive sites of the MnO surface. A full regeneration of partially deactivated MnO by oxidation of the sorbed Mn(II) with Mn(VII) could be achieved.

摘要

在这项研究中,评估了一种锰(IV)氧化物-介体(MnO 介体)体系来去除磺胺类抗生素。两种简单的模型腐殖质成分,丁香醛(SA)和乙酰丁香酮(AS),可以在 pH 值为 5-8 的条件下促进磺胺类抗生素的转化。另外两种潜在的介体,鞣酸和 2,2'-联氮-双(3-乙基苯并噻唑啉-6-磺酸)(ABTS),对 MnO 转化磺胺类抗生素几乎没有增强作用。这种增强作用归因于介体被 MnO 氧化产生的氧化介体(即酚氧基自由基或苯醌类似物)与 SMX 反应。因此,在 MnO-SA 体系中形成了来自磺胺甲恶唑(SMX)与氧化 SA 的交叉偶联产物,这通过液相色谱/电喷雾电离-三重四极杆质谱得到了证实。共存的金属离子(即 Ca(II)、Mg(II)和 Mn(II))的抑制作用顺序为 Mn(II)>Ca(II)>Mg(II)。对于 MnO-SA-SMX 体系的重复运行,由于 Mn(II)在 MnO 表面的反应性位点上的吸附,MnO 失去了氧化能力。通过用 Mn(VII)氧化吸附的 Mn(II)可以实现部分失活的 MnO 的完全再生。

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