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过氧乙酸与零价铁联用去除四环素:四环素与 Fe(II) 络合的作用。

Activation of peracetic acid with zero-valent iron for tetracycline abatement: The role of Fe(II) complexation with tetracycline.

机构信息

Department of Environment Science & Engineering, College of Chemical Engineering, Huaqiao University, Xiamen, Fujian 361021, China.

Department of Environment Science & Engineering, College of Chemical Engineering, Huaqiao University, Xiamen, Fujian 361021, China.

出版信息

J Hazard Mater. 2022 Feb 15;424(Pt D):127653. doi: 10.1016/j.jhazmat.2021.127653. Epub 2021 Nov 1.

Abstract

Peracetic acid (PAA) is an excellent oxidant that can produce multiple carbon-centered radicals (R•C). A novel advanced oxidation process (AOP) that combines PAA and nanoscale zero-valent iron (i.e. nZVI/PAA) is constructed to evaluate its performance toward tetracycline (TC) abatement. The nZVI/PAA process shows excellent abatement efficacy for TC in the pH range of 3.5-7.5. The presence of humic acid, HPO and HCO exerts inhibitory effects on TC abatement, while the presence of Cl displays negligible influence in the nZVI/PAA process. Nanoscale zero-valent iron (nZVI) exhibits excellent reusability with no apparent variation in crystallinity. CHC(O)OO• is the predominant active radical that contributes to TC abatement, in which leakage of Fe(II) from the nZVI surface is crucial for a radical generation. Due to the strong complexation tendency of TC towards Fe(II), the Fe(II)-TC complexes are formed, which significantly accelerates the PAA decomposition and TC abatement compared to free Fe(II). In addition, the degradation intermediates of TC are identified, and a possible degradation pathway is proposed. These results will be useful for the application of PAA-based AOPs in the treatment of water containing organic micropollutants.

摘要

过氧乙酸(PAA)是一种出色的氧化剂,可以产生多个碳中心自由基(R•C)。构建了一种将过氧乙酸和纳米零价铁(即 nZVI/PAA)结合的新型高级氧化工艺(AOP),以评估其对四环素(TC)去除的性能。nZVI/PAA 工艺在 pH 值为 3.5-7.5 的范围内对 TC 具有优异的去除效果。腐殖酸、HPO 和 HCO 的存在对 TC 的去除具有抑制作用,而 Cl 的存在在 nZVI/PAA 工艺中几乎没有影响。纳米零价铁(nZVI)表现出优异的可重复使用性,其结晶度没有明显变化。CHC(O)OO•是主要的活性自由基,有助于 TC 的去除,其中 nZVI 表面的 Fe(II)泄漏对于自由基的产生至关重要。由于 TC 与 Fe(II)之间的强络合倾向,形成了 Fe(II)-TC 配合物,与游离的 Fe(II)相比,它显著加速了 PAA 的分解和 TC 的去除。此外,鉴定了 TC 的降解中间产物,并提出了可能的降解途径。这些结果将有助于基于 PAA 的 AOP 在处理含有有机微量污染物的水中的应用。

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