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通过 Fe(III)饱和蒙脱石纳米层间限域的 Fe(III)/Fe(II)循环促进过一硫酸盐对微量污染物的催化降解。

Catalytic degradation of micropollutant by peroxymonosulfate activation through Fe(III)/Fe(II) cycle confined in the nanoscale interlayer of Fe(III)-saturated montmorillonite.

机构信息

State Key Laboratory of Urban Water Resource and Environment, Harbin Institute of Technology, Harbin, 150090, China.

School of Environmental and Material Engineering, Yantai University, Yantai, 264005, China.

出版信息

Water Res. 2020 Sep 1;182:116030. doi: 10.1016/j.watres.2020.116030. Epub 2020 Jun 11.

DOI:10.1016/j.watres.2020.116030
PMID:32679388
Abstract

Low cost, green, regenerable catalyst for persulfate activation is the popularly concerned topic for the degradation of persistent organic micropollutants in drinking water. In this work, natural montmorillonite (MMT) saturated with Fe(III) ions was used to activate peroxymonosulfate (PMS) for the degradation of atrazine in raw drinking water. Results showed that the adsorption of atrazine was quickly completed within 1 min and the percentage degradation was finally increased up to 94.1% in 60 min. The d-spacing of MMT was enlarged to 2.91 nm at the most by Fe(III) saturation. Atrazine was adsorbed into the nanoscale interlayer of Fe(III)-saturated montmorillonite (Fe-MMT), where the Fe(III)/Fe(II) cycle was sustainably realized through the accelerated transformation of electrons between Fe(III) and PMS. Meanwhile, the in-situ generated Fe(II) accelerated the decomposition of PMS to further proceed the degradation of atrazine through the oxidation of HO• and SO• radicals. This nanoconfined effect of PMS activation by Fe(III) was further confirmed through the degradation of various micropollutants in the backgrounds of river water. The selective catalytic oxidation of micropollutants through PMS activation was attributed to the 2D mesoporous structure of Fe-MMT, inhibiting the interlayer adsorption of larger molecular backgrounds (humic acids etc.). Fe(III)-saturated montmorillonite (Fe-MMT) provided a feasible and scalable method of PMS activation by Fe(III) for the degradation of micropollutants in drinking water.

摘要

用于过硫酸盐活化的低成本、绿色、可再生催化剂是饮用水中持久性有机微量污染物降解的热门研究课题。在这项工作中,用三价铁离子饱和的天然蒙脱石(MMT)来活化过一硫酸盐(PMS),以降解原水中的莠去津。结果表明,莠去津的吸附在 1 min 内迅速完成,60 min 内最终降解率提高到 94.1%。MMT 的层间距在三价铁饱和时最大扩大到 2.91nm。莠去津被吸附到三价铁饱和蒙脱石(Fe-MMT)的纳米层间,通过 Fe(III)和 PMS 之间电子的加速转化,实现了 Fe(III)/Fe(II)循环的持续进行。同时,原位生成的 Fe(II)加速了 PMS 的分解,通过 HO•和 SO•自由基的氧化进一步促进莠去津的降解。通过在河水背景下对各种微量污染物的降解,进一步证实了 Fe(III)对 PMS 活化的这种纳米限域效应。通过 PMS 活化对微量污染物的选择性催化氧化归因于 Fe-MMT 的二维介孔结构,抑制了较大分子背景(腐殖酸等)的层间吸附。三价铁饱和蒙脱石(Fe-MMT)为饮用水中微量污染物的降解提供了一种可行的、可扩展的三价铁活化过硫酸盐的方法。

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