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富里酸增强Fe(II)/过一硫酸盐对邻苯二甲酸二甲酯的降解:效率及可能机制

Degradation of dimethyl phthalate through Fe(II)/peroxymonosulphate heightened by fulvic acid: efficiency and possible mechanism.

作者信息

Ding Yi, Zhang Min, Zhou Sijie, Xie Linbei, Li Ao, Wang Ping

机构信息

College of Biology and the Environment, Nanjing Forestry University, Nanjing, People's Republic of China.

出版信息

Environ Technol. 2023 May;44(12):1850-1862. doi: 10.1080/09593330.2021.2014576. Epub 2022 Feb 3.

Abstract

Ferrous iron (Fe(II)) reacts with peroxymonosulphate (PMS) to form active oxidants that can degrade refractory organic pollutants. However, the conversion rate of Fe(III) to Fe(II) is slow, which limits its actual application. In the study, the effect of fulvic acid (FA) on the degradation of dimethyl phthalate (DMP) by Fe(II)/PMS was investigated. Moreover, the degradation process of DMP was predicted by the preliminary identification of active free radicals and intermediates. As expected, FA gave rise to a higher concentration of Fe(II) than that in Fe(II)/PMS to enhance the removal of DMP in Fe(II)/PMS system. The precipitate, involved in FA and iron, was an important composite to promote the degradation of DMP in the system. Also, the response surface methodology (RSM) was applied to model and optimize the degradation conditions of DMP. The highest removal efficiency (85.70%) was obtained at pH = 3.86, [PMS] = 0.96 mM, [FA] = 11.44 mg/L and [DMP] = 5 µM. The results of free radical quenching experiments and EPR showed that •OH and SO were the main active radicals in this system. The degradation intermediates of DMP were monomethyl phthalate (MMP), phthalic acid and benzoic acid. Discoveries of this study had raised the current understanding of the application of FA keeping the cycles of Fe(II)/Fe(III) for peroxymonosulphate activation, which could afford valuable information for the degradation of organic pollutants by FA/Fe(II)/PMS.

摘要

亚铁离子(Fe(II))与过一硫酸盐(PMS)反应生成活性氧化剂,可降解难降解有机污染物。然而,Fe(III)向Fe(II)的转化率较低,限制了其实际应用。本研究考察了富里酸(FA)对Fe(II)/PMS降解邻苯二甲酸二甲酯(DMP)的影响。此外,通过对活性自由基和中间体的初步鉴定,预测了DMP的降解过程。正如预期的那样,FA产生的Fe(II)浓度高于Fe(II)/PMS体系,从而提高了Fe(II)/PMS体系中DMP的去除率。FA与铁形成的沉淀物是促进体系中DMP降解的重要复合物。同时,应用响应面法(RSM)对DMP的降解条件进行建模和优化。在pH = 3.86、[PMS]=0.96 mM、[FA]=11.44 mg/L和[DMP]=5 μM时,去除效率最高(85.70%)。自由基淬灭实验和电子顺磁共振结果表明,•OH和SO是该体系中的主要活性自由基。DMP的降解中间体为邻苯二甲酸单甲酯(MMP)、邻苯二甲酸和苯甲酸。本研究的发现加深了目前对FA在过一硫酸盐活化中维持Fe(II)/Fe(III)循环应用的理解,可为FA/Fe(II)/PMS降解有机污染物提供有价值的数据。

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