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地下水氯苯降解性能研究:过硫酸氢钾、纳米过氧化钙和过碳酸钠在二价铁激活下的比较。

The performance of chlorobenzene degradation in groundwater: comparison of hydrogen peroxide, nanoscale calcium peroxide and sodium percarbonate activated with ferrous iron.

机构信息

State Environmental Protection Key Laboratory of Environmental Risk Assessment and Control on Chemical Process, East China University of Science and Technology, Shanghai 200237, China E-mail:

Shanghai Urban Construction Design & Research Institute (Group) Co., Ltd, 3447 Dongfang Road, Shanghai 200125, China.

出版信息

Water Sci Technol. 2021 Jan;83(2):344-357. doi: 10.2166/wst.2020.587.

Abstract

The chlorobenzene (CB) degradation performances by various oxidants, including hydrogen peroxide (HO), nanoscale calcium peroxide (nCaO) and sodium percarbonate (SPC), activated with ferrous iron (Fe(II)) were investigated and thoroughly compared. The results showed that all tested systems had strong abilities to degrade CB. The CB removal rate increased with increasing dosages of oxidants or Fe(II) because the generation of reactive oxygen species could be promoted with the chemical dosages' increase. Response surface and contour plots showed that CB could achieve a better removal performance at the same HO and Fe(II) molar content, but the Fe(II) dosage was higher than that of oxidants in the nCaO and SPC systems. The optimal molar ratios of HO/Fe(II)/CB, nCaO/Fe(II)/CB and SPC /Fe(II)/CB were 5.2/7.6/1, 8/8/1, and 4.5/8/1, respectively, in which 98.1%, 98%, and 96.4% CB removals could be obtained in 30 min reaction. The optimal pH condition was around 3, while CB removal rates were less than 20% in all three systems when the initial pH was adjusted to 9. The oxidative hydroxyl radicals (HO•) and singlet oxygen (O) had been detected by the electron paramagnetic resonance test. Based upon the results of liquid chromatograph-mass spectrometer analysis, the pathways of CB degradation were proposed, in which O roles were elaborated innovatively in the CB degradation mechanism. The CB degradation performance was significantly affected in actual groundwater, while increasing the molar ratio of oxidant/Fe(II)/CB was an effective way to overcome the adverse effects caused by the complex of actual groundwater matrix.

摘要

研究了各种氧化剂(包括过氧化氢(HO)、纳米过氧化钙(nCaO)和过碳酸钠(SPC))在亚铁离子(Fe(II))活化下对氯苯(CB)的降解性能,并进行了彻底比较。结果表明,所有测试系统都具有很强的降解 CB 的能力。随着氧化剂或 Fe(II)用量的增加,CB 的去除率增加,因为可以通过化学剂量的增加来促进活性氧物质的生成。响应面和等高线图表明,在相同的 HO 和 Fe(II)摩尔含量下,CB 可以达到更好的去除效果,但在 nCaO 和 SPC 系统中,Fe(II)的用量高于氧化剂。HO/Fe(II)/CB、nCaO/Fe(II)/CB 和 SPC/Fe(II)/CB 的最佳摩尔比分别为 5.2/7.6/1、8/8/1 和 4.5/8/1,在 30 min 反应中可分别获得 98.1%、98%和 96.4%的 CB 去除率。最佳 pH 值条件约为 3,而在三种系统中,当初始 pH 值调至 9 时,CB 的去除率均小于 20%。通过电子顺磁共振测试检测到了氧化羟基自由基(HO•)和单线态氧(O)。根据液相色谱-质谱分析的结果,提出了 CB 降解的途径,创新性地阐述了 O 在 CB 降解机制中的作用。实际地下水对 CB 降解性能有显著影响,增加氧化剂/Fe(II)/CB 的摩尔比是克服实际地下水基质复杂引起的不利影响的有效方法。

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