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铁(III)催化过碳酸钠氧化苯:基质成分的影响及降解途径

Benzene oxidation by Fe(III)-catalyzed sodium percarbonate: matrix constituent effects and degradation pathways.

作者信息

Fu Xiaori, Gu Xiaogang, Lu Shuguang, Sharma Virender K, Brusseau Mark L, Xue Yunfei, Danish Muhammad, Fu George Y, Qiu Zhaofu, Sui Qian

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.

Department of Environmental and Occupational Health, School of Public Health, Texas A&M University, 1266 TAMU, College Station, Texas 77843, USA.

出版信息

Chem Eng J. 2017 Feb 1;309:22-29. doi: 10.1016/j.cej.2016.10.006. Epub 2016 Oct 6.

Abstract

Complete degradation of benzene by the Fe(III)-activated sodium percarbonate (SPC) system is demonstrated. Removal of benzene at 1.0 mM was seen within 160 min, depending on the molar ratios of SPC to Fe(III). A mechanism of benzene degradation was elaborated by free-radical probe-compound tests, free-radical scavengers tests, electron paramagnetic resonance (EPR) analysis, and determination of Fe(II) and H2O2 concentrations. The degradation products were also identified using gas chromatography-mass spectrometry method. The hydroxyl radical (HO.) was the leading species in charge of benzene degradation. The formation of HO. was strongly dependent on the generation of the organic compound radical (R.) and superoxide anion radical (O.). Benzene degradation products included hydroxylated derivatives of benzene (phenol, hydroquinone, benzoquinone, and catechol) and aliphatic acids (oxalic and fumaric acids). The proposed degradation pathways are consistent with radical formation and identified products. The investigation of selected matrix constituents showed that the Cl and HCO had inhibitory effects on benzene degradation. Natural organic matter (NOM) had accelerating influence in degrading benzene. The developed system was tested with groundwater samples and it was found that the Fe(III)-activated SPC has a great potential in effective remediation of benzene-contaminated groundwater while more further studies should be done for its practical application in the future because of the complex subsurface environment.

摘要

研究表明,铁(III)活化过碳酸钠(SPC)体系可实现苯的完全降解。根据SPC与铁(III)的摩尔比,1.0 mM的苯在160分钟内被去除。通过自由基探针化合物试验、自由基清除剂试验、电子顺磁共振(EPR)分析以及铁(II)和过氧化氢浓度的测定,阐述了苯的降解机制。还采用气相色谱 - 质谱法鉴定了降解产物。羟基自由基(HO·)是负责苯降解的主要物种。HO·的形成强烈依赖于有机化合物自由基(R·)和超氧阴离子自由基(O·)的产生。苯的降解产物包括苯的羟基化衍生物(苯酚、对苯二酚、苯醌和邻苯二酚)和脂肪酸(草酸和富马酸)。所提出的降解途径与自由基形成和鉴定出的产物一致。对选定基质成分的研究表明,Cl和HCO对苯的降解有抑制作用。天然有机物(NOM)对苯的降解有促进作用。用地下水样品对所开发的体系进行了测试,发现铁(III)活化的SPC在有效修复受苯污染的地下水方面具有很大潜力,但由于地下环境复杂,未来在其实际应用方面还需进行更多深入研究。

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