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热激活过硫酸盐氧化过程中溴化物的转化。

Transformation of bromide in thermo activated persulfate oxidation processes.

机构信息

Department of Environmental Science and Engineering, Nanjing Agricultural University, Nanjing, 210095, China.

Department of Environmental Science and Engineering, Nanjing Agricultural University, Nanjing, 210095, China.

出版信息

Water Res. 2015 Jul 1;78:1-8. doi: 10.1016/j.watres.2015.03.028. Epub 2015 Apr 8.

DOI:10.1016/j.watres.2015.03.028
PMID:25898247
Abstract

Sulfate radicals ( [Formula: see text] ) are applied to degrade various organic pollutants. Due to its high oxidative potential, [Formula: see text] is presumed to be able to transform bromide to reactive bromine species that can react with natural organic matter subsequently to form brominated products including brominated disinfection by-products (Br-DBPs). This research was designed to investigate the transformation of bromide in thermo activated persulfate oxidation process in the presence of humic acid (HA). Significant formation of bromoform and bromoacetic acids was verified. Their formation was attributed to the reactions of HA and reactive bromine species including Br·, [Formula: see text] HOBr(-), and free bromine resulted from the oxidation of bromide by [Formula: see text] . Yields of Br-DBPs increased monotonically at persulfate concentration of 1.0 mM and working temperature of 70 °C. However, the time-depended formation exhibited an increasing and the decreasing profile when persulfate was 5.0 mM, suggesting further degradation of organic bromine. HPLC/ICP-MS analysis demonstrated that the organic bromine was eventually transformed to bromate at this condition. Thus, a transformation scheme was proposed in which the bromine could be recycled multiple times between inorganic bromide and organic bromine before being finally transformed to bromate. This is the first study that reveals the comprehensive transformation map of bromine in [Formula: see text] based reaction systems, which should be taken into consideration when such technologies are used to eliminate contamination in real practice.

摘要

硫酸根自由基 ([Formula: see text]) 被应用于降解各种有机污染物。由于其具有较高的氧化能力,[Formula: see text] 被认为能够将溴化物转化为活性溴物种,这些活性溴物种随后可以与天然有机物反应,形成溴化产物,包括溴化消毒副产物 (Br-DBPs)。本研究旨在研究在腐殖酸 (HA) 存在的情况下,热活化过硫酸盐氧化过程中溴化物的转化。验证了溴仿和溴乙酸的显著形成。它们的形成归因于 HA 和包括 Br·、[Formula: see text] HOBr(-) 和由 [Formula: see text] 氧化溴化物产生的游离溴在内的活性溴物种之间的反应。在过硫酸盐浓度为 1.0 mM 和工作温度为 70°C 的条件下,Br-DBPs 的产率单调增加。然而,当过硫酸盐为 5.0 mM 时,时间依赖性形成呈现出增加和减少的趋势,表明有机溴的进一步降解。HPLC/ICP-MS 分析表明,在这种条件下,有机溴最终转化为溴酸盐。因此,提出了一个转化方案,其中溴可以在无机溴和有机溴之间多次循环,然后最终转化为溴酸盐。这是首次揭示 [Formula: see text] 基反应体系中溴的全面转化图的研究,在实际应用中消除污染时应考虑到这一点。

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引用本文的文献

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Thermoactivated persulfate oxidation of pesticide chlorpyrifos in aquatic system: kinetic and mechanistic investigations.水生系统中热活化过硫酸盐氧化农药毒死蜱的动力学和机理研究。
Environ Sci Pollut Res Int. 2017 Apr;24(12):11549-11558. doi: 10.1007/s11356-017-8672-7. Epub 2017 Mar 20.