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Degradation of roxarsone in a sulfate radical mediated oxidation process and formation of polynitrated by-products

机译:硫酸盐自由基介导的氧化工艺中罗克斯松的降解及聚硝基 - 产物的形成

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Organoarsenicals such as roxarsone (ROX) are extensively utilized in the poultry industry, and land application of poultry litter is an important route by which arsenics are introduced into the environment. In the present study, degradation of ROX and structurally related nitrophenols by a heat activated persulfate (PS) oxidation process, one in situ chemical oxidation process (ISCO), was systematically explored. The effects of temperature, PS dosage, pH and natural water constituents ( i.e. , fulvic acid, Cl ~(?) ) on the degradation of ROX were investigated. Products analysis by solid phase extraction (SPE) and liquid chromatography-electrospray ionization-triple quadrupole mass spectrometry (LC-ESI-MS/MS) revealed that 2,4-dinitrophenol (2,4-DNP) and 2,4,6-trinitrophenol (2,4,6-TNP) were generated as major intermediate products, suggesting denitration–renitration process occurred during SO _(4) ˙ ~(?) -based oxidation of ROX. Interestingly, the formation of polynitration by-products was further confirmed in heat activated persulfate oxidation of nitrophenols. Formation of inorganic arsenics during ROX degradation was measured by inductively coupled plasma-mass spectrometry (ICP-MS). It was evident that the arsenic substituent of ROX was converted to As( V ). On the basis of the intermediate products identified, detailed mechanisms and transformation pathways for ROX oxidation were proposed. Results manifest that heat activated PS oxidation could be an efficient approach to treat ROX contamination. However, post-treatment is necessary for complete removal of As( V ) to minimize ecotoxicological risks.
机译:罗克斯松(ROX)如罗克斯松(ROX)的有机躯在家禽业中广泛使用,禽类垃圾的土地应用是砷引入环境的重要路径。在本研究中,系统地探索了通过热活化过硫酸盐(PS)氧化方法的ROX和结构相关硝基苯酚的降解,一种原位化学氧化过程(ISCO),是一种原位化学氧化过程。研究了温度,PS剂量,pH和天然水成分的影响(即,富发酸,Cl〜(α))对ROX降解的影响。通过固相萃取(SPE)和液相色谱 - 电喷雾电离 - 三重四极杆质谱(LC-ESI-MS / MS)的产品分析显示,2,4-二硝基苯酚(2,4-DNP)和2,4,6-产生三氯苯酚(2,4,6-TNP)作为主要中间产物产生,表明在α(4)℃氧化氧化过程中发生脱硝丙戊化过程。有趣的是,在热活化的过硫酸盐氧化中进一步证实了多硝化副产物的形成。通过电感耦合等离子体质谱(ICP-MS)测量ROX降解期间的无机砷的形成。显然,ROX的砷取代基转化为(v)。在鉴定的中间产物的基础上,提出了对ROX氧化的详细机制和转化途径。结果表明,热活化的PS氧化可能是治疗ROX污染的有效方法。然而,后处理是必要的,以完全去除(v)以最大限度地减少生态毒理学风险。

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