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Oxidation of PAHs in a simplified system using peroxy-acid and glass beads: Identification of oxidizing species

机译:使用过氧酸和玻璃珠在简化的系统中氧化多环芳烃:鉴定氧化物种

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Polycyclic aromatic hydrocarbons (PAHs) are organic contaminants of concern due to their ubiquity, persistence in the natural environment and adverse health effects. Numerous studies have looked into the removal and treatment of these contaminants, with mixed results. High molecular weight PAHs have been particularly problematic due to their hydrophobicity and high affinity for organics, resulting in mass transfer limitations for even the fastest advanced oxidation processes (AOPs). The peroxy-acid process has been used to successfully treat PAH contaminated matrices. Experiments were conducted on benzo[a]pyrene contaminated glass beads in order to elucidate the reaction mechanisms responsible for the effectiveness of this process. For the first time peracetic acid (PAA) was identified as the important oxidant in this reaction. Different v/v/v ratios of hydrogen peroxide/acetic acid/DI water were studied which illustrated the importance of reaction ratio on oxidant concentration and rate of formation. Approximately 60% degradation of benzo[a]pyrene was achieved in 24 hours with 1.7% PAA. Observations of the reaction kinetics suggest that the slow desorption/dissolution of benzo[a]pyrene limits the efficiency of the peroxy-acid process. Modifications of the reaction setup supported this observation as treatment efficiencies increased with reactive surface area, and an increase in system agitation. These limitations were also overcome by increasing the concentration of PAA delivered to the contaminated matrix. Greater than 80% degradation of benzo[a]pyrene was achieved in 24 hours with approximately 9.2% PAA.
机译:多环芳烃(PAH)是普遍存在的有机污染物,它们在自然环境中持久存在并且对健康造成不利影响。许多研究已经着眼于这些污染物的去除和处理,结果不一。高分子量的PAH由于其疏水性和对有机物的高亲和力而特别成问题,甚至对于最快的高级氧化过程(AOP)都存在传质限制。过氧酸工艺已成功用于处理受PAH污染的基质。在被苯并[a] py污染的玻璃珠上进行实验,以阐明负责该方法有效性的反应机理。过乙酸(PAA)首次被确定为该反应中的重要氧化剂。研究了过氧化氢/乙酸/去离子水的不同v / v / v比,这说明了反应比对氧化剂浓度和形成速率的重要性。用1.7%的PAA在24小时内可降解约60%的苯并[a] re。反应动力学的观察表明,苯并[a]]的缓慢解吸/溶解限制了过氧酸过程的效率。反应设置的修改支持该观察,因为处理效率随反应表面积的增加而增加,并且系统搅动也增加。这些限制还可以通过提高输送到受污染基质中的PAA的浓度来克服。在约24%的PAA浓度下,24小时内苯并[a] py的降解率达到80%以上。

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