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饮用水加氯消毒过程中溴离子对多环芳烃转化影响的研究及应用
Alternative TitleThe study on the impact of bromide ion in transfer mechanism of polycyclic aromatic hydrocarbons during the drinking water chlorination process and application
李强
Subtype硕士
Thesis Advisor王东红
2018-06
Degree Grantor中国科学院生态环境研究中心
Place of Conferral北京
Degree Name工程硕士
Degree Discipline环境工程
Keyword加氯消毒,多环芳烃,反应活性,溴代多环芳烃,转化机理 Chlorine Disinfection, Polycyclic Aromatic Hydrocarbons, Reactivity, Bromo-substituted Polycyclic Aromatic Hydrocarbons, Transformation Mechanism
Abstract

     本论文研究了溴离子对18种多环芳烃(包含8种杂环芳烃)在饮用水加氯消毒过程中转化机理的影响并将研究结果应用于再生水厂出水的水质评价中。主要从以下四个方面对转化机理进行了探讨:

       1,分析了溴离子存在条件下加氯消毒过程中母体多环芳烃的反应活性。发现pH值越低,母体多环芳烃的反应活性越高,不同多环芳烃的反应活性存在着较大的差异;而且不同多环芳烃随着 C(ClO-):C( Br- )的改变其活性变化较大,随着体系中Br-浓度的增加,萘、苯并[b]噻吩、芴等9种化合物的反应速率增加;吖啶、喹啉、二苯并噻吩的反应速率反而降低。吲哚、咔唑、苊烯和苊在此条件下,反应速率极快,不能准确的判断溴离子对母体多环芳烃反应活性的影响。 2,鉴定了溴离子存在下加氯消毒过程中的转化产物。发现这18种多环芳烃有的发生了亲电取代反应生成溴代多环芳烃,有的发生氧化反应生成氧化产物;在pH=4的条件下研究了不同C(ClO-):C(Br-)比例下的转化产物,研究发现,萘、苯并[b]噻吩、芴等9种化合物生成了溴代产物,而吲哚、苊烯、二苯并噻吩、蒽、吖啶、苯并[a]蒽均生成了氧化产物,二苯甲酮基本没有参与反应;其次,使用GC×GC-MS与计算化学的知识相结合预测了发生溴化反应的多环芳烃的反应路径。3,研究了溴代多环芳烃生成动力学。根据产物鉴定结果,选择部分主要溴代产物,进行定量分析,在pH=4时,随着溴离子浓度的增加,溴代多环芳烃的生成速率随之加快,或者转化程度加大。4,实际水厂案例分析。采集再生水厂出水进行定量分析,研究发现再生水厂加氯消毒过程中,确实会产生溴代多环芳烃;同时,1,6-二溴芘的检出率为100%,其次为6-溴苯并[a]芘,9-溴菲,2-溴芴,3,5,6-三溴苊也有检出,没有检出萘的溴代产物,这也印证了在加氯消毒过程中,芘与苯并[a]芘的活性较高,芴、菲也具有相对较强的反应活性,而萘的活性较低在实际条件下不易生成。

Other Abstract

        This thesis studied the impact of bromide ion in the transformation mechanism of 18 polycyclic aromatic hydrocarbons during the drinking water chlorine disinfection process and application in regenerated water works. And we mainly discussed from the following four aspects:

       1, The reactivity of the parent polycyclic aromatic hydrocarbons. The parent polycyclic aromatic hydrocarbons were more easily degrade under the low pH. Moreover, with the increase of the concentration of bromide ion, the degradation rate of naphthalene, benzo[b]thiophene, fluorene and the likes increased as well. But the degradation rate of arcidine, quinolone and dibenzo[b]thiophene decreased instead. 2, The degradation products identification. The degradation products under the condition of pH=4 and different bromide ion concentration were identified by using GC×GC-MS as a qualitative tool. We found that the products were just similar in different bromide ion concentration. The main products of naphthalene, benzo[b]thiophene, fluorene and the likes were bromo-substituted and the the main products of arcidine, dibenzo[b]thiophene, indole and the likes were oxidation products. 3, The production kinetics of bromo-substituted polycyclic aromatic hydrocarbons. We found that with the increase of bromide ion concentration the produce rate of bromo-substituted polycyclic aromatic hydrocarbons, such as 1-bromo-naphthalene and 1-bromo-pyrene, were increase as well. 4, The application in the actual regenerated water works. 1,6-dibromopyrene, 6-bromo-benzo[a]pyrene, 9-bromo-phenanthrene, 2-bromo-fluorene and 3,5,6-tribromo-acenaphthene were detected in the finished water. According to the reactivity of the parent polycyclic aromatic hydrocarbons, pyrene, fluoranthene were all easily degraded under chlorination.

Pages125
Language中文
Document Type学位论文
Identifierhttp://ir.rcees.ac.cn/handle/311016/41517
Collection环境水质学国家重点实验室
Recommended Citation
GB/T 7714
李强. 饮用水加氯消毒过程中溴离子对多环芳烃转化影响的研究及应用[D]. 北京. 中国科学院生态环境研究中心,2018.
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