化学氧化修复土壤PAHs过程中污染物的环境行为
发布时间：2018-11-29 13:50
【摘要】：多环芳烃是焦化工场地普遍存在的一类疏水性有机污染物。PAHs进入土壤后,可能会与土壤中不同有机质组分结合,而土壤有机质存在着高度的异质性,它其中的各组分(胡敏酸、富里酸、胡敏素)在结构上和对有机污染物的吸附能力上存在着很大的差异。因此,PAHs在有机质组分中的分配特征很可能影响其在土壤中生物有效性,进而影响其在环境中的生态风险。本文以北京某焦化厂土壤为研究对象,分析比较不同分级方法下PAHs的赋存形态。在此基础上以焦油为污染物,人工污染的胡敏酸、富里酸、胡敏素为研究对象,来研究PAHs随老化时间的迁移转化规律,比较不同氧化剂去除胡敏酸、富里酸、胡敏素中PAHs的去除效率,并分析污染物在化学氧化修复实验过程中的去向平衡,以期为实际的多环芳烃等有机污染物的化学氧化修复工程的进一步发展提供科学依据。具体研究结果如下:(1)分别采用酸碱提取法和非极性离子交换树脂(简称XAD-8树脂)提取法将土壤分为轻组分和重组分(胡敏酸、富里酸、胡敏素),并研究多环芳烃在各组分中的赋存特征。两种方法提取的各种组分物质吸收峰形基本相似,即提取物质一致,但提取物的响应值有明显差别。酸碱分级法和树脂分级法提取的总多环芳烃含量均为轻组高于重组,而重组中多环芳烃的含量主要分布在胡敏素中。与酸碱提取法相比,XAD-8树脂提取法提取的组分纯度较高,但实验步骤繁琐。(2)将焦油添加到北京农田土壤、胡敏酸、富里酸和胡敏素中进行老化实验。研究结果表明,焦油污染的胡敏酸、富里酸和胡敏素中16种多环芳烃的检出率均为100%,并且低环(2~4环)PAHs含量远远大于高环(5~6环)PAHs。此外,胡敏酸和富里酸会限制PAHs与胡敏素的结合。(3)研究了不同氧化剂对于老化后不同有机质组分中PAHs的去除效果及处理过程中污染物的去向。结果表明,过硫酸钠和高锰酸钾对于胡敏酸、富里酸、胡敏素中PAHs的去除,均有较好的修复效果;Fenton试剂能够较好的去除胡敏酸和富里酸中PAHs,但是对胡敏素中PAHs的去除效果一般;过氧化氢仅对胡敏酸中PAHs有较好的去除效果,对于富里酸和胡敏素中PAHs的去除较差。对于屈、苯并(b)荧蒽、苯并(k)荧蒽的4环PAHs,4种氧化剂的去除效果均较差。
[Abstract]:Polycyclic aromatic hydrocarbons (PAHs) are a common hydrophobic organic pollutant in coke chemical field. When PAHs enters the soil, it may combine with different organic components in soil, and soil organic matter has high heterogeneity. Its components (Hu Min acid, fulvic acid, humin) have great differences in structure and adsorption ability to organic pollutants. Therefore, the distribution characteristics of PAHs in organic components may affect the bioavailability of PAHs in soil, and then affect its ecological risk in the environment. Taking the soil of a coking plant in Beijing as the research object, the occurrence forms of PAHs under different classification methods were analyzed and compared. On this basis, using tar as pollutant, artificially polluted Hu Min acid, fulvic acid and humin as the research object, the migration and transformation of PAHs with aging time were studied, and the removal of Hu Min acid and fulvic acid by different oxidants was compared. The removal efficiency of PAHs from humin and the equilibrium of pollutants in chemical oxidation remediation experiment were analyzed in order to provide a scientific basis for the further development of chemical oxidation remediation engineering of organic pollutants such as polycyclic aromatic hydrocarbons (PAHs). The results are as follows: (1) the soil was divided into light components and recombined fractions (Hu Min acid, fulvic acid, humin) by acid-base extraction method and non-polar ion exchange resin (XAD-8 resin) extraction method, respectively. The occurrence characteristics of polycyclic aromatic hydrocarbons (PAHs) in each component were studied. The absorption peaks of each component extracted by the two methods were basically similar, that is, the extracted substances were the same, but the response values of the extracts were obviously different. The content of PAHs extracted by acid-base classification method and resin classification method was higher in light group than in recombination group, while the content of PAHs in recombination was mainly distributed in humin. Compared with acid-base extraction, the purity of components extracted by XAD-8 resin was higher, but the experimental steps were complicated. (2) Aging experiments were carried out by adding tar into Beijing farmland soil, Hu Min acid, fulvic acid and humin. The results showed that the detection rate of 16 PAHs in Hu Min acid, fulvic acid and humin was 100%, and the PAHs content of low ring (2o 4 ring) was much higher than that of high ring (5o 6 ring) PAHs.. In addition, Hu Min acid and fulvic acid can limit the binding of PAHs to humin. (3) the removal effect of different oxidants on PAHs in different organic components after aging and the fate of pollutants in the treatment process were studied. The results showed that sodium persulfate and potassium permanganate had good effect on the removal of PAHs from Hu Min, fulvic acid and humin. Fenton reagent could remove PAHs, from Hu Min acid and fulvic acid, but the removal effect of PAHs from humin was mediocre, and hydrogen peroxide had better removal effect on PAHs in Hu Min acid than PAHs in fulvic acid and humin. For flexion, benzo (b) fluoranthene and benzo (k) fluoranthene, the removal efficiency of PAHs,4 oxidant was poor.
【学位授予单位】：天津大学
【学位级别】：硕士
【学位授予年份】：2015
【分类号】：X53
[Abstract]:Polycyclic aromatic hydrocarbons (PAHs) are a common hydrophobic organic pollutant in coke chemical field. When PAHs enters the soil, it may combine with different organic components in soil, and soil organic matter has high heterogeneity. Its components (Hu Min acid, fulvic acid, humin) have great differences in structure and adsorption ability to organic pollutants. Therefore, the distribution characteristics of PAHs in organic components may affect the bioavailability of PAHs in soil, and then affect its ecological risk in the environment. Taking the soil of a coking plant in Beijing as the research object, the occurrence forms of PAHs under different classification methods were analyzed and compared. On this basis, using tar as pollutant, artificially polluted Hu Min acid, fulvic acid and humin as the research object, the migration and transformation of PAHs with aging time were studied, and the removal of Hu Min acid and fulvic acid by different oxidants was compared. The removal efficiency of PAHs from humin and the equilibrium of pollutants in chemical oxidation remediation experiment were analyzed in order to provide a scientific basis for the further development of chemical oxidation remediation engineering of organic pollutants such as polycyclic aromatic hydrocarbons (PAHs). The results are as follows: (1) the soil was divided into light components and recombined fractions (Hu Min acid, fulvic acid, humin) by acid-base extraction method and non-polar ion exchange resin (XAD-8 resin) extraction method, respectively. The occurrence characteristics of polycyclic aromatic hydrocarbons (PAHs) in each component were studied. The absorption peaks of each component extracted by the two methods were basically similar, that is, the extracted substances were the same, but the response values of the extracts were obviously different. The content of PAHs extracted by acid-base classification method and resin classification method was higher in light group than in recombination group, while the content of PAHs in recombination was mainly distributed in humin. Compared with acid-base extraction, the purity of components extracted by XAD-8 resin was higher, but the experimental steps were complicated. (2) Aging experiments were carried out by adding tar into Beijing farmland soil, Hu Min acid, fulvic acid and humin. The results showed that the detection rate of 16 PAHs in Hu Min acid, fulvic acid and humin was 100%, and the PAHs content of low ring (2o 4 ring) was much higher than that of high ring (5o 6 ring) PAHs.. In addition, Hu Min acid and fulvic acid can limit the binding of PAHs to humin. (3) the removal effect of different oxidants on PAHs in different organic components after aging and the fate of pollutants in the treatment process were studied. The results showed that sodium persulfate and potassium permanganate had good effect on the removal of PAHs from Hu Min, fulvic acid and humin. Fenton reagent could remove PAHs, from Hu Min acid and fulvic acid, but the removal effect of PAHs from humin was mediocre, and hydrogen peroxide had better removal effect on PAHs in Hu Min acid than PAHs in fulvic acid and humin. For flexion, benzo (b) fluoranthene and benzo (k) fluoranthene, the removal efficiency of PAHs,4 oxidant was poor.
【学位授予单位】：天津大学
【学位级别】：硕士
【学位授予年份】：2015
【分类号】：X53
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