南京城东大气中多环芳烃与颗粒物的污染特征研究

发布时间：2018-03-10 07:46

  本文选题：大气　切入点：多环芳烃　出处：《南京农业大学》2015年硕士论文　论文类型：学位论文

【摘要】：多环芳烃(PAHs)是一类具有"致畸、致癌、致突变"效应、高度疏水性的持久性有机污染物(POPs)。大气中PAHs来源广泛,生活燃煤、汽车尾气以及工业化石燃料燃烧等都会产生大量PAHs。相比其它环境介质,大气中PAHs可以通过呼吸作用或皮肤暴露接触而进入人体,直接对人群健康造成危害。同时,进入大气中的PAHs还可经由干、湿沉降进入水体或土壤,并通过食物链富集间接危害人体健康。研究大气中PAHs污染特征、解析其污染源,对从根本上控制PAHs排放、防治大气PAHs污染、保障人群健康具有重要意义。大气中PAHs主要以气态和颗粒态两种形式存在,其中,颗粒态PAHs吸附在大气颗粒物中,主要以高环高毒PAHs为主,对人群的健康危害较大。由于近年来,我国雾霾事件频发,大气颗粒物浓度"爆表",明晰大气中总悬浮颗粒物(TSP)与大气PAHs之间的关系,将为评估雾霾天气下PAHs对人群健康的影响提供重要基础依据。本文在改进大气中气态和颗粒态PAHs分离检测方法的基础上,对南京城东区内采样点大气中PAHs进行定期监测,研究了大气中不同形态PAHs的时间变化规律,并进行源解析。同时,采集TSP以及采样点处地表灰尘,分析其PAHs含量,探讨大气中PAHs与TSP浓度以及大气沉降之间的关系。主要研究结果如下:(1)采用梯度洗脱和双波长法,系统地优化了大气中16种优先控制的气态和颗粒态PAHs的采样、提取和检测方法。确定采用大流量采样仪以100 L/min的流速、每次采样4 h的采样量,并利用玻璃纤维滤膜截留收集的方法采集大气颗粒态PAHs。将采集到的样品充分干燥,经二氯甲烷超声萃取,氮气浓缩近干后,用1ml乙腈定容,过0.22 μm孔径滤膜,进行HPLC/UV分析。分析结果表明,该方法测定16种PAHs的回收率在50%-110%之间,相对标准偏差小于10%。气态PAHs的采集选择XAD-2多孔有机复合树脂作为吸附剂,并使用小流量采样器以1 L/min的流速采集4 h作为采样量。样品采集后,置入4℃冰箱内避光密封保存备用,提取方法同颗粒态PAHs提取。结果表明,16种PAHs的回收率在50%-110%之间,大部分高达80%-100%,且相对标准偏差小于9%。(2)研究了南京市城东区域大气中PAHs污染特征。通过对南京城东区域采样点大气的定期监测,发现大气中气态和颗粒态PAHs污染存在一定的季节性特征。冬季时PAHs污染浓度最高,秋季次之,而春季较低。强致癌物苯并[a]芘的污染特征表明,冬季大气中高环高毒PAHs的种类所占比例增大,特别是气态PAHs,苯并[a]芘浓度超过了国家限制数十倍,达到0.6 μg/m3。分析对比气态和颗粒态PAHs的含量可得,大气中PAHs主要以气态存在,其浓度高达10-20 μg/m3左右,而颗粒态PAHs的浓度多在0.05-0.1 μg/m3左右,低于气态两个数量级。气态和颗粒态PAHs的环数和种类特征表明,气态PAHs以低环种类为主,而颗粒态PAHs中高环类所占比较高。利用比值法对大气PAHs进行源解析,发现燃煤和汽油燃烧是南京城东大气中PAHs的最主要污染源,冬季燃煤导致的大气PAHs污染十分明显,其它季节大气中PAHs的污染以汽油燃烧为主。(3)探讨了大气中PAHs与TSP及地表灰尘之间的相关性。通过定期监测,发现南京城东区域大气TSP污染存在一定季节性,冬季污染水平总体要高于其它季节,但是这种季节性并不十分明显,数据波动大,在其他季节也经常出现TSP浓度较高的情况,这与TSP受短期天气和人类活动影响较大有关。分析比较大气中TSP与PAHs的监测数据发现,TSP与颗粒态PAHs存在显著相关性(P0.05).当TSP浓度升高时,颗粒态PAHs的浓度也会随之升高。然而,大气中TSP与气态PAHs并无显著相关性(P0.05)。分析地表灰尘中PAHs,其浓度变化具有明显地季节相关性,大小依次为冬季秋季春季.在冬季时,地表灰尘中PAHs的总量明显增加,且高环PAHs比例有所上升,主要污染源为煤炭燃烧以及汽油燃烧,这与大气中PAHs的季节变化规律和污染源相似,说明大气颗粒物是地表灰尘的重要来源。
[Abstract]:Polycyclic aromatic hydrocarbons (PAHs) is a kind of "carcinogenic, teratogenic, mutagenic effect, persistent organic pollutants are highly hydrophobic (POPs). PAHs source in the atmosphere of life, coal, automobile exhaust and industrial combustion of fossil fuel will produce a large number of PAHs. compared to other environmental media, the atmosphere can breathe through PAHs effect of skin contact or exposure directly into the human body, causing harm to human health. At the same time, PAHs can enter into the atmosphere through dry wet deposition into water or soil, and enriched through the food chain indirectly harmful to human health. The research of atmospheric PAHs pollution characteristics, analysis of the pollution sources of PAHs emissions from the fundamental control PAHs, the prevention and control of atmospheric pollution, it has important significance to protect human health. In the atmosphere of gaseous and particulate PAHs mainly exists in two forms, the particulate PAHs adsorbed on the atmospheric particles, mainly in high ring high Poison PAHs, great harm to people's health. In recent years, China's frequent occurrence of fog and haze, the concentration of atmospheric particulate scale, total suspended particulate matter in the atmosphere is clear (TSP) relationship between PAHs and the atmosphere, for evaluation of haze weather PAHs on human health effects provide an important basis for in this article. The improved detection method based gaseous and particulate PAHs separation in the atmosphere, on the east of Nanjing area sampling PAHs points were monitored regularly in the atmosphere, study on variation of different forms of PAHs in the atmosphere, and analyze the source. At the same time, acquisition and TSP sampling point surface dust, analysis of the content of PAHs to explore the relationship between the settlement of PAHs, and the concentration of TSP and the atmosphere in the atmosphere. The main results are as follows: (1) by using gradient elution and dual wavelength method, system to optimize the atmospheric sampling 16 priority control of gaseous and particulate PAHs , extraction and detection methods. Determined by flow sampling instrument at the rate of 100 L/min, 4 h each sampling sampling, and the use of glass fiber membrane interception method of collection of atmospheric particles collected PAHs. collected samples will fully dry, ultrasonic extraction with dichloromethane, nitrogen concentration nearly dry, with 1ml acetonitrile volume in 0.22, M pore diameter membranes, HPLC/UV analysis. The analysis results show that the recovery of the 16 methods for determination of PAHs ratio between 50%-110%, the relative standard deviation is less than 10%. PAHs XAD-2 acquisition of gaseous organic porous composite resin as adsorbent, and the use of small flow sampler at the rate of 1 L/min and 4 h as sample collection samples were collected. After the placement of 4 DEG C in the refrigerator light sealed with standby, extraction method of particulate PAHs extraction. The results showed that the recovery rate of PAHs 16 in 50%-110%, the majority of up to 80%-100%, and the relative standard The standard deviation is less than 9%. (2) of the PAHs regional air pollution characteristics in Nanjing City East. Through regular monitoring of atmospheric sampling points in Nanjing East region, found in the atmosphere of gaseous and particulate PAHs pollution there are some seasonal characteristics. The highest concentration of PAHs pollution in winter, autumn, spring and show low. The pollution characteristics of strong carcinogen benzo [a] pyrene in ambient air in winter, high ring type high toxic PAHs proportion increases, especially the gaseous PAHs, benzo [a] pyrene concentrations exceeding the national limit of dozens of times, reaching 0.6 g/m3. content analysis of gaseous and particulate PAHs available, mainly in the atmosphere PAHs the form of gas, its concentration is as high as 10-20 g/m3, and particulate PAHs concentrations in 0.05-0.1 g/m3, less than two orders of magnitude. That gaseous gaseous and particulate PAHs ring number and type characteristics of gaseous PAHs with low ring type, and Particulate PAHs high rings accounted for relatively high. To analyze the source of atmospheric PAHs using the ratio method, found that coal and gasoline combustion is the major source of pollution in the atmosphere of Nanjing East PAHs, PAHs air pollution caused by coal in winter is very obvious, other PAHs seasonal air pollution mainly in the combustion of gasoline (3). To investigate the correlation between PAHs and TSP in the atmosphere and surface dust. Through regular monitoring, found east of Nanjing regional atmospheric TSP pollution are seasonal, the overall level of pollution in winter than in other seasons, but this is not very obvious seasonal fluctuations in the data, in the other seasons are often in the higher concentration of TSP, the and TSP was affected by the short-term weather and human activities more relevant. Monitoring data analysis of TSP compared with PAHs in the atmosphere, TSP and particulate PAHs significant correlation (P0.05). When the concentration of TSP increased When the concentration of particulate PAHs also increased. However, no significant correlation between TSP and PAHs gas atmosphere (P0.05). PAHs analysis of surface dust, the concentration has obvious seasonal correlation, followed by the size of autumn winter spring. In winter, the total amount of PAHs in surface dust increased significantly, and high ring PAHs ratio has increased, the main pollution sources for coal combustion and combustion of gasoline, which is similar to seasonal variation and pollution sources of PAHs in the atmosphere, atmospheric particles are an important source of surface dust.

【学位授予单位】：南京农业大学
【学位级别】：硕士
【学位授予年份】：2015
【分类号】：X513

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