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题名: 大气中持久性有机污染物的被动采样研究
作者: 李晓敏
学位类别: 博士
答辩日期: 2012
授予单位: 中国科学院研究生院
授予地点: 北京
导师: 张庆华
关键词: 大气被动采样 ; passive air sampling ; POPs ; POPs ; PUF大气被动采样器 ; PUF-PAS ; SBSE ; SBSE ; 钢铁厂 ; steel industry
其他题名: A pilot study on passive air sampling of persistent organic pollutants
中文摘要:     持久性有机污染物(POPs)全球长距离迁移的主要途径是大气传输,这类化合物可通过呼吸作用被吸入体内,对人类造成潜在健康威胁。大气中的POPs含量较低,传统的大流量主动采样设备价格昂贵,无法同时进行大规模采样。针对主动采样技术缺陷而发展起来的被动采样技术已日渐成熟,近年来被广泛用于多种POPs全球大气大尺度研究中。本论文围绕被动采样技术在大气中POPs采集方面的应用展开,利用传统被动采样技术对典型污染地区大气中POPs含量水平、季节性变化和污染源进行分析;并对一种新型被动采样技术进行方法开发和实际应用方面的研究。全文主要分为以下3个部分: 首先,通过一种传统被动采样技术对钢铁厂及其周边地区大气中二恶英(PCDD/Fs),多氯联苯(PCBs)和多溴联苯醚(PBDEs)含量水平、空间分布、季节性变化规律以及潜在污染源等进行研究,评价钢铁生产对厂区内及周边地区大气中这三种污染物的贡献。我们选择我国北方一大型钢铁生产厂(鞍山钢铁厂)作为目标研究区域,通过在厂区内及周边地区布设聚氨酯泡沫(PUF)被动采样器,分别采集了2008年6月~2008年9月之间的夏季大气样品和2008年12月~2009年3月之间的冬季大气样品。结果表明,厂区及其周边地区大气中Σ17PCDD/Fs (夏季:0.02–2.77 pg/m3,冬季0.20–9.79 pg/m3),Σ19PCBs(夏季:23.5–155.8 pg/m3,冬季:14.6–81.3 pg/m3)和Σ13PBDEs (夏季:2.91–10.7 pg/m3,冬季:1.10–3.89 pg/m3)三种污染物浓度与其他城市和工业地区相比略低,说明钢铁生产并未对当地大气造成严重的二恶英影响。三种污染物的季节性变化趋势为:大气中PCDD/Fs冬季含量水平高于夏季,而PCBs和PBDEs则具有相反趋势。主成分分析(PCA)表明燃煤可能是当地地区PCDD/Fs主要源,但钢铁生产对当地大气中PCDD/Fs也有一定贡献。 其次,以聚二甲基硅氧烷(PDMS)涂层的搅拌子作为大气被动采样器,建立了搅拌子固相吸附-热脱附-气相色谱/质谱/质谱联用法(SBSE-TD-GC/MS/MS)快速测定室内空气中16种美国环保署(EPA)优先控制多环芳烃(PAHs)的方法。在搅拌子表面涂渍标准样品,待溶剂挥发后放于脱附管内,在多反应监测模式(MRM)下,对多环芳烃子离子、碰撞能量、热脱附参数(脱附温度,冷阱捕集温度和脱附时间)等条件进行了优化,并建立标准曲线;以12种氘代同位素PAHs为内标,建立了多窗口下16种EPA优先多环芳烃的分析方法,方法回收率在45.1%~109%之间,检出限为0.020~0.054 ng/sample。利用本方法对模拟燃煤前后室内大气中悬挂搅拌子中的多环芳烃进行了被动吸附与检测,燃煤前后室内大气样品中16种多环芳烃含量分别为4.24~5.32 ng/sample和172~200 ng/sample。 最后,采用聚二甲基硅氧烷(PDMS)涂层的搅拌子作为大气被动采样器,建立了搅拌子固相吸附-热脱附-气相色谱/质谱联用法(SBSE-TD-GC/MS)同时快速测定16种EPA优先的多环芳烃的方法,并对仪器条件进行优化。该方法检出限在0.024~0.103 ng/sample之间。利用本方法对云南宣威肺癌高发地区和其相邻的肺癌低发对比地区大气中PAHs进行采样与检测,结果显示,高发区室内炉灶处含量最高,Σ16 PAHs平均值约为118 ng/sample。高发区室内与低发区室内PAHs含量水平差别不大,均高于相应地区室外空气中PAHs含量。此外,结合当地地形,发现宣威地区工业分布及乌蒙山山区特殊地形致使当地产生的PAHs不易扩散,有可能是导致当地肺癌高发的原因之一。
英文摘要:     Persistent organic pollutants (POPs) are ubiquitous around the world because of its long range transport. These compounds could enter into the human bodies through respiration process and expose potential health risks. The traditional method which is used to determine atmospheric POPs is using high volume air samplers. However, this method is not quite suitable when samplings need to be simultaneously performed because instruments are expensive. Passive air samplers (PAS) are designed against the shortcomings of high volume air samplers, and now are widely and globally applied in environmental monitoring. This dissertation focused on the application of passive air sampling technology on atmospheric POPs. Firstly we used a common polyurethane foam-PAS to evaluate the levels, seasonal variation and pollutant sources around an iron and steel industrial park, and then a new PAS was developed and applied in field sampling. It consists of the following 3 parts: The first part focused on the emissions of polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs), polychlorinated biphenyls (PCBs), and polybrominated diphenyl ethers (PBDEs) from steel industrial parks. In this study, PUF-disk based passive air samples were collected in and around a big steel industrial park of Anshan, Northeast China. Summer samples were collected during June 2008 to September 2008, while winter samples were in the range of December 2008-March 2009. The levels, seasonal variations and potential sources of PCDD/Fs, PCBs and PBDEs in the atmosphere around the steel industrial complex were investigated, and potential contribution of these three groups of POPs from iron and steel production was also assessed. The air concentrations of ∑17 PCDD/Fs (summer: 0.02-2.77 pg/m3; winter: 0.20-9.79 pg/m3), ∑19 PCBs (summer: 23.5-155.8 pg/m3; winter: 14.6-81.3 pg/m3) and ∑13 PBDEs (summer: 2.91-10.7 pg/m3; winter: 1.10-3.89 pg/m3) in this targeted industrial park were relatively low in comparison to other studies, which implied that the industrial activities of iron and steel had not resulted in serious contamination of these POPs to the ambient air in this area. On the whole, the air concentrations of PCDD/Fs in winter were higher than those of summer, whereas the concentrations of PCBs and PBDEs showed opposite trends. The result from principal component analysis indicated that coal combustion might be the main contributor of PCDD/F sources in this area. In the second part, a method was developed for the determination of polycyclic aromatic hydrocarbons (PAHs) in indoor air by a novel passive air sampler, PDMS (polydimethylsiloxane)-coated stir bar sorptive extraction (SBSE), which was detected by thermal desorption (TD) coupled to gas chromatography/triple quadrupole mass spectrometry (GC/MS/MS). PAH standard solution was sprayed to the surface of the stir bar, and it was put into a desorption tube as soon as solvent was evaporated. Daughter ions, collision energy under multiple reaction monitoring (MRM) mode were optimized. TD parameters such as desorption temperature (300℃), cooled injection system (CIS) temperature (-60℃) and desorption time (6 min) were also optimized to enhance detection sensitivity. 12 deuterated internal standards were applied to identify and quantify 16 EPA-PAH congeners under 4 functions. The method recoveries were ranged from 45.1% to 109% and the limits of detection (LOD) were between 0.020 and 0.054 ng/sample. The established method was further applied to analyze 16 PAHs of indoor air before and after coal combustion by hanging the novel PAS in a room. The PAHs concentrations of stir bars were 4.24-5.32 ng/sample and 172-200 ng/sample before and after coal combustion, respectively. At last, the PDMS-coated stir bar was also used as PAS and then the stir bar was detected by TD-GC/MS. The detection method of 16 EPA-PAHs was optimized. The LOD were in the range of 0.024-0.103 ng/sample. The established method was further applied to air sampling at a lung cancer high incidence area and a control area. The highest ΣPAHs concentrations were found in the cooking room (average 118 ng/sample). The indoor PAHs levels were higher than the outdoor level both in the high incidence area and control area. Furthermore, we observed that the industrial area was located between two hills, and exhaust gas could be difficult to diffuse in this area, so the local topography might be one of the reasons caused the high incidence of lung cancer in this area.
内容类型: 学位论文
URI标识: http://ir.rcees.ac.cn/handle/311016/35099
Appears in Collections:环境化学与生态毒理学国家重点实验室_学位论文

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Recommended Citation:
李晓敏. 大气中持久性有机污染物的被动采样研究[D]. 北京. 中国科学院研究生院. 2012.
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