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题名: 极地大气中持久性有机污染物的污染特征、来源及变化趋势
作者: 郝艳芬1
学位类别: 硕士
答辩日期: 2017-05
授予单位: 中国科学院大学
授予地点: 北京
导师: 李英明
关键词: 极地地区,大气环境,被动采样,多氯联苯,多溴联苯醚,有机氯农药 ; polar regions, atmosphere, passive air sampling, PCBs, PBDEs, OCPs
其他题名: Pollution Characteristics, Sources and Variation ofPersistent Organic Pollutants in the Atmosphere of PolarRegions
学位专业: 环境科学
中文摘要: 持久性有机污染物(persistent organic pollutants, POPs)是一类具有半挥发 性、生物积累性、持久性以及高毒性的有机污染物的总称。多氯联苯 (polychlorinated biphenyls, PCBs)、多溴联苯醚(polybrominated diphenyl ethers, PBDEs)以及有机氯农药(organochlorine pesticides, OCPs)都属于典型的POPs 类,都被列入《关于持久性有机污染物的斯德哥尔摩公约》(简称《斯德哥尔摩 公约》)受控污染物名单之中。由于POPs 具有半挥发性的特点,其在全球转运 的主要途径之一是大气传输。POPs 可通过大气传输由污染源迁移至偏远地区。 目前有大量研究数据及报告表明,极地地区存在明显的POPs 检出及积累现象。 本论文是利用XAD 树脂被动采样技术,采集了2011 年到2015 年西南极长城 站及其周边地区以及北极黄河站及其周边地区大气样品,通过高分辨气相色谱- 高分辨质谱联用(HRGC-HRMS)技术分析样品中痕量的PCBs、PBDEs 以及 OCPs,并对其污染特征、变化趋势以及来源进行分析。本文主要围绕以下三方 面的研究工作展开: (1)对2011-2015 年南北极大气中PCBs 的浓度水平、单体分布特征以及 年变化规律进行了分析,结果表明南极地区大气中PCBs 的浓度范围为0.37 pg/m3-2.81 pg/m3,北极地区为0.96 pg/m3 -6.87 pg/m3,南极科考站周围大气中 PCBs 的浓度变化特征与其他点位有明显不同,说明南极科考站可能对其周围大 气中PCBs 的浓度变化有影响;北极地区各点位PCBs 浓度年变化不存在显著差 异,说明北极受到PCBs 的大气传输影响更明显。两极地区各点位大气中PCBs 单体多数处于可检出水平,并以三氯代单体PCB-28 为主要单体,也反映了大 气远距离传输对极地大气中PCBs 的单体分布的影响。 (2)对2011-2015 年南北极大气样品中PBDEs 的浓度水平、单体分布特 征以及年变化趋势进行了研究。结果显示南北极各点位大气中PBDEs 均有检 出,南北极地区大气中PBDEs 浓度水平无明显差异(南极为0.05 pg/m3-0.75 pg/m3,北极为0.09 pg/m3-0.30 pg/m3),各年份浓度水平变化不大。南北极大气 中PBDEs 均以BDE-47、-99、-153 以及-183 为主,单体分布呈现出高溴代单体 比例降低,低溴代单体比例增加的年变化趋势。通过对比南北极大气中和两种 商用PBDEs 工业化学品中主要PBDEs 单体的浓度比值发现,南北极大气中 PBDEs 受到商用五溴代以及八溴代PBDEs 产品的共同影响。 (3)研究了2011-2015 年南北极大气样品中OCPs 的浓度水平、分布特征 以及年变化规律,并分析了其可能的来源。在检测的25 类OCPs 中,检出14 类,其中六氯苯(HCB)是最主要检出的OCPs,其在北极大气(129 pg/m3)中的浓度明显高于南极大气(40.6 pg/m3)。六六六(HCHs)(α-HCH、β-HCH、 γ-HCH、δ-HCH)以及滴滴涕(DDTs)(o,p′-DDE、p,p′-DDE、o,p′-DDT、p,p′-DDT) 在南极大气中的浓度分别为: 0.63、0.23、0.28、0.05、0.07、0.21、0.04、0.09 pg/m3;在北极大气中的浓度分别为:6.10、0.70、0.81、0.10、0.09、0.40、0.08、 0.17pg/m3。通过分析大气中α-/γ-HCH 以及p,p′-DDT/p,p′-DDE 发现,南极大气 中HCHs 主要受到工业HCHs 以及林丹的共同影响,而北极大气中的HCHs 主 要受到工业HCHs 的影响;南北极大气中的DDTs 主要来自历史残留。
英文摘要: Persistent organic pollutants (POPs) are a kind of pollutants with the properties of semi-volatility, biological accumulation, persistence and highly-toxicity. Polychlorinated biphenyls (PCBs), polybrominated diphenyl ethers (PBDEs) and organochlorine pesticides (OCPs) are all typical POPs and were listed in the Stockholm Convention. Atmosphere is the main way for POPs global transport due to its properties of semi-volatility and POPs could reach to the remote regions through the air. Many researches have reported the existence and accumulation of POPs in Antarctic and Arctic regions. In this study, air samples were collected in Antarctic Great Station Station and Arctic Yellow River Station sites from 2011 to 2015 using XAD-resin based passive sir sampler(PAS). Determination of PCBs, PBDEs and OCPs in these air samples was performed by high resolution gas chromatography coupled with high resolution mass spectrometry (HRGC-HRMS) and the aim of this research was to investigate the air concentrations, congener profiles, temporal trend and sources of PCBs, PBDEs and OCPs in atmosphere of the Antarctic and Arctic. This thesis was mainly demonstrated in following three parts: (1) Concentrations, congener profiles and temporal trends of PCBs in the atmosphere of Antarctic and Arctic were analyzed. Results showed that concentrations of PCBs in the atmosphere of Antarctic and Arctic sampling sites were 0.37 pg/m3-2.81 pg/m3and 0.96 pg/m3-6.87 pg/m3, respectively. Temporal trends of PCBs were different between Antarctic and Arctic, which might related to geographical location and effect from human activities. In the Antarctic sites, temporal trend of PCBs in the ambient air around Chinese Great Station Station differed from that around other sampling sites, which implying that the station is a factor influencing the concentration of PCBs in the air. No different temporal trends of PCBs were observed among sampling sites in Arctic, indicating the effect of long-range atmospheric transport (LRAT). Most PCBs congeners were detectable in the atmosphere of polar region and tri-chlorinated PCBs (3-CBs) dominated, which might be related to the LRAT. (2) Concentrations, congener profiles and temporal trends of PBDEs in the atmosphere of Antarctic and Arctic were investigated. PBDEs were all detected in the air samples collected from different sites in Antarctic and Arctic. Levels of PBDEs were comparable between the polar areas with 0.05 pg/m3-0.75 pg/m3 in Antarctic and 0.09 pg/m3-0.30 pg/m3 in Arctic. There was no obvious temporal trend of concentrations of PBDEs in the air. PBDEs in the atmosphere were dominated by BDE-47 、-99 、-153 and -183. The proportions of high-brominated PBDEs decreased whereas the low-brominated PBDEs increased from 2011 to 2015. Comparison of ratios among PBDEs congeners between air samples and commercial products showed that congener profiles of PBDEs in air of Antarctic and Arctic were affected by the combination of Penta-BDEs and Octa-BDEs. (3) Concentrations, congener profiles, temporal trends and sources of OCPs in the atmosphere of Antarctic and Arctic were studied. Among 25 OCPs, 14 OCPs were detected in the air samples and the concentration of HCB was highest with 129 pg/m3 in Arctic and 40.6 pg/m3 in Antarctic, followed by α-HCH and endosulfan-I. Atmospheric concentrations of HCHs(α-HCH、β-HCH、γ-HCH、 δ-HCH)and DDTs(o,p′-DDE、p,p′-DDE、o,p′-DDT、p,p′-DDT)were 0.63、 0.23, 0.28, 0.05, 0.07, 0.21, 0.04 and 0.09 pg/m3 in Antarctic, 6.10, 0.70, 0.81, 0.10, 0.09, 0.40, 0.08 and 0.17 pg/m3 in Arctic, respectively. The ratio of α-/γ-HCH showed that HCHs in the atmosphere of Antarctic was related to the combination of HCHs products and lindane while those of Arctic was mainly affected by HCHs products. Analysis of p,p′-DDT/p,p′-DDE showed that DDTs in air of Antarctic were affected by aged source of technical DDTs and the same in Arctic.
内容类型: 学位论文
URI标识: http://ir.rcees.ac.cn/handle/311016/38628
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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作者单位: 1.中国科学院生态环境研究中心

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郝艳芬. 极地大气中持久性有机污染物的污染特征、来源及变化趋势[D]. 北京. 中国科学院大学. 2017.
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