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题名: 全氟化合物分析方法及其在纳木错流域陆生食物链中富集行为研究
作者: 李义莉1
学位类别: 硕士
答辩日期: 2017-06
授予单位: 中国科学院大学
授予地点: 北京
导师: 张爱茜 ; 傅建捷
关键词: 全氟化合物,纳木错流域,陆生食物连,分析方法,生物富集 ; Perfluoroalkyl substances (PFASs), Nam Co basin, Analyticalmethods, Bioaccumulation, terrestrial food chain
其他题名: Analytical Method Development of PFASs and Their Bioaccumulation Behavior in a Terrestrial Food Chain from Nam Co Basin
学位专业: 分析化学
中文摘要: 全氟化合物(PFASs)稳定性强,且具有疏水疏油的特殊性质,从上世纪 50年代起就被广泛应用于生产和生活领域。PFASs在生产、使用、以及产品的 最终处置过程中被释放到环境,目前 PFASs已经在包括南北极和青藏高原等偏 远区域的全球各种环境介质中被检出,成为一种全球性污染物。 本文首先选择鸟类羽毛作为生态系统中 PFASs污染指示物,对羽毛中 PFASs分析方法进行优化,提高 PFASs在羽毛中的分析灵敏度。然后对西藏纳 木错流域陆生生态系统中不同营养级的生物样品和介质中 PFASs进行测定,初 步研究讨论了该流域中 PFASs的环境行为。 论文第一部分对南北极,高海拔高寒山区等偏远区域 PFASs的分布情况以 及环境行为进行了综述,并对偏远区域 PFASs进行了源解析。在本论文的研究 内容中,由于猛禽等鸟类处于较高的营养级,在生态系统中具有很重要的地位, 包括我国在内的全球大部分国家都将猛禽列入保护动物,研究野生鸟类受损性 (包括肌肉,血样,组织等)样品中 PFASs的赋存状况存在很大的困难,因此, 本文第二部分针对羽毛这种非损伤性样品,通过比较各种前处理及富集净化手 段,最终选择甲醇溶剂直接萃取结合 WAX固相萃取柱以及 HPLC-ESI-MS/MS, 建立了羽毛中 13种 PFASs的前处理及分析方法,该方法相较于之前羽毛中 PFASs检测方法,其检出限下降 1-2个数量级,并成功的应用于纳木错流域鸟 类羽毛样品中 PFASs的测定。通过对纳木错流域鸟类羽毛的研究发现,PFOS 为该地区主要全氟污染物,PFBA,PFBS等短链 PFASs物的分布比例较高,这 也说明在长链 PFASs生产使用受到控制后,短链 PFASs对长链 PFASs的替代已 经在纳木错流域有所反映。通过对杂食性鸟类羽毛的研究发现,杂食性鸟类羽 毛中 PFASs浓度要低于捕食性猛禽羽毛中 PFASs浓度水平,这说明 PFASs可能 在该区域生态系统中具有生物放大效应。 论文的第三部分首次对青藏高原纳木错流域植物 -鼠兔-鹰陆生食物链中 PFASs的赋存和富集放大行为进行了研究。首先通过多种萃取溶剂优化肌肉样 品中 PFASs的前处理及分析方法,选定 0.1%甲酸-乙腈直接提取,经 WAX富 集净化后结合 HPLC-ESI-MS/MS对样品中 PFASs进行分析测定,PFASs的回收 率在 72-121%之间。通过研究发现该食物链中 PFOS是主要全氟污染物,PFBA 次之,与羽毛中 PFASs分布特征一致,因此羽毛中全氟污染物可特征性指示动 物体内污染物分布特征。虽然鹰类肌肉中 PFASs与羽毛中 PFASs之间并没有显 著相关性,但两者浓度在同一数量级,可通过羽毛中 PFASs指示肌肉中 PFASs 赋存与分布。进一步对 PFASs在纳木错流域植物-鼠兔-鹰形成的简单陆生食物 链的生物富集性进行研究,PFBA、PFOS和 PFDA在植物-鼠兔-鹰中 TMF分别 为 1.74,1.95和 2.57,表现出营养级放大现象,且 TMF值随碳链长度增长而变 大,但短碳链的 PFBA的 TMF也大于 1,说明短链 PFSAs也存在在生态系统中 富集放大的风险。通过生物放大因子进一步研究该食物链中 PFASs的传递行为, 植物和鼠兔之间多种 PFASs生物放大因子大于 1,鹰和鼠兔之间长链 PFCAs和 PFSAs也存在较明显的生物放大效应,进一步说明 PFASs在生物体内的富集效 应,PFASs可通过生物捕食关系在高营养级生物中富集。
英文摘要: Perfluoroalkyl substances (PFASs) have strong stability, and they show special properties on both hydrophobicity and lipophobicity. PFASs have been used in industrial and daily application widely since 1950s. PFASs can enter into the environment during their production, application, and production disposal. PFASs are ubiquitous in environmental matrixes including remote areas, such as the Arctic and Antarctic regions, and Tibetan Plateau. The distribution and environmental behavior of PFASs in remote areas such as Arctic, Antarctic, and high-altitude alpine region were summarized in the first part of this dissertation. Meanwhile the source of PFASs in these remote areas was also discussed. Environmental samples and biota samples of different tropic levels were collected from terrestrial ecological system in Nam Co Basin in the present study. Birds played an important role in the ecosystem for their relative high trophic level in the ecosystem, and most of birds were listed as protected animals in most countries including China, especially for Accipiters. So, it is hard to get destructive samples (including muscle, blood, organs and so on) of wild birds. Feather samples have been successfully applied as nondestructive indicators for several contaminants. The second part of this dissertation was focused on the analytical methods for feather PFASs. According to the spiked recoveries, a weak-anion exchange cartridge was chosen and the methanol was selected as the extraction solvent. In the present study, an optimized pretreatment procedure combined with high-performance liquid chromatography–electrospray ionization–tandem mass spectrometric (HPLC–ESI– MS/MS) method was established for the determination of PFASs in feathers. The recoveries and method detection limits of the PFASs ranged from 71 to 120% and 0.16 to 0.54 ng/g, respectively. Compared with a previous study, the LOD for feather samples were reduced by 1-2 orders of magnitude, especially for long-chain PFCAs. Finally, 13 PFASs in feather samples from Nam Co Basin, Tibetan Plateau, were analyzed, indicating that PFOS was the predominant PFAS in feathers, with an average of 7.04 ng/g, followed by PFBA and PFBS, with averages of 2.17 and 0.99 ng/g, respectively. The PFASs levels were higher in feathers of accipiter than those in other birds, which implied the possible biomagnification of PFASs in this area. These results partly indicated the current situation of PFAS pollution in the Nam Co Basin, especially the existence of short-chain PFASs in this region. In the third part of this dissertation, a terrestrial food chain in Nam Co Basin, plants - plateau pika - accipiter, was employed for studying the occurrences and bioaccumulation/biomagnification of the PFASs. Firstly, because accipiter muscle samples were very precious, we selected chicken muscle as alternative matrix for method optimization. By comparing various extraction solvents, 0.1% formic acid in acetonitrile was selected to extract PFASs in chicken muscle. Combined with WAX cartridge and HPLC-ESI-MS/MS, the method recoveries of PFASs were in the range of 74-121%. And the method recoveries of PFASs were in the range of 72-111% while it was applied to plant samples. PFOS was the predominant perfluorinated pollutants in this ecosystem, and followed by PFBA, which was consistent with the PFASs profile in feather samples. Though there was no significant correlation between PFASs content in accipiter feather and PFASs content in accipiter muscle, the concentration of feather and muscle were in the same order of magnitude. These results implied that PFASs in feathers could reflect the PFASs profile and level in accipiter muscle to some degree. Further, the bioaccumulation/biomagnification of the PFASs was evaluated through the terrestrial food chain, plants - plateau pika – accipiter. We calculated the trophic level these animal through both stomach contents and stable isotope analysis in the present study, and the trophic magnification factors (TMFs) values of PFASs showed biological magnification in this ecosystem. The TMFs of PFBA, PFOS, and PFDA were 1.74, 1.95, and 2.54, respectively, and the TMFs value of PFASs were increased with their carbon chain length in the present study. Moreover, we calculated biological magnification factors (BMFs) between prey and predator. The BMFs values between plateau pika and accipiter reached 7.23, which further confirmed the biomagnification potential of PFASs in this region. However, the studies about PFASs in remote areas are still lacking, more data was needed to reveal mechanism of the long range transport, bioaccumulation, and their sources.
内容类型: 学位论文
URI标识: http://ir.rcees.ac.cn/handle/311016/38652
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

Recommended Citation:
李义莉. 全氟化合物分析方法及其在纳木错流域陆生食物链中富集行为研究[D]. 北京. 中国科学院大学. 2017.
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