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博碩士論文 etd-0725116-165655 詳細資訊
Title page for etd-0725116-165655
論文名稱
Title
東海大陸棚及台灣海峽北部地區底泥岩心中全氟化物之濃度與污染趨勢
Historical trends of perfluorinated compounds from the sediment cores of East China Sea continental shelf and northern Taiwan Strait
系所名稱
Department
畢業學年期
Year, semester
語文別
Language
學位類別
Degree
頁數
Number of pages
85
研究生
Author
指導教授
Advisor
召集委員
Convenor
口試委員
Advisory Committee
口試日期
Date of Exam
2016-06-18
繳交日期
Date of Submission
2016-08-25
關鍵字
Keywords
岩心、全氟辛烷磺酸、全氟辛酸、全氟化物
Core, PFOS, PFOA, PFCs
統計
Statistics
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The thesis/dissertation has been browsed 5683 times, has been downloaded 66 times.
中文摘要
本研究主要調查東海南部大陸棚及台灣海峽北部沿岸河口區域之岩心沉積物,分析岩心樣品中全氟化物分布情形,並了解其對應之河川出海口或港灣地區之汙染物在不同深度的組成比例。分析方法主要使用固相萃取法和高效能液相層析串聯質譜儀(HPLC-MS/MS)檢測全氟化物的濃度含量。
研究結果顯示全部樣品中總全氟化物濃度和岩心深度的關係皆為深度越靠近表層,總全氟化物濃度呈現越高的趨勢,總全氟化物濃度最高的岩心為福建沙埕港附近海域的採樣點(B3),範圍介在ND~0.93 ng/g,濃度最低為長江出海口附近的採樣點(G1),範圍介在ND~0.42 ng/g,沉積物中全氟化物以全氟辛酸(PFOA)和全氟辛烷磺酸(PFOS)為主,這些結果與其它研究區域結果相似。
岩心樣品中總有機碳(total organic carbon, TOC)含量和中值粒徑(median particle size)具有顯著的相關性(r=-0.583, p=0.01),但TOC和總全氟化物相關性偏低。進一步使用主成分分析(PCA)及群集分析(HCA),來探討沉積物中的全氟化物之組成,結果顯示全氟化物分群主要依據PFNA、PFOA和PFOS之組成含量來區分。並加以針對台灣及大陸地區全氟化物的來源比例進行比較,顯示台灣地區全氟化物來源以PFOA、PFOS和PFNA為主,大陸地區則是PFOA為主要來源,這和當地工廠產業有關。
Abstract
Cores collected, along the estuaries and harbors, from the East China Sea continental shelf and northern Taiwan Strait were used to reconstruct historical record of perfluorinated compounds (PFCs) contamination and to investigate the possible sources associated. Solid phase extraction (SPE) and HPLC-MS/MS were used in analyzing the concentration of PFCs. The results show that the concentration decreases with the depth. The range of concentration is ND~0.93 ng/g from B3 (near Fujian Shacheng Harbor) which is the highest among all the cores analyzed; while ND~0.42 ng/g from G1 (near Yangtze River estuary) which is the lowest. Similar to those found in other areas, the major compounds in sediment cores are PFOA and PFOS.
Total organic carbon content (TOC) and median particle size in the samples are found significantly correlated (r=-0.583, p=0.01). The samples in sediment cores, analyzed by principal components analysis (PCA) and hierarchical cluster analysis (HCA), were clustered mainly according to the relative abundance of PFNA, PFOA and PFOS. The abundant compounds in sediment cores near Taiwan are PFOA, PFOS and PFNA; while PFOA for those near China area. This is related to the characteristics of regional industries.
目次 Table of Contents
謝誌 i
摘要 ii
Abstract iii
目錄 iv
圖目錄 vi
表目錄 vii
附錄目錄 viii
第一章 前言 1
1-1研究動機 1
1-2研究目的 2
第二章 文獻回顧 3
2-1全氟化物之用途與特性 3
2-2全氟化物在環境中傳輸與宿命 7
2-3全氟化物對人體之影響 11
2-4岩心沉積物之應用 11
2-5研究區域 12
第三章 研究方法 13
3-1實驗材料與儀器 13
3-1-1實驗材料 13
3-1-2儀器設備 14
3-2採樣與保存方法 14
3-3樣品前處理 16
3-4樣品分析方法 16
3-4-1粒徑分析 16
3-4-2總有機碳(TOC)分析 16
3-4-3全氟化物分析 17
3-5品保與品管(QA/QC) 20
3-5-1 方法回收率 20
3-5-2 實驗空白分析 20
3-5-3 方法偵測極限 20
3-6主成分分析法(Principal components analysis, PCA) 22
3-7階層群及分析法(Hierarchical Cluster Analysis, HCA) 22
第四章 結果與討論 23
4-1總全氟化物之濃度趨勢 23
4-2全氟化物組成比例與來源探討 27
4-3全氟化物濃度與全球文獻比較結果 29
4-4相關性分析 32
4-5主成分分析結果 33
4-6 階層群集分析法結果 34
4-7 比較台灣與大陸地區之全氟化物組成與分布 34
第五章 結論與建議 50
5-1結論 50
5-2建議 51
參考文獻 52
附錄 58
參考文獻 References
3M, 2000. Phase-out Plan for POSF-based Products. U.S. EPA Public Docket, AR226-0600(https://www.fluoridealert.org/wp-content/pesticides/pfos.fr.final.docket.0009.pdf).
Ahrens, L., Gerwinski, W., Theobald, N., Ebinghaus, R., 2010. Sources of polyfluoroalkyl compounds in the North Sea, Baltic Sea and Norwegian Sea: Evidence from their spatial distribution in surface water. Marine Pollution Bulletin 60 (2), 255-260.
Ahrens, L., Shoeib, M., Del Vento, S., Codling, G., Halsall, C., 2011. Polyfluoroalkyl compounds in the Canadian Arctic atmosphere. Environmental Chemistry 8 (4), 399-406.
Ahrens, L., Yamashita, N., Yeung, L.W., Taniyasu, S., Horii, Y., Lam, P.K., Ebinghaus, R., 2009. Partitioning behavior of per-and polyfluoroalkyl compounds between pore water and sediment in two sediment cores from Tokyo Bay, Japan. Environmental science & technology 43 (18), 6969-6975.
Bao, J., Liu, W., Liu, L., Jin, Y., Ran, X., Zhang, Z., 2010. Perfluorinated compounds in urban river sediments from Guangzhou and Shanghai of China. Chemosphere 80 (2), 123-130.
Brooke, D., Footitt, A., Nwaogu, T.A.,, 2004. Environmental risk evaluation report: perfluoroocatnesulphonate. Washington D.C.USEPA.
Chen, M., Covey, M., 1983. Radiocarbon dating of piston cored sediments from the Taiwan Strait: preliminary results. Acta Oceanographica Taiwanica 14, 9-15.
Corsolini, S., Sarkar, S.K., Guerranti, C., Bhattacharya, B.D., Rakshit, D., Jonathan, M.P., Godhantaraman, N., 2012. Perfluorinated compounds in surficial sediments of the Ganges River and adjacent Sundarban mangrove wetland, India. Marine Pollution Bulletin 64 (12), 2829-2833.
Ellis, D.A., Martin, J.W., De Silva, A.O., Mabury, S.A., Hurley, M.D., Sulbaek Andersen, M.P., Wallington, T.J., 2004. Degradation of fluorotelomer alcohols:  a likely atmospheric source of perfluorinated carboxylic acids. Environmental Science & Technology 38 (12), 3316-3321.
EPA, 2014. Emerging contaminants –perfluorooctane sulfonate (PFOS) and perfluorooctanoic acid (PFOA). U.S. EPA Public Docket.
Fujii, S., Polprasert, C., Tanaka, S., Hong Lien, N.P., Qiu, Y., 2007. New POPs in the water environment: distribution, bioaccumulation and treatment of perfluorinated compounds – a review paper. Journal of Water Supply: Research and Technology - Aqua 56 (5), 313-326.
Gómez, C., Vicente, J., Echavarri-Erasun, B., Porte, C., Lacorte, S., 2011. Occurrence of perfluorinated compounds in water, sediment and mussels from the Cantabrian Sea (North Spain). Marine pollution bulletin 62 (5), 948-955.
Giesy, J.P., Kannan, K., 2001. Global distribution of perfluorooctane sulfonate in wildlife. Environmental Science & Technology 35 (7), 1339-1342.
Giesy, J.P., Kannan, K., 2002. Peer reviewed: perfluorochemical surfactants in the environment. Environmental Science & Technology 36 (7), 146A-152A.
Giesy, J.P., Naile, J.E., Khim, J.S., Jones, P.D., Newsted, J.L., 2010. Aquatic toxicology of perfluorinated chemicals, reviews of environmental contamination and toxicology. Springer New York, New York, NY, pp. 1-52.
Guruge, K.S., Taniyasu, S., Yamashita, N., Wijeratna, S., Mohotti, K.M., Seneviratne, H.R., Kannan, K., Yamanaka, N., Miyazaki, S., 2005. Perfluorinated organic compounds in human blood serum and seminal plasma: a study of urban and rural tea worker populations in Sri Lanka. Journal of Environmental Monitoring 7 (4), 371-377.
Hölzer, J., Göen, T., Just, P., Reupert, R., Rauchfuss, K., Kraft, M., Müller, J., Wilhelm, M., 2011. Perfluorinated compounds in fish and blood of anglers at Lake Möhne, Sauerland Area, Germany. Environmental Science & Technology 45 (19), 8046-8052.
Higgins, C.P., Field, J.A., Criddle, C.S., Luthy, R.G., 2005. Quantitative determination of perfluorochemicals in sediments and domestic sludge. Environmental Science & Technology 39 (11), 3946-3956.
Higgins, C.P., Luthy, R.G., 2006. Sorption of perfluorinated surfactants on sediments. Environmental Science & Technology 40 (23), 7251-7256.
Holmström, K.E., Järnberg, U., Bignert, A., 2005. Temporal trends of PFOS and PFOA in guillemot eggs from the Baltic Sea, 1968−2003. Environmental Science & Technology 39 (1), 80-84.
Hyland, J., Balthis, L., Karakassis, I., Magni, P., Petrov, A., Shine, J., Vestergaard, O., Warwick, R., 2005. Organic carbon content of sediments as an indicator of stress in the marine benthos. Marine Ecology Progress Series 295, 91-103.
Kärrman, A., van Bavel, B., Järnberg, U., Hardell, L., Lindström, G., 2006. Perfluorinated chemicals in relation to other persistent organic pollutants in human blood. Chemosphere 64 (9), 1582-1591.
Lechner, M., Knapp, H., 2011. Carryover of perfluorooctanoic acid (PFOA) and perfluorooctane sulfonate (PFOS) from soil to plant and distribution to the different plant compartments studied in cultures of carrots (daucus carota ssp. sativus), Potatoes (solanum tuberosum), and Cucumbers (cucumis sativus). Journal of Agricultural and Food Chemistry 59 (20), 11011-11018.
Loos, R., Locoro, G., Huber, T., Wollgast, J., Christoph, E.H., de Jager, A., Manfred Gawlik, B., Hanke, G., Umlauf, G., Zaldívar, J.-M., 2008. Analysis of perfluorooctanoate (PFOA) and other perfluorinated compounds (PFCs) in the River Po watershed in N-Italy. Chemosphere 71 (2), 306-313.
Ma, R., Shih, K., 2010. Perfluorochemicals in wastewater treatment plants and sediments in Hong Kong. Environmental Pollution 158 (5), 1354-1362.
Martin, J.W., Muir, D.C.G., Moody, C.A., Ellis, D.A., Kwan, W.C., Solomon, K.R., Mabury, S.A., 2002. Collection of airborne fluorinated organics and analysis by gas chromatography/chemical ionization mass spectrometry. Analytical Chemistry 74 (3), 584-590.
Midasch, O., Drexler, H., Hart, N., Beckmann, M.W., Angerer, J., 2007. Transplacental exposure of neonates to perfluorooctanesulfonate and perfluorooctanoate: a pilot study. International Archives of Occupational and Environmental Health 80 (7), 643-648.
Moon, H.-B., Kannan, K., Choi, H.-G., An, Y.-R., Choi, S.-G., Park, J.-Y., Kim, Z.-G., 2010. Concentrations and accumulation features of PCDDs, PCDFs and dioxin-like PCBs in cetaceans from Korean coastal waters. Chemosphere 79 (7), 733-739.
Naile, J.E., Khim, J.S., Hong, S., Park, J., Kwon, B.-O., Ryu, J.S., Hwang, J.H., Jones, P.D., Giesy, J.P., 2013. Distributions and bioconcentration characteristics of perfluorinated compounds in environmental samples collected from the west coast of Korea. Chemosphere 90 (2), 387-394.
Nakata, H., Kannan, K., Nasu, T., Cho, H.-S., Sinclair, E., Takemura, A., 2006. Perfluorinated contaminants in sediments and aquatic organisms collected from shallow water and Tidal Flat Areas of the Ariake Sea, Japan:  environmental fate of perfluorooctane sulfonate in aquatic ecosystems. Environmental Science & Technology 40 (16), 4916-4921.
Nilsson, H., Kärrman, A., Westberg, H., Rotander, A., van Bavel, B., Lindström, G., 2010. A time trend study of significantly elevated perfluorocarboxylate levels in humans after using fluorinated ski wax. Environmental Science & Technology 44 (6), 2150-2155.
Olsen, G.W., Hansen, K.J., Stevenson, L.A., Burris, J.M., Mandel, J.H., 2003. Human donor liver and serum concentrations of perfluorooctanesulfonate and other perfluorochemicals. Environmental Science & Technology 37 (5), 888-891.
Paul, A.G., Jones, K.C., Sweetman, A.J., 2009. A first global production, emission, and environmental inventory for perfluorooctane sulfonate. Environmental Science & Technology 43 (2), 386-392.
Perra, G., Focardi, S.E., Guerranti, C., 2013. Levels and spatial distribution of perfluorinated compounds (PFCs) in superficial sediments from the marine reserves of the Tuscan Archipelago National Park (Italy). Marine Pollution Bulletin 76 (1–2), 379-382.
Prevedouros, K., Cousins, I.T., Buck, R.C., Korzeniowski, S.H., 2006. Sources, fate and transport of perfluorocarboxylates. Environmental Science & Technology 40 (1), 32-44.
Richardson, S.D., 2009. Water Analysis: Emerging contaminants and current issues. Analytical Chemistry 81 (12), 4645-4677.
Roose, P., Brinkman, U.A.T., 2005. Monitoring organic microcontaminants in the marine environment: principles, programmes and progress. TrAC Trends in Analytical Chemistry 24 (11), 897-926.
Schumacher, B.A., 2002. Methods for the determination of total organic carbon (TOC) in soils and sediments. Ecological Risk Assessment Support Center 2002, 1-23.
So, M.K., Yamashita, N., Taniyasu, S., Jiang, Q., Giesy, J.P., Chen, K., Lam, P.K.S., 2006. Health risks in infants associated with exposure to perfluorinated compounds in human breast milk from Zhoushan, China. Environmental Science & Technology 40 (9), 2924-2929.
Strynar, M.J., Lindstrom, A.B., Nakayama, S.F., Egeghy, P.P., Helfant, L.J., 2012. Pilot scale application of a method for the analysis of perfluorinated compounds in surface soils. Chemosphere 86 (3), 252-257.
Thompson, J., Roach, A., Eaglesham, G., Bartkow, M.E., Edge, K., Mueller, J.F., 2011. Perfluorinated alkyl acids in water, sediment and wildlife from Sydney Harbour and surroundings. Marine Pollution Bulletin 62 (12), 2869-2875.
Thomsen, C., Haug, L.S., Stigum, H., Frøshaug, M., Broadwell, S.L., Becher, G., 2010. Changes in concentrations of perfluorinated compounds, polybrominated diphenyl ethers, and polychlorinated biphenyls in Norwegian breast-milk during twelve months of lactation. Environmental Science & Technology 44 (24), 9550-9556.
Tseng, C.-L., Liu, L.-L., Chen, C.-M., Ding, W.-H., 2006. Analysis of perfluorooctanesulfonate and related fluorochemicals in water and biological tissue samples by liquid chromatography–ion trap mass spectrometry. Journal of Chromatography A 1105 (1–2), 119-126.
Wang, Z., Cousins, I.T., Scheringer, M., Buck, R.C., Hungerbühler, K., 2014. Global emission inventories for C4–C14 perfluoroalkyl carboxylic acid (PFCA) homologues from 1951 to 2030, Part I: production and emissions from quantifiable sources. Environment International 70, 62-75.
Wong, C.S., Sanders, G., Engstrom, D.R., Long, D.T., Swackhamer, D.L., Eisenreich, S.J., 1995. Accumulation, inventory, and diagenesis of chlorinated hydrocarbons in Lake Ontario sediments. Environmental science & technology 29 (10), 2661-2672.
Xu, J., Tian, Y.-Z., Zhang, Y., Guo, C.-S., Shi, G.-L., Zhang, C.-Y., Feng, Y.-C., 2013. Source apportionment of perfluorinated compounds (PFCs) in sediments: Using three multivariate factor analysis receptor models. Journal of Hazardous Materials 260, 483-488.
Yamashita, N., Kannan, K., Taniyasu, S., Horii, Y., Petrick, G., Gamo, T., 2005. A global survey of perfluorinated acids in oceans. Marine Pollution Bulletin 51 (8–12), 658-668.
Yeung, L.W.Y., De Silva, A.O., Loi, E.I.H., Marvin, C.H., Taniyasu, S., Yamashita, N., Mabury, S.A., Muir, D.C.G., Lam, P.K.S., 2013. Perfluoroalkyl substances and extractable organic fluorine in surface sediments and cores from Lake Ontario. Environment International 59, 389-397.
Yeung, L.W.Y., So, M.K., Jiang, G., Taniyasu, S., Yamashita, N., Song, M., Wu, Y., Li, J., Giesy, J.P., Guruge, K.S., Lam, P.K.S., 2006. Perfluorooctanesulfonate and related fluorochemicals in human blood samples from China. Environmental Science & Technology 40 (3), 715-720.
Young, C.J., Furdui, V.I., Franklin, J., Koerner, R.M., Muir, D.C.G., Mabury, S.A., 2007. Perfluorinated acids in Arctic snow:  new evidence for atmospheric formation. Environmental Science & Technology 41 (10), 3455-3461.
Zushi, Y., Tamada, M., Kanai, Y., Masunaga, S., 2010. Time trends of perfluorinated compounds from the sediment core of Tokyo Bay, Japan (1950s-2004). Environ Pollut 158 (3), 756-763.
高燕, 傅建捷, 朱娜麗, 王亞韡, 江桂斌, 2013. 東海表層沉積物中全氟化合物污染水平研究, 第七屆全國環境化學學術大會論文集, 貴陽, pp. 58-59.
彭飞, 韩增林, 2014. 东海问题的周边地缘环境解析. 世界地理研究 23 (2), 35-42.
汤婕, 张银龙, 2014. 土壤/沉积物中全氟辛酸 (PFOA), 全氟辛烷磺酸 (PFOS) 吸附–解吸行为研究进展 ①. 土壤 (Soils) 46 (4), 599-606.
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