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研究生: 林霧霆
Lin, Wu-Ting
論文名稱: PCDD/Fs污染水域水生物及鳥類之 生物濃縮及生物放大研究
The bioconcentration and biomagnification of polychlorinated dibenzo-p-dioxins and dibenzofurans in the aquatic organisms and bird in contaminated area
指導教授: 李俊璋
Lee, Ching-Chang
侯平君
Hou, Ping-Chun
學位類別: 碩士
Master
系所名稱: 醫學院 - 環境醫學研究所
Department of Environmental and Occupational Health
論文出版年: 2004
畢業學年度: 92
語文別: 中文
論文頁數: 244
中文關鍵詞: 生物濃縮生物放大多氯戴奧辛/口夫喃水生物
外文關鍵詞: PCDD/Fs, aquatic organism, bioconcentration, biomagnification
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  •   多氯戴奧辛/口夫喃(polychlorinated dibenzo-p-dioxins/ dibenzofurans, PCDD/Fs)為環境荷爾蒙之一,具備在環境中不易生物或非生物分解之特性,而且由於PCDD/Fs為親脂性化合物,極易透過食物鏈蓄積於動物或人體之脂肪組織。在生態環境中,生物間之關係性以食物鏈最為明顯,人類是位於生態系食物鏈的最高階層,因此人體中化學物質的累積量會相對增加,故欲瞭解PCDD/Fs對人體風險危害時進行生態系中不同階層之累積放大時,經由食物鏈進行PCDD/Fs之生物濃縮與生物放大研究日益重要。
      本研究以受到PCDD/Fs高度污染水域為對象,分析底泥及食物鏈中之各種生物體內17種PCDD/Fs同源物之含量與分布,進而探討不同階級消費者之間PCDD/Fs之生物放大、生物累積之特性。在戴奧辛污染水域選取,本研究以台鹼安順廠區旁之海水貯存池為對象,採集水域中環境樣本(9個底泥),水生物樣本包括蝦(6隻草蝦)、蟹(14隻短槳蟳、紅腳蟳及遠海梭子蟹)和魚體(吳郭魚、虱目魚、大鱗鯔、環球海鰶共100隻),鳥類樣本(小白鷺4隻和夜鷺3隻),樣本經前處理後,以高解析氣相層析儀/高解析質譜儀(HRGC/HRMS)分析17種2,3,7,8-取代之PCDD/Fs同源物,進而探討PCDD/Fs透過食物鏈在各階層之生物濃縮及生物放大之特性。
      研究結果顯示,底泥樣本之PCDD/Fs平均濃度為511,418(89,002~2,298,348)pg/g,在同源物分布上,以,2,3,4,6,7,8-HpCDF、1,2,3,4,6,7,8-HpCDD、OCDF及OCDD為主要同源物,總計佔98.9%,與過去文獻比較,顯示與受PCP污染土壤中PCDD/Fs同源物分布非常類似。生物樣本中PCDD/Fs原始濃度高低順序為蝦子>螃蟹>環球海鰶>虱目魚>吳郭魚>大鱗鯔(80,559~5,260 pg/g lipid)。研究顯示生活習性靠近底泥之生物,如蝦蟹其體內所累積PCDD/Fs濃度較高,尤其在高氯數同源物含量比魚體高出甚多。此外,魚體中肝臟PCDD/Fs濃度比魚肉濃度高。水生物之PCDD/Fs總毒性當量濃度範圍為15.7~123 pg WHO -TEQ/g sample高於歐盟規範濃度(4 pg WHO-TEQ/g sample)約4-38倍。主要毒性當量貢獻來自2,3,4,7,8, -PeCDF與1,2,3,7,8,-PeCDD(蝦蟹:55.7%、魚體:64.8%)。小白鷺及夜鷺PCDD/Fs平均濃度為1519(114~3755) pg/g,夜鷺體內PCDD/Fs濃度高於小白鷺。
      在PCDD/Fs之生物濃縮特性方面,以蝦蟹所含PCDD/Fs所計算之平均生物濃縮係數(Bioconcentration factor, BCF)為148,238(lipid base)及3,783 (sample base);四種魚魚體平均BCF為58,657(lipid base)、3,479(sample base),顯示此污染水域之生物具明顯之PCDD/Fs生物濃縮特性。其中蝦蟹之BCF高於魚體,此差異與物種棲息特性,攝食方式及PCDD/Fs代謝能力有關。數據顯示BCF隨著PCDD/Fs含氯數增加而有下降之情形。而水生物間之生物放大特性,僅在僅2,3,7,8-TCDD、1,2,3,7,8-PeCDD和1,2,3,6,7,8-HxCDF之BMF>1,具有生物放大特性,然而多數同源物無生物放大特性,其原因在魚與蝦蟹間,因所採魚體及蝦蟹均屬較大體型,其營養階層相關性較差所致:至於小白鷺、夜鷺與魚體間,可能與小白鷺、夜鷺均為幼鳥,累積濃縮時間較短及其與大型魚體之營養階層相關性較差有關。探討底泥-水生物累積係數,蝦蟹PCDD/Fs之BSAF 值0.0003~0.2698;魚體魚肉之BSAF值0.00002~0.1009;魚體肝臟之BSAF值0.0003~0.2687。BSAF值在水生物中高低依序:蝦蟹>魚體肝臟>魚體魚肉。數據顯示,BSAF亦依循著PCDD/Fs同源物含氯數增加而遞減之現象,此現象與PCDD/Fs同源物之分子大小(PCDD/Fs含氯數愈高其分子越大,不易被生物體所利用)及PCDD/Fs溶解度(PCDD/Fs含氯數愈高,水中溶解度愈低,底泥中濃度愈高)有關。

      Polychlorinated dibenzo-p-dioxins/dibenzofurans (PCDD/Fs)are kind of environmental hormones。Due to these lipophilic nature chemicals are high potential for accumulation in biological lipid tissue. In the environment, PCDD/Fs will accumulate in animals or human body through the food chain. Human is the top-level consumers in the food web, in order to evaluate the potential risk of PCDD/Fs to humans, it is important to understand the level and characteristics of bioconcentration and biomagnification of PCDD/Fs in the aquatic food web.The aim of this study is to investigate the level and distributions of the PCDD/Fs in sediment, aquatic biota and bird from PCP contaminate area. This study also aimed to provide information on the bioconcentration, biomagnification factors for PCDD/Fs. The samples includes sediments, grass prawn (Penaeus monodon), crab (Portunus pelagicus), Thalamita crenata, Scylla olivacea ), fish (Oreochromis mossambicus, Chanos chanos, Liza macrolepis, Nematolosa come) and bird (Nycticorax nycticorax, Egretta garzett ) were collected from the sea reservoir located near the deserted factory. All samples were after the extraction and cleanup procedures, the quantification of 2,3,7,8-substituted PCDD/Fs is performed with HRGC/HRMS.The concentration of total PCDD/Fs in sediment was 511,418(89,002~2,298,348)pg/g, and 1,2,3,4,6,7,8-HpCDF、1,2,3,4,6,7,8- HpCDD、OCDD and OCDF are the predominant congeners of PCDD/Fs about (98.9%). According the references, the congener profile is very similar then that in the PCP contaminated area. The concentration of aquatic biota is grass prawn>crab>Hairback herring>Salmon herring>Tilapia>Big scale liza(80559~5259.7pg/g lipid). The concentration of PCDD/Fs was found to be higher in the liver tissues of fish than those in muscle tissues. The concentration of PCDD/Fs-TEQ in aquatic biota is 15.7~123 pg WHO-TEQ/g sample which is high than EU(4pg WHO-TEQ/g sample)4-38 fold and the main congeners contribution are 2,3,4,7,8,-PeCDF and 1,2,3,7,8,-PeCDD(shellfish:55.7%、fish:64.8%)。Therefore, the concentration of PCDD/Fs of bird is 1519(114~3755)pg/g lipid, and the concentration of PCDD/Fs in Black-crowned Night Heron is high than Little Egre.
      Furthermore, BCF were estimated the shellfish is 148238(lipid base)、3783(sample base), in fish is 58657(lipid base)、3479(sample base).BMF were estimated from fish to shellfish and bird to fish. The BMF value were estimated higher than 1 in 2,3,7,8-TCDD、1,2,3,7,8-PeCDD and 1,2,3,6,7,8 -HxCDF and there are no biomagnification on other congeners. The reason might be due to the tropic position. The average BSAFs were estimated and range from 0.0003~0.2698 and 0.00002~0.1009 and 0.0003~0.2687 for shellfish, muscle of fish and liver of fish. In the meantime, the BSAF value tended to decrease as the number of chlorines increased on both groups of PCDD and PCDF compound. This might be due to the water solubility of PCDD/Fs and the molercular cross-sectional size of PCDD/Fs.

    目錄 第一章序論…………………………………………………………………………1 1-1研究背景…………………………………………………………………..1 1-2研究目的…………………………………………………………………..2 第二章文獻回顧……………………………………………………………………3 2-1戴奧辛簡介………………………………………………………………..3 2-1-1戴奧辛之物理化學特性…………………………………………..3 2-1-2戴奧辛之來源……………………………………………………..3 2-1-3戴奧辛之毒理特性及健康危害…………………………………..5 2-2 PCDD/Fs之生物濃縮及生物放大特性…………………………………6 2-2-1 PCDD/Fs之生物濃縮之特性…………………………………….7 2-2-2 PCDD/Fs之生物放大之探討…………………………………….8 2-2-3 PCDD/Fs之生物可利用性探討………………………………..10 2-3台鹼安順廠簡介…………………………………………………………12 2-4世界各國底泥、水生物及鳥類PCDD/Fs濃度分佈…………………..12 2-4-1底泥………………………………………………………………13 2-4-2水生物……………………………………………………………14 2-4-3鳥類………………………………………………………………16 第三章研究材料與方法…………………………………………………………..18 3-1研究對象選取……………………………………………………………18 3-2採樣策略…………………………………………………………………18 3-2-1採樣對象…………………………………………………………18 3-2-2採樣地點選取……………………………………………………18 3-2-3採樣時間與頻率…………………………………………………18 3-2-4底泥樣本採樣方法………………………………………………19 3-2-4-1底泥採樣設備…………………………………………….19 3-2-4-2底泥採樣及保存………………………………………….19 3-2-4-3底泥樣本數……………………………………………….19 3-2-5水生物採樣方法…………………………………………………19 3-2-5-1水生物採樣設備………………………………………….19 3-2-5-2水生物採樣方法及保存………………………………….19 3-2-5-3水生物樣本數…………………………………………….20 3-2-6鳥類採樣方法……………………………………………………20 3-2-6-1鳥類採樣設備…………………………………………….20 3-2-6-2鳥類採樣方法及保存…………………………………….20 3-2-6-3鳥類樣本數……………………………………………….21 3-3底泥樣本前處理分析方法………………………………………………21 3-3-1底泥樣本乾燥前處理方法………………………………………21 3-3-2底泥樣本前處理方法……………………………………………21 3-3-3底泥樣本有機物分析方法………………………………………25 3-4生物樣本前處理分析方法………………………………………………25 3-4-1生物樣本保存及前處理方法……………………………………25 3-4-2生物樣本前處理方法……………………………………………26 3-5樣本儀器分析方法………………………………………………………28 3-5-1底泥樣本…………………………………………………………28 3-5-2生物樣本…………………………………………………………29 3-5-3分析儀器及操作條件……………………………………………29 3-5-3-1儀器設備………………………………………………….29 3-5-3-2儀器操作條件設定……………………………………….29 3-6樣本數據品質保證及品質管制(QA/QC)………………………………30 3-6-1採樣及前處理品保品管…………………………………………30 3-6-1-1同位素標記標準品添加…………………………………30 3-6-1-2基質添加標準品驗證……………………………………31 3-6-1-3實驗室空白樣本………………………………………….31 3-6-2儀器分析之品保品管……………………………………………32 3-6-2-1滯留時間(Retention Time)建立………………………..32 3-6-2-2管柱解析度(Column resolution)……………………….32 3-6-2-3儀器靈敏度……………………………………………….33 3-6-3儀器檢量線………………………………………………………33 3-6-3-1檢量線之建立…………………………………………….33 3-6-3-2起始檢量線之建立……………………………………….33 3-6-3-3檢量線查核……………………………………………….34 3-7數據計算方式……………………………………………………………34 第四章結果與討論………………………………………………………………..35 4-1樣本基本資料整理………………………………………………………35 4-1-1底泥樣本資料……………………………………………………35 4-1-2水生物樣本資料…………………………………………………35 4-1-3鳥類樣本資料……………………………………………………36 4-2底泥中PCDD/Fs濃度值分布………………………………………….36 4-2-1 九區底泥PCDD/Fs濃度分布………………………………….36 4-2-2底泥樣本與國內外文獻比較……………………………………37 4-3水生物PCDD/Fs濃度值分布………………………………………….38 4-3-1魚體內PCDD/Fs濃度值分布…………………………………..38 4-3-2四種魚體樣本綜合比較…………………………………………46 4-3-3魚體樣本與國內外文獻比較……………………………………49 4-3-4甲殼類體內PCDD/Fs濃度值分布…………………………….49 4-4鳥類PCDD/Fs濃度值分布……………………………………………..51 4-4-1 小白鷺PCDD/Fs分析結果…………………………………….51 4-4-2夜鷺PCDD/Fs分析結果………………………………………..52 4-4-3鳥類樣本國內外文獻比較………………………………………53 4-5污染水域各項介質之PCDD/Fs分布比較…………………………….53 4-5-1底泥V.S.蝦蟹…………………………………………………….53 4-5-2底泥V.S.魚體(魚肉和肝臟)…………………………………….54 4-5-3鳥V.S.魚體V.S.蝦蟹…………………………………………….55 4-6污染水域PCDD/Fs生物濃縮(BCF)係數分析………………………..56 4-6-1甲殼類PCDD/Fs生物濃縮係數分析…………………………..56 4-6-2魚類PCDD/Fs生物濃縮分析…………………………………..56 4-6-3本研究BCF與國外文獻比較…………………………………...57 4-7污染水域PCDD/Fs生物放大(BMF)係數分析……………………….58 4-7-1魚體對蝦蟹PCDD/Fs生物放大係數分析……………………..58 4-7-2鳥對魚體PCDD/Fs生物放大係數分析………………………..59 4-7-3本研究BMF和國外文獻比較…………………………………...60 4-8污染水域PCDD/Fs生物可利用性係數(BSAF)分析…………………60 4-8-1甲殼類PCDD/Fs之BSAF係數………………………………...60 4-8-2魚類PCDD/Fs之BSAF係數分析……….……………………61 4-8-3本研究之BSAF和國外文獻比較……………………………….62 第五章結論與建議………………………………………………………………..63 5-1結論………………………………………………………………………63 5-2建議………………………………………………………………………65 參考文獻…………………………………………………………………………..66

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