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研究生:陳重羽
研究生(外文):Chung-Yu Chen
論文名稱:台灣地區主要河川多溴聯苯醚污染分布研究
論文名稱(外文):THE INVESTIGATION ON POLYBROMINATED DIPHENYL ETHERS (PBDEs) POLLUTION OF PRINCIPAL RIVERS IN TAIWAN
指導教授:李俊璋李俊璋引用關係
指導教授(外文):Ching-Chang Lee
學位類別:碩士
校院名稱:國立成功大學
系所名稱:環境醫學研究所
學門:醫藥衛生學門
學類:公共衛生學類
論文種類:學術論文
論文出版年:2005
畢業學年度:93
語文別:中文
論文頁數:175
中文關鍵詞:生物可利用係數魚體底泥多溴聯苯醚主要河川
外文關鍵詞:BSAFfishsedimentPBDEsprincipal rivers
相關次數:
  • 被引用被引用:24
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  • 下載下載:101
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  多溴聯苯醚(polybrominated diphenyl ethers, PBDEs)廣泛的應用於各種民生用品及建築材料作為防火耐燃劑(Brominated flame retardants, BFRs),用以延緩或抑制火災的發生。研究證據顯示PBDEs於製造、使用過程及產品廢棄後可能釋放至環境,經由食物鏈之生物濃縮及累積,對生物及人體健康產生潛在的威脅。近十幾年來,PBDEs在各種環境介質、水生物及人體母乳中的濃度趨勢,有顯著上升甚至呈倍數關係增長,然而台灣環境中PBDEs的分布情形卻缺乏廣泛且深入的瞭解。因此,本研究主要目的在建立河川底泥及魚體中PBDEs之前處理、淨化及高解析層析/高解析質譜儀(HRGC/ HRMS)分析方法,並針對台灣地區主要河川進行枯水及豐水期河川底泥、魚體中22種PBDEs同源物之濃度分布調查,最後希望能建立台灣河川中PBDEs之生物-底泥累積係數(Biota/Sediment Accumulation Factor,BSAF)。研究結果顯示,底泥以toluene為萃取溶劑所得到的回收率較穩定,淨化方面,當增加氧化鋁使用量時,亦同時需要增加流洗溶劑的極性,以確保BDE-209回收率不致過低。底泥淨土基質添加回收率介於101.7%~125.2%;魚體基質添加回收率介於44.9%~221.2%,分析各個樣品中的同位素標幟內標準品回收率介於21%~178%之間。12條河川底泥PBDEs的總平均濃度介於828 pg/g dry wt.~80120 pg/g dry wt.,以八掌溪濃度最高,卑南溪最低。魚體總PBDEs濃度介於1280 pg/g dry wt.~ 33,724 pg/g dry wt.之間,以台灣鏟頜魚(苦花)濃度最高。底泥中22種PBDEs同源物以BDE-209濃度最高,BDE-197、BDE-47、BDE-183、BDE-99次之。魚體中21種PBDEs同源物以BDE-209濃度最高,BDE-47、BDE-100、BDE-154次之。主成份分析顯示,魚類與底泥的相關性高,顯示河川中魚體PBDEs暴露途徑可能是來自底泥。依據所計算之生物可利用係數顯示,以BDE-126生物可利用性最高,在溪哥體內BDE-126的濃度是底泥中的348.93倍。整體而言,以4溴、5溴、6溴同族物的生物可利用性較高。
 Polybrominated diphenyl ethers (PBDEs) are widely used as flame retardants in many kinds of plastic consumer products and building materials to slow down or inhibit the fire hazards. There are growing evidences showed that PBDEs are released to the environment during the manufacture of these chemicals, use of electronic equipments or disposal of consumer products. Recently, environmental problems relating to brominated flame retardants (BFRs) have become a matter of greater concern than ever before, because of the markedly increase in levels of polybrominated diphenyl ethers (PBDEs) were found in environmental media, aquatic organisms and human milk. Several PBDE congeners were potentially bio-accumulated or bio-concentrated in the food chain and may threaten the health of biota and human being. In recent decades, the environmental concentrations of PBDEs show a rapidly increasing trend and even doubling every five years. However, the investigations of this pollutant situation in Taiwan environment are quite lack. This study is aimed to establish the pretreatment, cleanup and analytical methods for the PBDEs in river sediment and fish, and to investigate the levels of twenty two congeners of PBDEs in sediments and fishes from principal rivers in Taiwan. Then the investigated data were used to calculate biota/sediment accumulation factor (BSAF) between fish and sediment. The analytical data shows that toluene is a good solvent for sediment extraction because of it can provide stable 12C-lable-PBDE recovery. In sample clean up test, analytical data shows that the height of the alumina column will affect the recovery of BDE-209. Therefore, we suggested to increase the polarity of the eluting solvent to get good recovery of BDE-209. The recoveries of sediment and fish matrix were ranged from 101.7% to 125.2% and from 44.9% to 221.2% respectively. The recoveries of 13C12-labeled PBDEs congeners in samples are ranged from 21% to 178%. The PBDEs concentrations of the sediments from 12 principal rivers in Taiwan are ranged from 828 pg/g dry wt. to 80120 pg/g dry wt. The highest concentration is founded in Bajhang River, and the lowest is founded in Bei-nan river. The PBDEs concentrations of fish from 12 principal rivers in Taiwan are ranged from 1280 pg/g dry wt. to 33,724 pg/g dry wt.. Taiwan shoveljaw carp (Varicorhinus barbatulus) have highest concentration than other fishes. BDE-209 is the most dominate congener in all the sediment and fish samples. BDE-197, BDE-47, BDE-183, BDE-99 are also the major components in sediment samples, but the major components in fish samples were BDE-47, BDE-100, BDE-154. The results of principal component analysis show that there are high correlation in some PBDEs congeners between fish and sediment. The conclusion suggested that the sediments may have a lot of contribution to the PBDEs levels in fish. According the calculated BSAF in this study, BDE-126 is highly bioavailable congener among 21 PBDEs congeners. The BSAF of BDE-126 in Freshwater minnow (Zacco platypus) are 348.93. Beside BDE-126, the bioavailabilities of tetra-, penta-, hexa-BDE are higher than other homologues.
第一章 諸論 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多溴聯苯醚之物理化學特性 3
2-2多溴聯苯醚的製造、使用及環境宿命 4
2-2-1多溴聯苯醚之製造、使用 6
2-2-2排放來源及排放途徑 7
2-2-3多溴聯苯醚的環境流布 10
2-2-4多溴聯苯醚之生物濃縮及生物可利用性 16
2-3多溴聯苯醚之毒理特性及健康危害 17
2-4環境介質中多溴聯苯醚之檢測方法 21
第三章 研究材料與方法 22
3-1研究對象選取 22
3-2 採樣策略與方法 22
3-2-1 採樣對象 22
3-2-2 採樣地點選取 22
3-2-3 底泥樣本採樣方法 23
3-2-4 魚體樣本採樣方法 24
3-3底泥及魚體樣本前處理方法 24
3-3-1底泥及魚體樣本含水量測定方法 25
3-3-2底泥樣本前處理方法 26
3-3-3魚體樣本前處理方法 28
3-3-4底泥樣本總固體、固定性及揮發性固體含量檢測方法 31
3-4底泥及魚體樣本多溴聯苯醚分析方法 32
3-4-1分析儀器及操作條件 32
3-5樣本數據品質保證及品質管制(QA/QC) 33
3-5-1河川採樣品保品管 33
3-5-2實驗室前處理及分析品保品管 34
3-5-3儀器分析之品保品管 35
3-5-4儀器檢量線 36
第四章 結果與討論 38
4-1分析方法建立 38
4-1-1氧化鋁測試 38
4-1-2檢量線測試 38
4-2 樣本基本資料整理 39
4-3底泥中PBDES濃度值分布 40
4-3-1 12條河川中底泥22種PBDEs同源物濃度分布情形 40
4-3-2 底泥樣本濃度與國外文獻比較 50
4-4魚體中PBDES濃度值分布 51
4-4-1 10條河川魚體21種PBDEs濃度分布 51
4-4-2 魚體樣本濃度與國外文獻比較 55
4-5 PBDES主成分分析(PRINCIPAL COMPONENT ANALYSIS) 55
4-6 河川中PBDES生物可利用係數(BSAF)分析 57
4-6-1 本研究之BSAF和國外文獻比較 58
第五章 結論與建議 60
5-1結論 60
5-2建議 62
參考文獻 …………………………………………………………………... 64
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