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系統識別號 U0026-0812200913515366
論文名稱(中文) 環境介質對草料中多氯戴奧辛/呋喃濃度之影響及貢獻量評估
論文名稱(英文) The study on PCDD/Fs transportation and contribution from environmental media to forages
校院名稱 成功大學
系所名稱(中) 環境醫學研究所
系所名稱(英) Institute of Environmental and Occupational Health
學年度 95
學期 2
出版年 96
研究生(中文) 陳義賜
研究生(英文) Yi-tzu Chen
電子信箱 S7693102@mail.ncku.edu.tw
學號 s7693102
學位類別 碩士
語文別 中文
論文頁數 200頁
口試委員 口試委員-鄭福田
口試委員-蘇慧貞
口試委員-張艮輝
口試委員-黃英豪
指導教授-李俊璋
中文關鍵字 多氯戴奧辛/呋喃  主成分分析  土壤  空氣  草料 
英文關鍵字 PCA  soil  air  forages  PCDD/Fs 
學科別分類
中文摘要 過去調查顯示,市售牛羊肉品及乳品中多氯戴奧辛/呋喃(Polychlorinated dibenzo-p-dioxin/furans, PCDD/Fs)之含量與草料(牧草及玉米)之PCDD/Fs含量有關,牛羊若以高PCDD/Fs含量之草料為食物,所生產牛羊肉品及乳品之PCDD/Fs含量亦偏高,顯示如欲降低牛羊肉品及乳品之PCDD/Fs含量,需先瞭解草料所含PCDD/Fs之來源及貢獻量。本研究以玉米及尼羅草為例,藉由草區各環境介質(空氣、落塵及土壤)與草料中PCDD/Fs特徵成分含量之調查解析,探討PCDD/Fs進入草料之傳輸路徑,並評估各種環境介質對草料中PCDD/Fs之貢獻量。本研究參考環保署環境檢驗所公告之NIEA A809.10B及NIEA S102.61B進行空氣及土壤採樣,並依據NIEA A810.11B、NIEA M801.11B及美國環保署M1613B等方法進行樣本前處理後,以高解析氣相層析儀/高解析質譜儀(HRGC/HRMS)進行17種PCDD/Fs濃度之分析,最後以主成分分析(Principal Component Analysis, PCA)及美國環保署多介質模式(Multiple Medium Model)推估環境介質對草料中PCDD/Fs之貢獻量。
本研究以2個玉米產區及2個尼羅草產區為研究對象,於草料生長區域及周界設置空氣及土壤採樣點,並於草料生長期間每月進行乙次各種樣本之採樣,研究期間共完成空氣(氣固相)、土壤、草料樣本各12個與落塵樣本7個之17種PCDD/Fs分析。研究結果顯示空氣中PCDD/Fs平均濃度及範圍為0.097(0.032-0.284)pg I-TEQ/Nm3、土壤中PCDD/Fs平均濃度及範圍為1.17(0.495-2.36)pg I-TEQ/g d.w.、落塵中PCDD/Fs平均濃度及範圍為26.52(4.13-55.3)pg I-TEQ/g d.w.、玉米中PCDD/Fs平均濃度及範圍為0.762(0.183-1.50)WHO98-TEQDF/g (12% water)、尼羅草中PCDD/Fs平均濃度及範圍為0.667(0.138-1.50)WHO98-TEQDF/g (12% water),且草料中PCDD/Fs濃度隨生長期增長有降低之趨勢,所有最終收割之成品均符合歐盟之規範。由環境介質與草料中PCDD/Fs同源物分布比較顯示,落塵與草料皆以OCDD、OCDF、1,2,3,4,6,7,8-HpCDF、1,2,3,4,6,7,8-HpCDD等高氯數同源物為主要同源物;草料與土壤在OCDD、OCDF、1,2,3,4,6,7,8-HpCDF、1,2,3,4,6,7,8-HpCDD皆高;而空氣中氣固相PCDD/Fs與草料中PCDD/Fs同源物分布比較,亦可發現草料與空氣固相中高氯數同源物分布較為相似,而草料與空氣氣相中低氯數PCDFs相似,顯示草料在低氯數PCDFs可能受到空氣氣相的影響。進一步進行主成分分析後,結果顯示東光國小之玉米與環境介質之第一及第二主成分共可解釋70.7%的變異,且玉米與落塵及空氣氣相之相關程度較高;建華國小之玉米與環境介質之第一及第二主成分共可解釋68.1%的變異,且玉米與落塵及空氣固相之相關程度較高,進而推測由於玉米為高莖作物,所以受到空氣中PCDD/Fs濃度之影響較大。而尼羅草與環境介質之第一及第二主成分共可解釋83. 5%的變異,且與土壤及落塵之相關程度較高。推測兩種草料差異之原因,應是尼羅草株高約60公分後會傾斜,而較接近地面易受落塵及土壤揚塵所含PCDD/Fs之影響。最後,以USEPA多介質模式進行貢獻量之推估,結果顯示玉米與尼羅草皆以乾濕沈降之貢獻量大於空氣氣相吸附之貢獻量,其中空氣氣相吸附對草料之平均貢獻量為17.9%,而乾濕沈降為82.1%,表示草料中PCDD/Fs含量主要來自乾濕沈降量。
英文摘要 The past investigations showed that the PCDD/F levels of beef, mutton and milk were related to PCDD/F levels of forages (grass and maize). If cattle or sheep were fed with forages contained high PCDD/Fs levels, the PCDD/F levels in the beef, mutton and milk would be increased. It revealed that if we would like to reduce PCDD/Fs levels in these products, we should identify the PCDD/Fs contamination sources of the forages and their contribution. In this study, maize and nilegrass were selected as study subjects, and congener patterns of PCDD/Fs in environmental media (ambient air, dust fall and soil) and forages (maize and nilegrass) were analyzed and assessed for identification of the transfer pathway and sources contribution from environmental media into forages. Methods of NIEA A809.10B and NIEA S102.61B were referred to implement air and soil sampling, and then the PCDD/F levels of samples were analyzed according to Methods of NIEA A810.11B, NIEA M801.11B and USEPA M1613B. Principal Component Analysis (PCA) and USEPA Multiple Medium Model were used to assess the association between PCDD/Fs congeners and levels of environmental media and forages and the contribution of environmental media to forages respectively.
Two maize and two nilegrass production areas were selected as study areas, and the air, dust fall and soil samples were monthly sampled around the production areas during growing period of the forages. In this study, 12 airborne (gas and particle), 12 soil, 12 forages and 7 dust fall samples were collected and analyzed for 17 PCDD/Fs. The results showed average airborne PCDD/Fs levels was 0.097(0.032-0.284)pg I-TEQ/Nm3,and 1.17(0.495-2.36)pg I-TEQ/g d.w. in soil, 26.52(4.13-55.3)pg I-TEQ/g d.w. in dust fall, 0.762(0.183-1.50)WHO98-TEQDF/g (12% water) in maize and 0.667(0.138-1.50)WHO98-TEQDF/g (12% water) in nilegrass. Besides, the PCDD/Fs levels in forages decreased with plant growing, and all harvested plants were below the maximum limits of European Union (EU) for dioxin in feedingstuffs. After comparing PCDD/Fs congener patterns between environmental media and forages, the results showed that the PCDD/Fs congener profile of dust fall and forages were both dominated by highly chlorinated PCDD/Fs such as OCDD, OCDF, 1,2,3,4,6,7,8-HpCDF,and 1,2,3,4,6,7,8-HpCDD. Forages and soil were both dominated by OCDD、OCDF、1,2,3,4,6,7,8-HpCDF、1,2,3,4,6,7,8-HpCDD, these data showed that forages may be influenced by soil within these congeners. When comparing the PCDD/Fs congener patterns between forages and gas-particle phase of air, it showed the high chlorinated congener profile of forages was similar with particle phase, but the lower chlorinated congener profile of forages were similar with gas phase within PCDFs. All the data were further analyzed by PCA. At one site of maize production area, the results showed that the first and second principal components could account for a total of 70.7% of the variance, and maize was more related to gaseous phase PCDD/Fs and dust fall. At the other site of maize production area, the PCA results showed the first and second principal components could accounted for a total of 68.1% of the variance, and maize was related to dust fall and particle phase PCDD/Fs. Hence, maize was mainly influenced by airborne PCDD/Fs and dust fall because maize was high-stem crop. On nilegrass, the first and second principal components of nilegrass and environmental media could account for a total of 83.5% of the variance, and nilegrass was more related to soil and dust fall. When nilegrass grew up to 60 cm, it will bend and be closer to the ground, and therefore nilegrass will easily affected by dust fall and re-suspension of soil. Finally we used Multiple Medium Model to assess contribution of environmental media, and the result showed the PCDD/Fs contribution from dry and wet deposition was higher than gas phase PCDD/Fs sorption for both maize and nilegrass. The average contribution of gas phase PCDD/Fs to the forages was 17.9% and 82.1% from dry and wet deposition, indicating that the PCDD/Fs levels in forages mainly came from dry and wet deposition.
論文目次 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 戴奧辛之來源及特性 3
2-1-1 戴奧辛之物理、化學特性 3
2-1-2 戴奧辛的來源 3
2-1-3 戴奧辛之毒性當量 5
2-2 戴奧辛之環境流布 6
2-2-1 戴奧辛於空氣中之流布機制 6
2-2-2 戴奧辛於土壤中之流布情形 9
2-2-3 戴奧辛於水體中之流布情形 10
2-3 戴奧辛進入植物之傳輸路徑 10
2-3-1 空氣-植物傳輸路徑之探討 11
2-3-2 土壤-植物傳輸路徑之探討 12
第三章、研究材料與方法 14
3-1 研究對象選取 14
3-2 採樣策略與方法 14
3-2-1 採樣地點選擇 14
3-2-2 採樣時間與頻率 14
3-2-3 空氣樣本採樣方法 15
3-2-4 土壤樣本採樣方法 16
3-2-5 落塵樣本採樣方法 16
3-2-6 草料樣本採樣方法 17
3-3 樣本分析方法 17
3-3-1 空氣樣本中氣固相PCDD/Fs前處理分析方法 18
3-3-2 土壤樣本中PCDD/Fs前處理分析方法 18
3-3-3 落塵樣本中PCDD/Fs前處理分析方法 18
3-3-4 草料樣本中PCDD/Fs前處理分析方法 18
3-4 儀器分析方法 19
3-5 分析方法之相關品質保證及品質管制(QA/QC) 19
3-5-1 同位素標記化合物添加 20
3-5-2 基質添加樣品測試 20
3-5-3 空白樣品測試 21
3-6 儀器檢量線 22
3-6-1 檢量線建立 22
3-6-2 起始檢量線建立 22
3-6-3 檢量線中點查核 23
3-7 數據計算方式 23
3-8 主成分分析(PCA, Principal Component Analysis) 24
3-9 USEPA多介質模式 24
第四章、結果與討論 26
4-1 空氣中戴奧辛採樣及分析結果 26
4-2 土壤中戴奧辛採樣分析結果 30
4-3 草料樣本戴奧辛含量分析結果 33
4-4 落塵中戴奧辛採樣及分析結果 37
4-5 環境介質與草料(玉米及尼羅草)之綜合分析 39
4-5-1 空氣綜合分析 39
4-5-2 土壤綜合分析 40
4-5-3 草料綜合分析 40
4-5-4 落塵綜合分析 41
4-5-5 各採樣點環境介質與草料中戴奧辛同源物分布比較 42
4-5-6 各介質中PCDFs/PCDDs比值分析 49
4-5-7 主成分分析結果 51
4-5-8 貢獻量推估結果 52
第五章、結論與建議 54
5-1 結論 54
5-2 建議 55
參考文獻 56
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