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系統識別號 U0026-0808201721353700
論文名稱(中文) 室內粉塵中內分泌干擾活性、磷系阻燃劑、溴化阻燃劑、與多環芳香烴之檢測
論文名稱(英文) Detection of endocrine disrupting activities, organophosphorus flame retardants, brominated flame retardants and polycyclic aromatic hydrocarbons in indoor dust
校院名稱 成功大學
系所名稱(中) 環境工程學系
系所名稱(英) Department of Environmental Engineering
學年度 105
學期 2
出版年 106
研究生(中文) 李振華
研究生(英文) Chen-Hua Lee
學號 P56041196
學位類別 碩士
語文別 中文
論文頁數 107頁
口試委員 指導教授-周佩欣
口試委員-柯風溪
口試委員-曾美郡
中文關鍵字 室內粉塵  內分泌干擾活性  基因毒性  多環芳香烴  多溴二苯醚  有機磷阻燃劑  基因報導酵母菌試驗法  氣相層析質譜儀 
英文關鍵字 Endocrine disrupting chemicals  Indoor dust  Yeast-based repoter gene assays  PAHs  Flame retardants 
學科別分類
中文摘要 本研究使用基因重組酵母菌生物試驗法檢測室內粉塵之類(抗)雌激素活性、類(抗)雄激素活性、類(抗)甲狀腺激素活性、芳香烴受體促進活性與基因毒性,並以氣相層析質譜儀與液相層析串聯式質譜儀分析室內粉塵中多環芳香烴 (PAHs)、多溴二苯醚 (PBDEs)、有機磷阻燃劑 (OPFRs)、雙酚A (BPA)、三氯沙 (TCS)、壬基酚 (NP)與雙酚S (BPS)之濃度。生物試驗結果顯示,芳香烴受體促進活性 (156-13766 ng β-NF-EQ/g)可於所有室內粉塵中測得,且於1、27、29、6、及11個粉塵樣本中檢測出類雌激素活性 (145 ng E2-EQ/g)、抗雌激素活性 (10-389 µg 4-OHT-EQ/g)、抗雄激素活性 (376-11736 μg FLU-EQ/g)、抗甲狀腺激素活性 (21-1220 mg DEHP-EQ/g)與基因毒性。
儀器分析結果顯示,PAHs、PBDEs、OPFRs、BPA與NP可於所有粉塵樣本中檢測出,TCS與BPS則於22與16個粉塵樣本中檢測出。本研究測得之51種PAHs濃度之中位數 (2637 ng/g)相較其他國家稍微偏低,並以低分子量之含2-3個苯環的PAHs為主,由BaA/(BaA+(C+T))與IcdP/(IcdP+BghiP)之比率推估其污染來源為燃燒所產生。粉塵樣本中PBDEs濃度之中位數 (3777 ng/g)與他國相似,多以BDE209為主。OPFRs測得濃度之中位數 (2125 ng/g)與其他國家相比差異不大,其中TPhP可於所有粉塵樣本中檢測出,而TnBP、TDCPP、TCEP則分別可於20、19、9個樣本中測得。BPA、TCS、NP與BPS濃度之中位數 (2684、986、2234與294 ng/g)與其他國家文獻結果相似。
粉塵樣本中PAHs之芳香烴受體促進活性貢獻介於0.5-62.2%,顯示粉塵中還有其他芳香烴受體促進物質。BPA、TCS及NP的抗雄激素活性貢獻度約0.02-2.2%、0.22-47.6%及0.09-8.7%。此外,本研究利用生物試驗法發現OPFRs具有抗雌激素、抗雄激素及抗甲狀腺激素活性,然而其活性貢獻約只有0.002-0.7%、0.02-7.8%及0.002-0.8%,顯示檢測之4種OPFRs並不是樣本中內分泌干擾活性的主要來源。
將儀器分析檢測之PBDEs與OPFRs進行暴露量評估後,可得知暴露於本研究採集之室內粉塵中並不會危害身體健康,但教室與住家粉塵中的BDE209及TDCPP對於高暴露量之嬰幼兒已超過10%參考劑量,應注意其他暴露途徑,避免超過參考劑量標準。
英文摘要 Many kinds of endocrine disrupting chemicals are used in our daily lives, including plasticizers and flame retardants. This study examined whether indoor dust samples collected from Taiwan may show estrogen receptor (ER), androgen receptor (AR), thyroid hormone receptor (TR), aryl hydrocarbon receptor (AhR) disrupting activities, and genotoxicity using in vitro bioassays. The concentrations of legacy pollutants and flame retardants, such as polycyclic aromatic hydrocarbon (PAHs), polybrominated diphenyl ethers (PBDEs), organophosphorus flame retardants (OPFRs), bisphenol A (BPA), triclosan (TCS) and nonylphenol (NP) were also analyzed by gas chromatography mass spectrometry and liquid chromatography tandem mass spectrometry. Thirty indoor dust samples were collected from classrooms (4 sites), laboratories (3 sites), offices (4 sites), and houses (10 sites). Bioassay results revealed that ER antagonist, AR antagonist, TR antagonist and AhR agonist activities and genotoxicity were often detected in indoor dust samples, whereas no ER, AR or TR agonist activities were found except one sample. PAHs showed about 0.5~62.2% contributions to AhR agonist activities. BPA, TCS, NP and OPFRs although they exhibited estrogenic, anti-estrogenic, anti-androgenic or anti-thyroid hormone activities, were only minor contributors to the endocrine disrupting activities detected in indoor dust samples using bioassays. Accroding to exposure assessment, daily intake values of PBDEs and OPFRs were lower than the reference doses. It is important to reduce the accumulation of dust in indoor environment to avoid dust exposure, particularly for pregnant women, babies and toddlers.
論文目次 摘要 I
Abstract III
誌謝 VI
目錄 VII
表目錄 XI
圖目錄 XIII
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 內分泌干擾物質 3
2-1-1 類(抗)雌激素物質 3
2-1-1-1 類雌激素物質 3
2-1-1-2 抗雌激素物質 5
2-1-2 類(抗)雄激素物質 6
2-1-2-1 類雄激素物質 6
2-1-2-2 抗雄激素物質 7
2-1-3 類(抗)甲狀腺激素物質 8
2-1-3-1 類甲狀腺激素物質 8
2-1-3-2 抗甲狀腺激素物質 9
2-1-4 芳香烴受體促進物質 10
2-1-5 基因毒性物質 11
2-2 多環芳香烴 (PAHs)之特性與危害 12
2-3防火阻燃劑 13
2-3-1 有機磷阻燃劑之特性與危害 13
2-3-2 溴化阻燃劑之特性與危害 15
2-4 生物試驗法 16
2-4-1 活體內生物試驗 16
2-4-2 活體外生物試驗 17
2-5 儀器分析法 18
2-6 暴露量評估 20
第三章 實驗方法與步驟 21
3-1 樣本採集 21
3-2 實驗材料及設備 23
3-2-1 實驗材料 23
3-2-2 實驗設備 25
3-3 實驗流程及方法 27
3-4 樣本前處理 28
3-5 報導基因重組酵母菌試驗法 30
3-5-1 檢測方法 30
3-5-2 類(抗)雌激素活性試驗 33
3-5-3 類(抗)雄激素/甲狀腺激素活性試驗 36
3-5-4 芳香烴受體促進活性試驗 38
3-5-5 基因毒性試驗 40
3-6 層析儀器分析 44
3-6-1 氣相層析質譜儀 (GC-MS) 44
3-6-2 液相層析串聯式質譜儀 (LC-MS/MS) 45
3-6-3 質譜儀資料分析與計算 47
第四章 結果與討論 49
4-1 內分泌干擾活性 49
4-1-1 類(抗)雌激素活性 49
4-1-2 類(抗)雄激素活性 50
4-1-3 類(抗)甲狀腺激素活性 51
4-1-4 芳香烴受體促進活性 52
4-1-5 基因毒性 54
4-2 氣相層析質譜儀與液相層析串聯式質譜儀分析 55
4-2-1 粉塵中多環芳香烴濃度 55
4-2-2 粉塵中多溴二苯醚濃度 57
4-2-3 粉塵中有機磷阻燃劑濃度 59
4-2-4 粉塵中雙酚A、三氯沙、壬基酚、雙酚S與雙酚F濃度 61
4-3 生物試驗法與儀器分析法綜合討論 63
4-4 暴露量計算 72
第五章 結論與建議 75
5-1 結論 75
5-2 建議 76
參考文獻 77
附錄 94
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