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系統識別號 U0026-2603202023464500
論文名稱(中文) 臺灣國小室內粉塵中內分泌干擾活性及有機磷阻燃劑之檢測
論文名稱(英文) Detection of endocrine disrupting activities and organophosphate flame retardants in Taiwanese elementary schools
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 108
學期 2
出版年 108
研究生(中文) 葉文琪
研究生(英文) Wen-Chi Yeh
學號 P56064160
學位類別 碩士
語文別 中文
論文頁數 131頁
口試委員 指導教授-周佩欣
口試委員-廖寶琦
口試委員-趙浩然
中文關鍵字 室內粉塵  內分泌干擾活性  報導基因生物試驗法  有機磷阻燃劑  液相層析串聯式質譜儀 
英文關鍵字 Endocrine disrupting chemicals  Indoor dust  Organophosphate flame retardants  Yeast-based reporter gene assays  Liquid chromatography tandem mass spectrometry 
學科別分類
中文摘要 室內環境中存在著各種不同的化學物質,許多具致癌性或造成生物體內分泌系統紊亂之物質可能吸附於室內粉塵之上,對於長時間待在室內的現代人產生威脅。
為了解國小室內粉塵中是否含有內分泌干擾物質,本研究利用基因重組酵母菌試驗法檢測粉塵樣本之多種內分泌干擾活性,包含類(抗)雄激素活性、類(抗)甲狀腺激素活性、類(抗)糖皮質激素活性以及芳香烴受體促進活性,亦利用液相層析串聯式質譜儀分析國小室內粉塵樣本中有機磷阻燃劑及其他內分泌干擾物質之濃度。本研究共採集20個國小教室室內粉塵樣本,以及4個幼稚園室內粉塵樣本作為對照組。生物試驗法結果顯示,所有的粉塵樣本都具有明顯的抗糖皮質激素活性 (26.4-589.4 µg TeCBPA -EQ/g)及芳香烴受體促進活性 (790.5-43734.6 ng β-NF-EQ/g),21個粉塵樣本具有抗雄激素活性 (454.5-802.1 μg FLU-EQ/g),3個粉塵樣本具有抗甲狀腺激素活性 (144.9-4549 μg BHT-COOH-EQ/g)。
儀器分析有機磷阻燃劑之結果顯示,除了2個室內粉塵樣本未檢測到磷酸三(2-氯乙基)酯之外,本研究所選擇之目標有機磷阻燃劑幾乎於所有的室內粉塵中都可檢測到。國小室內粉塵中有機磷阻燃劑之濃度分布為磷酸三(2-氯乙基)酯 (ND-227.4 ng/g)、磷酸三(1-氯-2-丙基)酯 (266.99-6807.36 ng/g)、磷酸三(1,3-二氯異丙基)酯 (61.5-614.95 ng/g)、磷酸三苯酯 (239.82-3650.8 ng/g)、磷酸三正丁酯 (1126.77-7638.6 ng/g)及磷酸三(丁氧基乙)酯 (382-1050000 ng/g)。其中,於幼稚園粉塵樣本中測得較高的磷酸三(丁氧基乙)酯濃度,可能為該教室地板曾經使用含有該物質之拋光臘進行保養。此外,磷酸三正丁酯和磷酸三苯酯之濃度在不同室內環境之間呈現顯著正相關 (r = 0.74),可能為具有相同的污染源。
儀器分析常見內分泌干擾物質之結果顯示,除了1個室內粉塵樣本未檢測到對羥基苯甲酸甲酯之外,其餘樣本皆有檢測到對羥基苯甲酸甲酯 (12.6-296.5 ng/g)、對羥基苯甲酸丙酯 (82.8-4552 ng/g)、雙酚A (341.4-353.8 ng/g)以及三氯沙 (36.6-287.4 ng/g)。然而,僅各有2個樣本測得單氯雙酚A (33.1 ng/g、31.4 ng/g)和四氯雙酚A (30 ng/g、90.6 ng/g),其餘樣本皆未測得對羥基苯甲酸甲酯及雙酚A之氯化產物。此外,本研究之國小室內粉塵樣本中,對羥基苯甲酸甲酯與對羥基苯甲酸丙酯之濃度僅有中度正相關 (r = 0.42),因此其污染來源可能不盡相同。
具有抗甲狀腺激素活性之3個粉塵樣本中,磷酸三正丁酯及磷酸三(1,3-二氯異丙基)酯之抗甲狀腺激素活性貢獻度介於0.0013-0.0333%。此外,所有國小室內粉塵樣本中,磷酸三正丁酯、磷酸三(1,3-二氯異丙基)酯、磷酸三(丁氧基乙)酯、磷酸三苯酯之抗糖皮質激素活性貢獻度介於0.012-5.3%,顯示檢測之4種有機磷阻燃劑並非樣本中抗糖皮質激素活性的主要來源。
粉塵樣本之暴露評估結果則顯示,室內粉塵中有機磷阻燃劑對成人之危害指數皆小於1。然而,於幼稚園粉塵樣本中測得高濃度的磷酸三(丁氧基乙)酯對孩童之總暴露量則明顯高於其參考劑量,且其危害指數大於1,顯示其對孩童具有危害風險。
英文摘要 Indoor dust, which is absorbed by human body via inhalation or ingestion, may contain carcinogenic or endocrine disrupting substances and pose a threat to people staying indoors for a long time. To understand the occurrence of endocrine disrupting compounds in indoor dust of Taiwan, this study used bioassays to detect androgen receptor (AR), glucocorticoid receptor (GR), thyroid hormone receptor (TR) and aryl hydrocarbon receptor (AhR) disrupting activities in dust collected from Taiwanese elementary schools. Concentrations of methyl 4-hydroxybenzoate (MeP) and their chlorinated derivatives, n-propyl 4-hydroxybenzoate (PrP), bisphenol A (BPA) and their chlorinated derivatives, triclosan (TCS) and 6 organophosphate flame retardants (OPFRs), including tri-n-butyl phosphate (TnBP), triphenyl phosphate (TPhP), tributoxyethyl phosphate (TBEP), tris(2-chloroethyl) phosphate (TCEP), tris(2-chloro-1-methylethyl) phosphate (TCPP), and tris(1,3-dichloro-2-propyl) phosphate (TDCPP) in indoor dust samples were also analyzed by liquid chromatography-tandem mass spectrometry. Bioassay results showed that significant GR antagonist and AhR agonist activities were detected in all indoor dust samples, whereas no AR/GR/TR agonist activities were found in any dust samples. Instrumental results revealed that 6 OPFRs, MeP, PrP, BPA and TCS were often detected in Taiwanese elementary schools. Our findings suggested that the issue of endocrine disrupting substances and emerging contaminants in indoor environment cannot be ignored.
論文目次 目錄
摘要 I
誌謝 VII
目錄 IX
表目錄 XIV
圖目錄 XVII
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)雄激素物質 3
2-1-1-1 類雄激素物質 3
2-1-1-2 抗雄激素物質 4
2-1-2 類(抗)甲狀腺激素物質 5
2-1-2-1 類甲狀腺激素物質 5
2-1-2-2 抗甲狀腺激素物質 6
2-1-3 類(抗)糖皮質激素物質 8
2-1-3-1 類糖皮質激素物質 8
2-1-3-2 抗糖皮質激素物質 10
2-1-4 芳香烴受體促進物質 11
2-2 酚類抗氧化劑 12
2-2-1 天然酚類抗氧化劑 13
2-2-2 合成酚類抗氧化劑 14
2-3 防火阻燃劑 17
2-3-1 有機磷阻燃劑之特性與危害 18
2-3-2 室內環境中之有機磷阻燃劑 20
2-3-3 溴化阻燃劑之特性與危害 23
2-4 其他常見之新興污染物 24
2-4-1 對羥基苯甲酸甲酯 24
2-4-2 對羥基苯甲酸丙酯 24
2-4-3 雙酚A 24
2-4-4 三氯沙 25
2-5 生物試驗法 27
2-5-1 活體內生物試驗 27
2-5-2 活體外生物試驗 28
2-5-2-1 酵素連結免疫吸附法 (ELISA) 28
2-5-2-2 細胞增殖試驗法 (E-Screen assay) 30
2-5-2-3 報導基因試驗法 (Reporter gene assay) 30
2-6 儀器分析法 31
2-6-1 層析儀器 32
2-6-2 偵測儀器 33
2-7 暴露量評估 35
第三章 實驗方法與步驟 39
3-1 樣本採集 39
3-2 實驗材料及設備 40
3-2-1 實驗材料 40
3-2-2 實驗設備 42
3-3 實驗流程及方法 44
3-4 樣本前處理 45
3-5 報導基因重組酵母菌試驗法 46
3-5-1 類(抗)雄激素/甲狀腺激素/糖皮質激素活性試驗 46
3-5-1-1 酵母菌培養 47
3-5-1-2 酵母菌與樣本共培養 47
3-5-1-3 ONPG代謝呈色反應 47
3-5-2 芳香烴受體促進活性試驗 48
3-5-2-1 酵母菌培養 48
3-5-2-2 酵母菌與樣本共培養 48
3-5-2-3 β-gal代謝ONPG呈色反應 48
3-5-3 類(抗)雄激素/甲狀腺激素/糖皮質激素活性計算 51
3-6 儀器分析 51
3-6-1 液相層析串聯式質譜儀 51
3-6-2 回收率及偵測極限 56
第四章 結果與討論 58
4-1 SPAs之內分泌干擾活性 58
4-1-1 類(抗)雄激素活性 59
4-1-2 類(抗)甲狀腺激素活性 60
4-1-3 類(抗)糖皮質激素活性 61
4-1-4 芳香烴受體促進活性 62
4-2 OPFRs之內分泌干擾活性 64
4-3 國小室內粉塵中之內分泌干擾活性 65
4-3-1 類(抗)雄激素活性 65
4-3-2 類(抗)甲狀腺激素活性 66
4-3-3 類(抗)糖皮質激素活性 67
4-3-4 芳香烴受體促進活性 68
4-3-5 內分泌干擾活性綜合討論 69
4-4 國小室內粉塵中之OPFRs濃度分析 71
4-4-1 國小室內粉塵中TnBP濃度 71
4-4-2 國小室內粉塵中TPhP濃度 72
4-4-3 國小室內粉塵中TCEP濃度 73
4-4-4 國小室內粉塵中TCPP濃度 74
4-4-5 國小室內粉塵中TDCPP濃度 75
4-4-6 國小室內粉塵中TBEP濃度 76
4-4-7 室內粉塵中OPFRs濃度之綜合討論 78
4-5 OPFRs之暴露評估分析 83
4-6 國小室內粉塵中之其他新興污染物濃度分析 85
4-6-1 國小室內粉塵中MeP及氯化MeP濃度 85
4-6-2 國小室內粉塵中PrP濃度 86
4-6-3 國小室內粉塵中BPA及氯化BPA濃度 87
4-6-4 國小室內粉塵中TCS濃度 89
4-6-5 室內粉塵中新興污染物濃度之綜合討論 90
4-7 生物試驗法與儀器分析法之綜合討論 93
第五章 結論與建議 95
5-1 結論 95
5-2 建議 96
參考文獻 97
附錄 118

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