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研究生: 黃正君
Huang, Cheng-Chun
論文名稱: 臺灣污水處理廠中多環芳香烴受體與孕激素受體干擾活性之綜合評估
Integrated assessment of aryl hydrocarbon receptor and progesterone receptor disrupting activities in wastewater treatment plants in Taiwan
指導教授: 周佩欣
Chou, Pei-Hsin
學位類別: 碩士
Master
系所名稱: 工學院 - 環境工程學系
Department of Environmental Engineering
論文出版年: 2016
畢業學年度: 104
語文別: 英文
論文頁數: 98
中文關鍵詞: 多環芳香烴受體孕激素受體污水處理廠重組酵母菌報導基因試驗法液相層析串聯式質譜儀
外文關鍵詞: Aryl hydrocarbon receptor, Progesterone receptor, Wastewater treatment plant, Recombinant yeast reporter gene assays, Liquid chromatography tandem mass spectrometry
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  •   近年來,內分泌干擾物質的議題在各國間備受關注,不論是工業、農業或民生用品,處處皆可見到內分泌干擾物質的蹤跡。為了解內分泌干擾物質於污水處理廠中之降解情形,本研究利用重組酵母菌報導基因試驗法檢測臺灣六座民生污水處理廠與一座畜牧污水處理廠之各操作處理單元水樣,評估其是否具有多環芳香烴受體與孕激素受體干擾活性,並搭配液相層析串聯式質譜儀,選定十二種目標物質進行分析,以探討廢水中已知與未知內分泌干擾物質之活性貢獻。
      重組酵母菌報導基因試驗法結果顯示,不論在水相或是懸浮固體相樣本中,皆可測得多環芳香烴受體促進與孕激素受體拮抗活性,而孕激素受體促進活性在所有樣本中皆無測得。懸浮固體相樣本之活性檢出頻率相較於水相樣本高,而畜牧污水處理廠進出流樣本之內分泌干擾活性通常較民生污水處理廠高。經過污水廠之處理程序,內分泌干擾活性有下降趨勢,然而,一級民生污水處理廠之移除效率較二級民生污水處理廠和畜牧污水處理廠來得差。
      液相層析串聯式質譜儀分析結果顯示,民生及畜牧污水處理廠之樣本可測得雙酚A、靛玉紅、對羥基苯甲酸甲酯、對羥基苯甲酸丙酯、壬基酚、孕酮、三氯卡班與三氯沙。目標物質於各污水處理廠之水相樣本所佔比例並不固定,然而,懸浮固體相樣本中三氯沙所佔比例常為最高。將生物試驗與儀器分析結果進行比較,生物試驗結果往往高於儀器分析結果,顯示可能尚有具多環芳香烴受體與孕激素受體干擾活性之物質未被列入目標物質。
      污水處理廠之出流水仍不時可檢測出內分泌干擾物質,顯示污水處理廠之出流水可能為臺灣環境水體中內分泌干擾物質污染來源之一。未來,對於承受水體所造成之影響需更加關注。

    The issues of endocrine disrupting chemicals (EDCs) have raised concerns in recent years since various kinds of EDCs may cause adverse effects on organisms. To understand the removal of EDCs in the wastewater treatment processes, wastewater samples from 6 domestic wastewater treatment plants (WWTPs) and 1 swine WWTP in Taiwan were analyzed in this study. Recombinant yeast reporter gene assays were used to detect whether WWTPs samples showed aryl hydrocarbon receptor (AhR) and progesterone receptor (PR) disrupting activities. In addition, 12 target EDCs were selected and analyzed by liquid chromatography tandem mass spectrometry, and the contributions of known and unknown EDCs to the bioassay-derived endocrine disrupting activities were evaluated.
    Results of recombinant yeast reporter gene assays showed that AhR agonist and PR antagonist activities could be detected in water (W) and suspended solids (SS) of WWTP samples, whereas no samples showed PR agonist activities. AhR agonist and PR antagonist activities were more often found in SS samples than in W samples, and receptor disrupting activities in influents and effluents of swine WWTP were usually higher than those in domestic WWTPs. β-Naphthoflavone and nonylphenol equivalent concentrations showed a downward tendency after treatment of WWTPs. Also, removal efficiencies of primary WWTPs were lower than those of secondary WWTPs and swine WWTP.
    Results of liquid chromatography tandem mass spectrometry showed that bisphenol A, indirubin, methyl paraben, nonylphenol, progesterone, propyl paraben, triclocarban and triclosan could be found in samples from Taiwanese WWTPs. Amount of target compounds detected in W samples varied; however, triclosan concentrations were usually the highest in SS samples. The estimated AhR agonist and PR antagonist activities calculated from liquid chromatography tandem mass spectrometry results were usually lower than the bioassay-derived AhR agonist and PR antagonist activities, which may be due to unknown EDCs showing AhR agonist and PR antagonist activities.
    In conclusion, various kinds of EDCs were detected in the treated effluents of domestic and swine WWTPs in Taiwan. Therefore, effluents of WWTPs may be one of the main sources of EDCs in Taiwanese aquatic environment, thus more attention should be paid to the impacts on receiving waters.

    Table of Contents 摘要 I Abstract III 誌謝 V Chapter 1 Introduction 1 Chapter 2 Literature Review 2 2.1 Endocrine disrupting chemicals (EDCs) 2 2.2 Aryl hydrocarbon receptor (AhR) 2 2.3 Progesterone receptor (PR) 6 2.4 Wastewater treatment plants (WWTPs) 7 2.5 Bioassay analysis 9 2.6 Chemical analysis 10 Chapter 3 Materials and Methods 13 3.1 Experimental procedure 13 3.2 Chemicals and equipment 14 3.2.1 Chemicals 14 3.2.2 Equipment 15 3.3 Sample collection and preparation 16 3.3.1 Sampling sites 16 3.3.2 Sample collection 18 3.3.3 Sample pretreatment 18 3.4 Recombinant yeast bioassays 19 3.4.1 AhR agonist activity assay 20 3.4.2 PR agonist/antagonist activity assay 21 3.4.3 Activity calculation 22 3.5 Liquid chromatography tandem mass spectrometry analysis 24 3.5.1 Instrumental conditions 24 3.5.2 Recovery rates and method detection limits 27 Chapter 4 Results and Discussion 29 4.1 Bioassay analysis 29 4.1.1 AhR agonist activities 29 4.1.2 PR agonist activities 40 4.1.3 PR antagonist activities 40 4.1.4 Removal efficiencies 51 4.1.5 Comprehensive discussions 54 4.2 Chemical analysis 56 4.2.1 Primary WWTPs (BL and CD) 56 4.2.2 Secondary WWTPs (DH, NH, FT and AP) 58 4.2.3 Swine WWTP (L) 61 4.3 Comparison of bioassay and chemical analysis results 66 Chapter 5 Conclusions 70 5.1 Conclusions 70 5.2 Suggestions 71 Reference 72 Appendix 81

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