臺灣博碩士論文加值系統

本研究為了解萬丹堤防河道測人工溼地對雌激素活性及內分泌干擾物質之去除效率。特別利用LC-MS/MS進行壬基苯酚(NP)、辛基苯酚(OP)及雙酚A(BPA)等酚類化合物及天然、合成雌激素化合物如雌酮(E1)、雌二醇(E2)、雌三醇(E3)、乙烯雌酚(DES)及乙炔雌二醇(EE2)分析探討，並結合T47D-KBluc生物試驗進行雌激素活性評估。
生物試驗結果顯示，於人工濕地各處理系統中皆可檢測出含有雌激素活性，結果顯示，進流口、沉砂池、預曝池、接觸曝氣池、水生植物區及放流口雌激素活性分別介於1.18~30.4、0.85~27.74、0.46~3.32、0.53~6.48、0.48~13.44及0.52~21.16ng/L；針對不同流量的研究，100CMD、200CMD、350CMD及500CMD之雌激素活性結果顯示，平均去除率分別為64%、42%、36%及31%。
化學分析結果顯示，雌酮、雌二醇、乙炔雌二醇及乙烯雌酚檢出率為0%，雌三醇、壬基苯酚、辛基苯酚及雙酚A檢出率分別為16%、3%、21%及1%。對於雌三醇及辛基苯酚之平均去除率分別為&;gt;99%及37%；壬基苯酚則無法去除；而雙酚A則只偵測到一個位於水生植物區的樣品，因此無去除率。
比較化學分析及生物分析結果發現，化學分析之計算雌激素活性範圍介於ND~0.46ng/L；而生物分析之實測雌激素活性範圍介於0.48~30.3ng/L，可發現生物試驗可檢出環境水體中具雌激素活性之已知及未知化合物，為一快速檢測可能產生生物體效應的方法。

The first objective of this study was to investigate the removal efficiency of the endocrine disrupting chemicals(EDCs), including phenolic compounds such as nonylphenol(NP), octylphenol(OP) and bisphenol A(BPA), and natural and synthetic chemicals such as estrone(E1), 17β-estradiol(E2), estriol(E3), diethylstilbestrol(DES) and 17α-ethinylestradiol(EE2) of wastewater treated by the constructed wetland from the Wan-Dan embankment. The second objective was to assess the estrogenic activity with different treatment units using the T47D-KBluc bioassay.
According to the T47D-KBluc assay, the estrogenicities in influent(In), grit chamber(GC), pre-aeration tank (AT), the contact aeration tank(CAT), aquatic plants area (PA) and effluent(Eff) were ranged from 1.18 to 30.4, 0.85 to 27.74, 0.46 to 3.32, 0.53 to 6.48, 0.48 to 13.44 and 0.52 to 21.16ng 17β-estradiol(E2) equivalents/L. The results of the different flows from the constructed wetland, 100CMD, 200CMD, 350CMD and 500CMD showed the mean removal efficiency of estrogenic activity, 64%, 42%, 36% and 31%, respectively.
In chemical analysis, the samples were pre-concentrated by solid phase extraction, and analyzed for target compounds by LC-MS/MS method. According to the results, estrone, estradiol, ethynyl estradiol and diethylstilbestrol were not detected throughout the study period. The detection frequency of estriol, nonylphenol, octylphenol and bisphenol A were approximately 16%, 3%, 21% and 1%, respectively. The removal efficiency of estriol and octylphenol, showed was larger than 99% and 37%,respectively. Nonylphenol can’t be removed in the system. Bisphenol A detected only in one sample located in the aquatic plants area.
Comparison of to the chemical analysis and bioassay, the concentration of estrogenic activity ranged from ND to 0.46ng / L and 0.48 to 30.3ng / L, respectively. Bioassay could be used to detect known and unknown estrogenic compounds, as a rapid and effective detection method.

摘要+I
ABSTRACT+II
目錄+IV
表目錄+VII
圖目錄+VIII
第1章 前言+1
1.1研究緣起+1
1.2研究目的+3
第2章 文獻回顧+5
2.1濕地背景介紹+5
2.1.1濕地的定義 +5
2.1.2濕地的分類 +6
2.1.3人工濕地之分類+7
2.1.4人工濕地之應用+8
2.2研究區域背景資料+11
2.2.1東港溪流域概況+11
2.2.2 氣候水文+11
2.2.3 人口分佈+12
2.2.4產業結構+13
2.2.5萬丹堤防人工濕地+15
2.3環境荷爾蒙+16
2.3.1荷爾蒙概述+16
2.3.2環境荷爾蒙概述+16
2.3.3環境荷爾蒙種類+17
2.3.4本研究中內分泌干擾物質之概述+19
2.4雌激素類化合物於環境水體之分佈+23
2.4.1污水處理廠+23
2.4.2河川+ 27
2.4.3 人工濕地+31
2.5內分泌干擾物質之去除機制+35
2.5.1結合態雌激素水解及生物轉化為游離態雌激素+35
2.5.2 生物轉化途徑+35
2.5.3 降解作用(Degradation)+38
2.5.4 吸附作用(Sorption)+38
2.5.5 光解作用(Photolysis)+40
2.5.6 揮發作用(Volatilization)+41
2.6 內分泌干擾物質之生物試驗法 +42
2.6.1 活體外試驗(in vitro)+42
2.6.2 各國水體中之雌激素當量濃度(EEQ)+44
第3章 實驗設備與方法+47
3.1實驗材料+47
3.1.1 實驗藥品+47
3.1.2 實驗器材+48
3.1.3 實驗設備+49
3.1.4 現場偵測儀器+49
3.1.5 細胞株來源+50
3.2 樣品收集與來源+51
3.2.1萬丹堤防人工濕地系統採樣點描述+51
3.2.2 樣品採集+51
3.3 化學分析+53
3.3.1 前處理+53
3.3.2 高效液相層析質譜儀參數設定+53
3.4 生物分析+56
3.4.1 原水培養液製備+56
3.4.2細胞培養+56
3.4.3 實驗流程+57
3.4.4 E2標準曲線+57
3.5 樣品化學分析之品保品管+58
3.5.1 檢量線+58
3.5.2 偵測極限+58
3.5.3 回收率+58
3.6 雌激素當量濃度之計算與統計分析+61
3.6.1 雌激素當量濃度(EEQcal)+61
3.6.2 樣品生物試驗雌激素當量計算(EEQbio)+61
第4章 結果與討論+63
4.1 基本水體資料+63
4.1.1 溫度+63
4.1.2 pH值+64
4.1.3 溶氧+64
4.1.4 導電度+65
4.2 生物分析結果+67
4.2.1 雌二醇(E2)標準曲線+67
4.2.2 人工濕地之雌激素活性分佈+67
4.2.3 雌激素活性於不同月份之進流變化+69
4.2.4 人工濕地於不同流量之雌激素活性衰減率+69
4.3 化學分析+73
4.3.1 雌激素類化合物於人工濕地之濃度分佈+73
4.3.2 酚類化合物於人工濕地之濃度分佈+74
4.3.3 小結+76
4.4 化學分析與生物分析之雌激素活性比較+79
第5章 結論與建議+83
5.1 結論+83
5.2 建議+84
第6章 參考文獻+85
附錄+105

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