||Effects of environmental organic matters on the distribution of bisphenol A in soil-water interface
||Department of Environmental Engineering
Organic carbon content
Accelerated solvent extraction
Environmental sample analysis
雙酚A (bisphenol A) 是一種化學原料廣泛被運用於工業上，常用於製造聚碳酸脂塑膠與環氧樹脂等。其部分結構與雌激素相似，會干擾人體內分泌系統，因此雙酚A被視為一種環境賀爾蒙，雙酚A的化學結構有兩個酚官能基，在土壤中具有中等至低等的流動性，許多研究利用吸附及分配等模式來預測雙酚A在土水介面的流動性。在本研究中，我們藉由採集兩條不同流域(鹽水溪及急水溪)的河川樣品，分析在表面水、孔隙水與底泥中的總有機碳含量以及雙酚A濃度來觀察其是否與理論的推測相符。本實驗選用加速溶劑萃取系統萃取底泥中的雙酚A，以高效能液相層析儀串聯螢光偵測器定量雙酚A，並以螢光矩陣光譜來觀察樣品中水溶性有機物質之種類，以探討有機物質對雙酚A在環境中移動性之影響。
本實驗在萃取底泥樣品具有穩定且高之回收率(62.3%-124 %)，我們觀察到底泥中有機碳含量及雙酚A濃度具有正相關之趨勢，然而在液相中並無類似的正相關趨勢。在鹽水溪中底泥的有機碳平均含量為1.27%，相較於急水溪的0.56%高，然而在土水分配圖中的斜率，鹽水溪為25.0 L/kg，急水溪則為34.6 L/kg，顯示雙酚A在急水溪流域傾向於儲存在固相中。在螢光矩陣分析的結果我們看到鹽水溪的有機質具有較高的芳香蛋白質及溶解性微生物副產物之訊號，其可能是讓雙酚A傾向於儲存在水相中之因素。當我們假設雙酚A並非均勻散布於底泥而是集中於有機相中，與雙酚A在孔隙水中之濃度作圖，可以發現在河川流域以及雨量大小的分類下，雙酚A於土壤有機質與孔隙水之相關係數皆高於0.6，甚至在鹽水溪乾季的分類下，其相關係數高達0.9.
Bisphenol A (BPA) is widely used by the industry to make plastics and epoxy resins. Due to the structural similarity to human estrogen, it can interfere with normal hormonal processes and therefore is recognized as a postulated endocrine-disrupting chemical. BPA is an organic compound having two phenolic functional groups and having a low to moderate degree of mobility in soil. Several approaches including adsorption and partition models have been developed to estimate the distribution of BPA and to predict its mobility in the soil-water interface. In this work, we collected and analyzed environmental samples including surface water, sediment/soil, and soil pore water from two rivers (Yanshuei river and Jishuei river in Tainan, Taiwan) to test the hypothesis that the amount of organic content is, in general, proportional to the concentration of BPA in both liquid and solid phases. An accelerated solvent extractor was used to extract BPA from sediment/soil samples and the quantification of BPA was conducted by HPLC with a fluorescence detector. Excitation-emission matrix (EEM) fluorescence spectroscopy was used to characterize dissolved organic matter (DOM) in water samples.
A stable and high recovery rate (between 62.3% - 124%) from 69 soil/sediment samples was obtained. Positive correlation was found between BPA concentration and organic carbon content in solid phase. The BPA concentration in Yanshuei river samples, of which average organic content in sediment was 1.27%, was generally higher than that in Jishuei river samples of which average organic content in sediment was 0.56%. However, the slope calculated from soil-water distribution was 25.0 L/kg for Yanshuei river and 34.6 L/kg for Jishuei river, suggesting that BPA tended to accumulate in solid phase in the Jishuei river area. EEM analysis results showed there were more microbial by-product-like substances in Yanshuei river samples which may help BPA stay in the liquid phase. As we concentrate the BPA in sediment into organic phase and plot with BPA concentration in pore water, highly positive correlation were observed under the classification of river basin and rainfall.
Chapter1 Introduction 1
Chapter2 Literature Review 2
2-1 Bisphenol A 2
2-1-1 Physical and chemical properties of bisphenol A 2
2-1-2 Physical and chemical properties of bisphenol A internal standard 3
2-1-3 Application of bisphenol A 4
2-1-4 The regulation of bisphenol A 6
2-1-5 Bisphenol A in the environment 7
2-2 Organic matter 8
2-2-1 Dissolved organic matter 8
2-2-2 Soil Organic matter 10
2-2-3 Influence of organic matter on organic compound 12
2-3 Distribution mechanism 13
2-3-1 Sorption mechanism 13
2-3-2 Distribution mechanism of organic compound in soil-water interface 14
2-3-3 Distribution behavior of BPA 17
Chapter3 Material and method 21
3-1 Chemicals and standards 22
3-2 Sampling 22
3-2-1 Sampling site 22
3-2-2 Sample procedure 25
3-2-3 Sample pretreatment 25
3-3 Analysis 29
3-3-1 Water quality 29
3-3-2 Total organic carbon 29
3-3-3 Quantification of BPA 30
3-3-4 Excitation/Emission Matrix Spectrofluorometer (EEM) analysis 31
3-3-5 Statistical analysis 33
Chapter4 Result and discussion 34
4-1 Water quality 34
4-2 TOC in surface water, pore water and sediment 35
4-3 BPA concentration and ASE recovery 37
4-3-1 BPA concentration 37
4-3-2 Recovery of ASE extraction 39
4-4 The relationship between BPA and TOC among surface water, pore water and sediment 41
4-4-1 River basin 41
4-4-2 Rainfall 44
4-4-3 Stream reach 47
4-5 The relationship of BPA concentration in pore water and sediment 49
4-6 The relationship of BPA concentration in pore water and organic carbon 52
4-7 EEM analysis result 57
Chapter5 Conclusion and Suggestion 60
5-1 Conclusions 60
5-2 Suggestions 61
Appendix (A) Relationship between water quality and bisphenol A in different medium 70
Appendix (B) Recovery rate of all sediment samples 73
Appendix (C) Rainfall data from measure station in Tainan 74
Appendix (D) BPA distribution between pore water and organic carbon in upstream and downstream 76
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