臺灣博碩士論文加值系統

近40年來，全球烷基酚聚乙氧基醇(alkylphenol ethoxylates, APnEO)的年生產量均超過50萬公噸，主要應用於工業製程、農業用殺蟲劑與家用清潔產品等，釋放至環境中的污水或空氣，會經由生物降解產生短鏈的APnEO和具有毒性之降解產物烷基酚(alkyphenols, APs)，如壬基酚(nonylphenol, NP)、辛基酚(octylphenol, OP)、雙丁基酚(butylphenol, BP)，人類可能攝取已污染的食物，而遭受暴露。故本研究利用尿液作為國內北、中、東、南部地區成年非職業暴露族群NP、OP、BP之暴露的生物偵測指標，並且以食物攝取量問卷調查計算人體內攝取壬基酚的情形，以了解國人烷基酚類暴露程度和情形。
台灣北、中、東及南部地區回收之有效問卷共289份，上、下班時段收集之有效尿液樣本共510個。其中男性有70位，女性219位。而本研究上班時段之尿液樣本中NP、OP、BP檢出率分別為27.4%、28.2%及31.1%，而平均原始濃度分別為1.47±1.53、4.88±14.92、3.64±14.33ng/mL，平均校正濃度則是2.63±4.18、11.67±41.46與11.86±79.00μg/g cr.。而下班時段的尿液樣本中NP、OP、BP檢出率則分別為28.8%、27.9%及30.8%，而平均原始濃度分別為2.04±6.47、4.50±15.08、7.46±45.00ng/mL，平均校正濃度則是3.77±12.03、8.53±24.75與12.12±56.69μg/g cr.。其中，NP、OP、BP的檢出率、原始濃度與校正濃度均普遍呈現北部較其他地區顯著較高的情形。將同一受測者之上、下班尿液進行比較，結果發現兩個時間點NP、OP、BP暴露量結果並無顯著不同，受測者在短時間內的烷基酚類暴露不會有明顯變化。而本研究計算成年人每日平均NP攝取量為22.48±17.74μg/day。另外，分析成年人每日平均NP攝取量與上、下班尿液中NP原始或校正濃度的相關性，顯示各地區成年人每日平均NP攝取量與尿液中的NP濃度無顯著相關性存在。
與美國及日本相關文獻相比，本研究測得之台灣地區成年人體內含有較高的NP濃度，且我國成年人每日平均NP攝取量為德國成年人的3倍與紐西蘭成年人的5倍。顯示具有較嚴重的暴露程度。而食物之NP攝取量與尿液樣本中的NP濃度沒有顯著相關，推測可能還有其他污染途徑。同時發現，都市化越高的地區，成年人之烷基酚類暴露程度較為嚴重。本研究結果提供了我國一般成年人烷基酚類暴露的情形，未來的研究能再針對一些可能的暴露來源加以探討。

Alkylphenol ethoxylates(APnEO), which are widely used in industrial processes, agricultural pesticides and household cleaning products, is producted over five hundred thousand tons in global production each year in recent 40 years. Due to biodegration, the waste water and air released into environment yields a mixture containing short-chained APnEO and toxic alkyphenols(APs) such as nonylphenol(NP), octylphenol(OP), and butylphenol(BP). The human body could expose to APs via ingesting the contaminated food. The urine samples were analyzed for this study were collected from the non-occupational exposure adults residing in northern, middle, eastern and southern Taiwan, and used as the biological monitoring samples to evaluate the exposure of NP, OP, and BP. Moreover, with a questionnaire survey for the personal food intake, the APs intake can be calculated by each subject with the APs concerntration of each food, and extent of the APs exposure among these populations can be obtained.
A total of 289 valid questionnaires and 510 urine samples collected at work, 270 in the morning and 240 by the end of the shift. In 289 questionnaires 70 are replied by male and 219 female. Our results showed the detection rates were 27.4% for NP, 28.2% for OP, and 31.1 for BP in the urine samples. The average concentrations of these metabolites were, respectively, 1.47±1.53, 4.88±14.92, and 3.64±14.33 ng/mL in samples collected in the morning and with the adjusted were 2.63±4.18, 11.67±41.46, and 11.86±79.00μg/g cr.. The corresponding detection rate of NP, OP, and BP in the urine samples collected on the end of the shift were are respectively 28.8%, 27.9%, and 30.8%, respectively. The average urinary concentrations were 2.04±6.47, 4.50±15.08, 7.46±45.00ng/mL, respectively, and 3.77±12.03, 8.53±24.75, and 12.12±56.69μg/g cr.. The detection rates and average concentrations of NP, OP, and BP were higher in urinary samples collected in the highest urbanized area than that in the other three areas. There were no significant differences in the average. APnEO levels in the urine samples collected from the same people between the on-duty and off-duty. In this work we estimated that the average food daily intakes of NP in adults was 22.48±17.74μg/day. We also found that there were no significant differences among the average daily intakes of NP and the urinery NP concentrations in adult populations residing in northern, middle, eastern and southern Taiwan.
Compared our results with the relative references found in the United States and Japan, a higher concentrations of NP are observed in adult populations in Taiwan. Moreover, with the amounts of average daily intakes of NP of adult populations in Taiwan being three-times more than those in Germany and five times more than those in New Zealand, it shows that our subjects experience more serious exposure of NP. Due to the low relevance between the food intakes of NP and the NP concentrations in urine samples, we conjecture that there probably exists other contaminating paths. We also find that the adult habitants in more urbanized regions tended to have higher contamination levels of APs than those in more remote regions. The results of this work provide the profiles of the exposure of APs of the adult populations. Future work could further discuss about the other possible contaminating paths.

摘要....................................................I
Abstract...............................................II
目錄...................................................IV
表目錄...............................................VIII
圖目錄..................................................X
附錄目錄................................................X
第一章 前言.............................................1
1-1 研究緣起............................................1
1-2 研究目的............................................2
第二章 文獻探討.........................................4
2-1 內分泌系統..........................................4
2-2 內分泌干擾物質......................................4
2-3 烷基酚聚乙氧基醇類..................................5
2-3-2 污水處理..........................................5
2-3-3 生物降解..........................................6
2-4 烷基酚類............................................6
2-4-1 合成與應用........................................6
2-4-2 生物降解..........................................7
2-4-3 物理特性..........................................7
2-5烷基酚類對生物體之影響效應...........................8
2-5-1 植物..............................................8
2-5-2 魚貝類............................................8
2-5-3 老鼠..............................................8
2-5-3-1 代謝............................................8
2-5-3-2 毒性及生理效應..................................9
2-5-4 豬...............................................10
2-5-5 人類.............................................10
2-5-5-1 代謝...........................................10
2-5-5-2 生理效應.......................................11
2-5-5-3 暴露情形.......................................11
2-6 烷基酚類之環境流佈.................................11
2-6-1 污水及污泥.......................................11
2-6-2 河水、海水與底泥.................................12
2-6-3 粉塵.............................................13
2-6-4 空氣.............................................13
2-6-5 食物.............................................14
第三章 材料與方法......................................15
3-1材料................................................15
3-1-1 試藥.............................................15
3-1-2 器材.............................................15
3-1-3 儀器.............................................16
3-2 方法...............................................16
3-2-1 研究對象與樣本收集...............................17
3-2-2 問卷調查.........................................17
3-2-3 尿液樣本的收集...................................17
3-2-4 標準品配製.......................................18
3-2-5 試劑配製.........................................18
3-2-6 尿液creatinine檢測...............................18
3-2-7樣本前處理........................................19
3-2-8 樣本分析條件.....................................19
3-2-9 分析方法之品保與品管.............................20
3-3 結果換算...........................................21
3-3-1 尿液樣本濃度.....................................21
3-3-2 尿液樣本烷基酚類校正濃度.........................21
3-3-3每日壬基酚攝取量之計算方法........................21
3-4 統計分析...........................................21
第四章 結果............................................21
4-1 分析方法之品保/品管................................22
4-2 研究對象之基本資料.................................22
4-3 各地區成年人尿液樣本烷基酚類濃度比較...............23
4-4 各地區男性成年人尿液樣本烷基酚類濃度比較...........25
4-5 各地區女性成年人尿液樣本烷基酚類濃度比較...........28
4-6 各地區成年人上、下班之尿液樣本中烷基酚類濃度比較...30
4-7 各地區成年人之食物攝取量...........................33
4-8 各地區成年人每日平均壬基酚攝取量...................33
4-9 每日平均壬基酚攝取量與尿液中壬基酚濃度之相關性.....33
第五章 討論............................................35
5-1 尿液樣本之烷基酚類濃度比較.........................35
5-2 各地區樣本之烷基酚類濃度比較.......................36
5-3 上、下班尿液樣本之烷基酚類濃度比較.................37
5-4 食物中壬基酚攝取量比較.............................38
5-5 壬基酚的攝取量與生物偵測樣本濃度的相關性...........38
第六章 結論與建議......................................41
參考文獻...............................................42
表.....................................................50
圖.....................................................59
附錄...................................................62

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