亞硝胺（Nitrosamine）為一種具高致癌性含氮新興污染物，常微量存在於廢污水或飲用水中。本研究選擇高屏溪上游至下游五個採樣點（包含下游飲用水廠取水口）進行四次採樣（2016/8、2017/1、2017/4、2017/8），並分析雙氯芬酸（Diclofenac）與二甲雙胍（Metformin）兩種藥品、八種亞硝胺生成潛勢以及常見水質，藉由相關性分析探究常見水質與八種亞硝胺生成潛勢關聯性，調查Metformin於表面原水中之亞硝胺生成潛勢貢獻情形，並以健康影響潛勢作為解析亞硝胺生成潛勢與藥品所對應亞硝胺生成潛勢之健康影響潛勢潛勢之工具。結果顯示，在亞硝胺生成潛勢分布方面，第一次採樣（ND至6000 ng/L）測得之濃度遠高於其他三次採樣，顯示亞硝胺生成潛勢分布以可能受到季節（如豐、枯水季）或天氣狀況影響。亞硝胺生成潛勢自上游site1至取水口區間逐漸上升，其中又以第一次採樣最為顯著，第一次採樣NDMA-FP、NPY-FP與NMOR-FP平均濃度分別由495上升至3142 ng/L、由62上升至1113 ng/L以及由470上升至854 ng/L後，經過Site 2至Site 4區間普遍有呈現下降趨勢，顯示亞硝胺生成潛勢污染集中上游河段。高屏溪整段流域以及取水口位置皆觀察到Diclofenac與Metformin濃度，其中Metformin受到國內高使用量影響濃度普遍高於Diclofenac。四次採樣結果顯示Metformin與Diclofenac高濃度主要發生在中下游河段（如site2或site3），可能原因與中下游河段之人為排放如民生污水有關。此外，第二次與第三次採樣結果中，Metformin（59.74 -428.84 ng/L、22.97-119.39 ng/L）與Diclofenac（1.16-34.89 ng/L、ND-32.3 ng/L）濃度普遍高於其餘兩次採樣結果，顯示藥品濃度變化亦可能受到季節（豐、枯水季）影響。除了溶氧（Dissolved oxygen，DO）與濁度，水中化學需氧量（Chemical oxygen demand，COD）濃度亦可對亞硝胺生成潛勢產生影響，如高分子量（>100 g/mole）、鍊狀（NDBA-FP）、以及環烷類（NPYR-FP、NPIP-FP、NMOR-FP）亞硝胺生成潛勢。Metformin與Diclofenac其NDMA生成潛勢莫爾轉換率分別為0.05 %以及0.01 %，經由八種亞硝胺生成潛勢與兩種藥品濃度間相關性分析結果指出，亞硝胺生成潛勢並非由單一藥品前驅物如Metformin或Diclofenac即可決定。國內大量使用之Metformin對亞硝胺生成潛勢貢獻率在高屏溪中下游河段，在第二以及第三次採樣（~0.08-1%）最為顯著，除了中下游多為民生污染為主外，季節變化（豐、枯水季）亦為影響因素之一。亞硝胺生成潛勢估算增量健康影響潛勢結果顯示，高屏溪流域中主要風險來自NDMA生成潛勢，八種亞硝胺生成潛勢增量健康影響潛勢普遍有往中下游段逐漸上升趨勢。將Metformin轉換為其對應之NDMA-FP健康影響潛勢潛勢，三次採樣結果顯示其貢獻率介於0.03至1 %且普遍從上游至site3位置間有上升趨勢，其中以第二次採樣最為顯著（0.3至0.92 %）。本研究透過原水流域亞硝胺生成潛勢污染之調查，評估原水水質中亞硝胺生成潛勢與國內大量使用藥品之關聯性，希冀藉此提供此兩類新興污染物管理策略之相關資訊。

Given the carcinogenicity of nitrosamines as emerging nitrogenous contaminants, this study investigated the correlations among typical water quality parameters, pharmaceuticals including metformin and diclofenac, and nitrosamines formation potentials (FPs) in a major surface drinking water source in southern Taiwan. The contributions of two pharmaceuticals to nitrosamine-FPs in the source water were analyzed, followed by estimating the overall health effect potentials caused by the nitrosamine-FPs. The sampling sites of concern contained five locations from upstream to downstream in Gaoping River, including one near the intake for drinking water of Kaohsiung City in southern Taiwan. In the results from four sampling seasons, the highest nitrosamine-FPs occurred in the 1st sampling events (e.g., ND to 6000 ng/L), indicating the effect of seasonal variation (i.e., dry or wet season). In the 1st season, the nitrosamine-FPs generally increased from the upstream (site1) to intake, as the NDMA-FP, NPY-FP and NMOR-FP concentrations was greatly elevated near the intake (e.g., the average concentrations were 3142, 1113 and 854 ng/L, respectively). Nitrosamine-FPs generally decreased from the intake to downstream sites, possibly attributable to the nitrosamine-FP pollution being sourced from the anthropogenic activities near the mid- and downstream areas. The metformin and diclofenac concentrations were both detected through the sites in Gaoping River. The concentrations of metformin were higher those of diclofenac, with metformin being the mostly used pharmaceutical in Taiwan. The elevated pharmaceutical concentrations typically occurred near the mid- and downstream areas in Gaoping River. The anthropogenic activities such as domestic sewage was one possible explanation. In addition, high concentrations of metformin and diclofenac were observed in the 2nd samplings events (59.74-428.84 and 1.16-34.89 ng/L, respectively) and 3rd (22.97-119.39 and ND-32.3 ng/L, respectively) due to the impacts of seasonal and meteorological variations. By correlation analysis, besides dissolved oxygen (DO) and turbidity, nitrosamine-FPs, notably those with high molecular weights (i.e., >100 g/mole), chain chemical structures (e.g., NDBA-FP), and cycloalkanes nitrosamine-FPs (e.g., NPYR-FP, NPIP-FP, or NMOR-FP), were more likely to be affected by chemical oxygen demand (COD) in the source water. The NDMA-FP molar conversions of metformin and diclofenac were 0.05% and 0.01%, respectively. By correlation analysis between eight nitrosamines-FPs and two pharmaceutical concentrations, the nitrosamine-FPs was not predictable by one individual pharmaceutical concentration. The contribution of metformin toward the NDMA-FP in the Gaoping River ranged from 0.08% to 1% during four sampling seasons. In the result of health risk assessment, the excess cancer risks caused by eight nitrosamines-FPs were typically elevated near the mid- and downstream areas. The contribution of metformin toward the excess cancer risk posed by the NDMA-FP generally increased from the upstream to midstream areas (e.g., from 0.03% to 1%), suggesting the importance of metformin in these areas. This study investigates insights into the nitrosamine-FPs and two widely used pharmaceuticals in one critical surface drinking water source, with respect to the correlation analysis among these concentrations and health risk assessment, providing valuable information for future development of management strategies of these emerging contaminants.

摘要 ....................................................................................................................... ii
Abstract ..................................................................................................................... iv
目錄 ...................................................................................................................... vi
圖目錄 .................................................................................................................... viii
表目錄 ....................................................................................................................... x
第一章 前言 ....................................................................................................... 1
1.1 研究緣起 ....................................................................................................... 1
1.2 研究目的 ....................................................................................................... 4
第二章 文獻回顧 ............................................................................................... 5
2.1 新興含氮消毒副產物 ................................................................................... 5
2.2 亞硝胺類化合物 ........................................................................................... 6
2.2.1 物化特性 .............................................................................................................. 7
2.2.2 危害與規範 ........................................................................................................ 10
2.3 亞硝胺類化合物之生成 ............................................................................. 13
2.3.1 氯胺化生成亞硝胺 ............................................................................................ 13
2.3.2 亞硝化生成亞硝胺 ............................................................................................ 16
2.3.3 臭氧化生成亞硝胺 ............................................................................................ 17
2.3.4 活性碳催化生成亞硝胺 .................................................................................... 19
2.4 亞硝胺前驅物 ............................................................................................. 20
2.4.1 胺基化合物 ........................................................................................................ 22
2.4.2 天然有機物 ........................................................................................................ 24
2.4.3 藥品與個人保健用品 ........................................................................................ 25
2.5 亞硝胺類化合物之流佈 ............................................................................. 29
2.6 藥品與個人保健用品簡介 ......................................................................... 36
2.7 藥品與個人保健用品處理技術 ................................................................. 39
2.8 藥品與個人保健用品生成亞硝胺化合物途徑 ......................................... 43
2.9 環境中藥品與個人保健用品來源與流佈 ................................................. 45
第三章 採樣與方法 ......................................................................................... 53
3.1 研究架構 ..................................................................................................... 53
3.2 藥品與設備 ................................................................................................. 55
3.2.1 本研究之相關藥品與化學品 ............................................................................ 55
3.2.2 本研究使用之儀器設備 .................................................................................... 59
3.3 採樣場址選定 ............................................................................................. 60
3.4 水質、亞硝胺、藥品分析 ......................................................................... 61
3.4.1 水質分析 ............................................................................................................ 61
3.4.2 消毒劑製備 ........................................................................................................ 62
3.4.3 亞硝胺類化合物生成潛勢前處理 .................................................................... 63
3.4.4 藥品前處理 ........................................................................................................ 63
vii
3.4.5 亞硝胺類化合物與藥品分析 ................................................................................ 66
3.5 品質管理 ..................................................................................................... 68
3.5.1 檢量線製備與查核 ................................................................................................ 68
3.5.2 偵測極限 ................................................................................................................ 69
3.5.3 回收率校正 ............................................................................................................ 69
3.6 Metformin 對NDMA 之貢獻率 ................................................................. 70
3.7 相關性分析 ................................................................................................. 70
3.8 亞硝胺生成潛勢健康影響潛勢評估 ......................................................... 71
3.8.1 亞硝胺生成潛勢之暴露劑量評估 .................................................................... 72
3.8.2 亞硝胺生成潛勢之健康影響潛勢評估 ............................................................ 73
3.8.3 健康影響潛勢之不確定分析 ............................................................................ 73
第四章 結果與討論 ......................................................................................... 75
4.1 一般常見水質參數 ..................................................................................... 75
4.2 亞硝胺生成潛勢 ......................................................................................... 78
4.3 藥品濃度 ..................................................................................................... 81
4.4 亞硝胺生成潛勢與常見水質參數之相關性 ............................................. 83
4.5 濁度對水中亞硝胺生成潛勢之影響 ......................................................... 86
4.6 水中藥品濃度與亞硝胺生成潛勢之相關性 ............................................. 88
4.7 兩種藥品對水中亞硝胺生成潛勢之貢獻率 ............................................. 90
4.8 健康影響潛勢 ............................................................................................. 92
4.8.1 亞硝胺生成潛勢之健康影響潛勢 .................................................................... 92
4.8.2 藥品濃度之NDMA 生成潛勢的健康影響潛勢 .............................................. 97
第五章 結論與建議 ....................................................................................... 101
5.1 結論 ........................................................................................................... 101
5.2 建議與未來研究方向 ............................................................................... 105
第六章 文獻 ................................................................................................... 106
中英文對照表 ....................................................................................................... 123

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