本研究主要分析二仁溪水體中溶解相與顆粒相多環芳香烴(PAHs)化合物濃度於空間及季節變化的分布情況及可能的影響因子。另外，利用化學指紋鑑定(finger printing)、主成分分析(principal component analysis, PCA)和群集分析(hierarchical cluster analysis, HCA)來推測水體中多環芳香烴的可能來源。

　　研究結果顯示二仁溪近出海口測站水體在全年監測期間，溶解相總多環芳香烴濃度為13.8 to 516 ng/L，顆粒相濃度為4.05-55.9 ng/L。三月份（乾季）二仁溪中下游流域各測站溶解相與顆粒相多環芳香烴濃度分別為38.3-186 ng/L和4.05-25.9 ng/L，九月份（溼季）溶解相與顆粒相多環芳香烴濃度分別為32.3-82.8 ng/L和14.8-85.3 ng/L。支流（三爺宮溪）顆粒相與溶解相多環芳香烴濃度皆大於主流（二仁溪）。受地形與地質特性影響，主流溼季濃度會大於乾季濃度，而支流則乾季濃度大於溼季。

　　相關性分析結果，二仁溪流域顆粒相多環芳香烴濃度，主要受流量、懸浮顆粒濃度與鹽度因子間的交錯且牽動所影響，以位於二仁溪流域之最下游測站Er-1被鹽度影響為最深；其餘僅測站Er-2及測站Er-3離出海口較近亦受鹽度影響。其它測站顆粒相多環芳香烴濃度分布主要受流量及水中懸浮顆粒濃度因子與測站周遭有機污染物排放源所影響。

　　從指紋分析、主成分分析與群集分析結果，可得知本研究區域多環芳香烴化合物的來源為是屬複雜多元，包含著燃燒來源、石油來源、成岩作用/生物性源與混合性（其混合性可能包含燃燒、石油與生物來源等）來源。溶解相以燃燒特性和石油特性的來源為主，而顆粒相以燃燒來源為主，其中溶解相與顆粒相多環芳烴燃燒源偏以液態燃料燃燒來源為主。另外也發現在主流測站顆粒相多環芳香烴具有成岩作用/生物性來源特性，特別在溼季期間較有明顯的來源特性。

　　監測期間，二仁溪多環芳香烴的總計年輸出通量為23.1 kg/year；溶解相之年輸出通量為11.3 kg/year，乾、溼季分別為5.88與65.8g/day；顆粒相之多環芳香烴年輸出通量為11.8 kg/year，乾、溼季分別為0.77與76.2 g/day；以溶解相通量為主要貢獻，溼季總通量大於乾季；總計年輸出通量普遍低於其它地區，僅較接近於San Francisco River, USA及高於Le Havre River, France地區。

In this study our purposes were to investigate the spatial distribution and seasonal variation of polycyclic aromatic hydrocarbons (PAHs) in the dissolved and particulate phase of PAHs in Er-Jen River. In addition, the potential sources of PAHs in Er-Jen River were investigated not only by finger printing, but also principal component analysis (PCA) and hierarchical cluster analysis (HCA).

　　Concentrations of dissolved and particulate PAHs ranged from 13.8 to 516 ng/L and from 4.05 to 55.9 ng/L, respectively. In March (dry season), concentrations of dissolved and particulate PAHs ranged from 38.3 to 186 ng/L and from 4.05 to 25.9 ng/L, respectively. In addition, concentrations of dissolved and particulate PAHs ranged from 32.3 to 82.8 ng/L and from 14.8 to 85.3 ng/L, respectively in September (wet season). The highest total PAH concentration in this area was found in Station Er-3 which is located on a tributary of Er-Jen River. Total PAH concentrations in wet season were higher than those found in dry season for all stations in Er-Jen River, except for station Er-3, which suggesting that different geography might be the reason.

　　Results from correlation analysis indicated that distributions of PAH concentrations for particulate phase in Er-Jen River correlated well with flow rate, suspended solid concentrations and salinity. Total PAH concentration of station Er-2, which was located at the downstream Er-Jen River, was highly correlated with salinity; while total PAH concentrations in other stations were mainly affected by flow rate, suspended solid concentrations and some potential sources of pollution.

Results from PCA, HCA and finger printing all indicated the origins of PAHs were complex sources in the study area, including pyrogenic, petrogenic and diagenetic/biogenic origins. The origins of PAHs in dissolved phase were mainly from both pyrogenic and petrogenic sources; while those in particulate phase were mainly from pyrogenic sources. In addition, the pyrogenic origins in both dissolved and particulate phase were mostly from liquid fuel combustion. In wet season, howerer, diagenetic/biogenic origins were also found in particulate phase at the sampling sites of Er-Jen River.

　　The annual total PAH fluxes of Er-Jen River were estimated to be 23.1 kg For dissolved phase, the average daily fluxes in dry and wet season were 5.9 g/day and 65.8 g/day, respectively, with an annual mean fluxe of 11.3 kg/year. For particulate phase, the mean daily fluxes in dry and wet season were 0.8 g/day and 76.2 g/day, respectively, with an annual mean flux of 11.8 kg/year. In general, the total PAH fluxes in wet season were higher than dry season. The total annual PAH fluxes in Er-Jen River were generally less than those reported worldwide, and comparable to those in San Francisco River in USA, but higher than those in Le Havre River in France.

論文審定書……………………………………………………………………....i
謝 誌…………………………………………………………………..……….ii
摘 要…………..………………………………………..…………….........…iii
Abstract………...…………………………….…………..……………………...v
目 錄…………..……………………………………………………..........…vii
圖 次…………...……………………………...……...……………..….……..x
表 次…………..………………………………...….......…….…………..….xii
附 錄…………...…………………………………..…......………..……..…xiii
本研究圖表化合物所使用的縮寫表……………..……...……….……...…..xiv
第一章 前言………………………………………………..…………...….…….…….1
1-1 研究動機...…………………………………………………….....……….……….1
1-2 研究目的…………..……………………………….…………..……........……….2
第二章 文獻回顧………………..………………….……………………………….....3
2-1 多環芳香烴之特性……………………………………….……..........….….…….3
2-2 多環芳香烴對人體之影響…………………………………….…….….…..…….3
2-3 多環芳香烴之產生及來源………………………………….............…....……….3
2-4 多環芳香烴的指紋鑑定………………….……………….……...…….…...…….4
第三章 研究方法…………………..…………..…………………........….…………...8
3-1 採樣地點、時間與方法……………….……..…….……….…...…...….…..……..8
3-2 材料與儀器設備…………………………..…..……………..……………...…….8
3-2-1 材料…………………………....……..……………...…….....…………...8
3-2-2 儀器設備………………………….….……………......….....……………9
3-2-3 試藥與器材前處理…………………….....………………………………9
3-3 樣品前處理………………………….…………...……………...………..…….10
3-4 樣品多環芳香烴化合物(PAHs)分析…………………..……….......………10
3-5 儀器分析………………………………………………….….……..…….......…12
3-5-1 氣相層析質譜儀(GC-MS)分析……………….….........…...…………...12
3-5-2 多環芳香烴化合物之定量方式…………………..…...……...…………12
3-6 主成分分析(Principal Component Analysis, PCA)…………….......…….……13
3-7 群集分析(Hierarchical Cluster Analysis, HCA).…....……...........................…..13
3-8 品質管制...……………………………………………………………..………..13
3-8-1 回收率…………………..……..…………………..………………………13
3-8-2 空白試驗與偵測極限..………………………..…..…...………….……..14
第四章 結果與討論…………………………………………………....…..…..……17
4-1 多環芳香烴(PAHs)…..…………………………………………………...….….17
4-1-1 二仁溪之溶解相及顆粒相PAHs 濃度分佈以及文獻比較…..…..…..….17
4-1-2 二仁溪之溶解相與顆粒相多環芳香烴濃度於空間及時間變化…..........17
4-1-3 二仁溪之溶解相及顆粒相多環芳香烴濃度與文獻比較…......................26
4-1-4 二仁溪之溶解相及顆粒相多環芳香烴之環數分布……………...……..30
4-2 影響多環芳香烴濃度分佈之因子………………………….……….........….…31
4-2-1 二仁溪河口與三爺宮溪水樣多環芳香烴濃度分布之影響因子…..........31
4-2-2 乾溼季測站多環芳香烴濃度分布之影響因子……………….........…….31
4-3 多環芳香烴在顆粒相及溶解相上分配係數………………………………...…38
4-3-1 全年(2008-07 至2009-07)多環芳香烴在顆粒相及溶解相分配係數…...38
4-3-2 乾溼季(2009-03 與2008-09)多環芳香烴在顆粒相及溶解相分配係數...41
4-4 多環芳香烴之化學指紋鑑定………………………………..…..…...…………45
4-4-1 溶解相多環芳香烴之化學指紋鑑定…………..……….…………......….45
4-4-2 顆粒相多環芳香烴之化學指紋鑑定…………..…….……………......….46
4-5 主成分分析……………………………………………………….…...…….…..53
4-5-1 溶解相之主成分分析……………………………………...………......….53
4-5-2 顆粒相之主成分分析………………………………………..………...….54
4-6 群集分析………………………………………………….………......…………61
4-6-1 溶解相………………………………………….....………...………….….61
4-6-2 顆粒相……………………………..………………...……...……...…..….62
4-7 河川多環芳香烴化合物輸送通量初步估算…………………………...………68
第五章結論與建議…………………….………………...……….…….……..………71
5-1 結論……………………………….…………………………….…....………71
5-2 建議…………………………….……………………………….……....……73
第六章參考文獻………………………..…………………………………….…...…..74
附錄………………………………………….…...……...………………..…………….81

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