持久性有機污染物（persistent organic pollutants, POPs）廣泛存在於自然界中，對環境及人體具有危害。其中多氯聯苯（polychlorinated biphenyls, PCBs）由於高毒性及生物累積性，世界各國家於1970年代已禁用含此類化合物的所有製品。但多氯聯苯不易分解，並藉由水氣交換等傳輸機制分布於全球，因此環境中仍可測得濃度。本研究延續Fang et al.,（2008）及陳（2010）於高雄港區空氣及水體中多氯聯苯之水氣交換討論，再將測站延伸至高屏海域及蘭嶼，探討港內及開放式海域之多氯聯苯水氣交換通量。本研究討論空氣及水體中氣相、溶解相及顆粒相之濃度含量、分布與同族物組成，進而討論水氣交換及乾沉降之污染傳輸機制；並以群集分析、主成分分析與美國多氯聯苯產品Aroclor作統計分析推估多氯聯苯的可能污染來源。
空氣總多氯聯苯的濃度範圍介於116∼439 pg m-3，平均濃度為164 pg m-3；氣相及顆粒相平均濃度分別為161 pg m-3及2.91 pg m-3。水體總多氯聯苯的濃度範圍介於14.1∼1750 pg L-1，平均濃度為233 pg L-1；溶解相及顆粒相平均濃度分別為162 pg L-1及70.4 pg L-1。空氣總多氯聯苯濃度以11月高屏溪口（GRE）最高，推測受到風向與鄰近林園工業區的影響。水體總多氯聯苯以8月高雄港區（KHH）最高，可能與莫拉克颱風過後降雨及地面逕流將污染物帶入港區內有關。
以百分比組成、群集分析及主成分分析探討污染物來源，在空氣氣相及水體溶解相部份皆以低氯數的二至四氯為主要貢獻；空氣顆粒相及水體顆粒相則以中高氯數的四至六氯為主要貢獻。
毒性當量用來判斷污染物危害環境及人體的程度，本研究在空氣氣相平均毒性當量為0.0008 pg-TEQ m-3，水體溶解相平均毒性當量為0.0006 pg-TEQ L-1，皆以PCB114為最主要貢獻的同源物。
污染傳輸機制包括水氣交換及乾沉降，平均水氣交換通量為＋31.5 ngm-2day-1，平均乾沉降通量－0.54 ng m-2 day-1，水氣交換通量明顯高於乾沉降通量。高雄港區年度多氯聯苯淨通量＋40.2 mg m-2 yr-1，估計每年由水體往空氣輸出約0.5公斤的多氯聯苯。

Persistent organic pollutants (POPs) were widely distributed in the environment, and may cause hazardous effects to human health. Among these pollutants, polychlorinated biphenyls (PCBs), due to their toxicity and bioaccumulation, have been banned in the mid 1970s in most countries. They are ubiquitous and highly persistent, and therefore, PCBs are of most concern for their potential to be globally transported through air-water exchange. Previous studies such as Fang et al.（2008） and Chen（2010）have studied the air-water exchange of PCBs in Kaohsuing Harbor. This study not only continued monitoring this area but also included Gao-Ping coastal areas and Lanyu Island in order to determine the air-water exchange fluxes of PCBs in harbor and coastal area. The aim of this study was to determine the magnitude of PCB air-water exchange fluxes and dry deposition fluxes by measuring the gas/particle phase concentrations in ambient air and dissolved/particle phase concentrations in water column, and to analyze the compositional patterns of PCB homologs. Hierarchical cluster analysis (HCA) and principal components analysis (PCA) were performed with compositional patterns of commercial products such as Aroclor mixtures to gain a better understanding of pollution topography for PCBs .
The concentrations of ΣPCBs in the ambient air ranged from 116 to 439 pg m-3, with an average concentration of 164 pg m-3 . The average PCB concentrations in gas and particle phase were 161 pg m-3 and 2.91 pg m-3, respectively. The concentrations of ΣPCBs in water column ranged from 14.1 to 1750 pg L-1, with an average concentration of 233 pg L-1. The average PCB concentrations in dissolved and particle phase were 162 pg L-1 and 70.4 pg L-1, respectively. The highest gaseous concentration of ΣPCBs was observed in GRE in November, suggesting that wind direction and Linyuan Industrial Park may be the major contributor of PCBs there. However, the highest dissolved concentration of ΣPCBs was found in KHH in August, indicating that rainfall and runoff of Typhoon Morakot were evident in source.
Results from HCA, PCA and compositional patterns indicate that lower chlorinated congeners (dichlorobiphenyls to tetrachlorobiphenyls) were predominant in the gas and dissolved phase of ambient air and water column. In particle phase of ambient air and water column, PCB compositions were dominated by higher chlorinated congeners (tetrachlorobiphenyls to hexachlorobiphenyls).
TEQ was used to determine the level of pollution for environment and human health. The average TEQ was 0.0008 pg-TEQ m-3 in gas-phase of ambient air and was 0.0006 pg-TEQ L-1 in dissolved phase in water. PCB114 was observed to be the predominant congener in this study.
The average flux of air-water exchange was ＋31.5 ng m-2 day-1, and was much higher than the average flux of dry deposition (－0.54 ng m-2 day-1). The net PCB fluxes in KHH suggest that annual air-water exchange was ＋40.2 mg m-2 yr-1 and estimated yearly, 0.5 kg of PCBs were emitted from water column of Kaohsiung harbor to the ambient atmosphere.

論文審定書 i
謝誌 ii
摘要 iv
Abstract vi
目錄 viii
圖目錄 xi
表目錄xiv
附錄目錄 xvi
第一章 前言 1
1-1 研究動機 1
1-2 研究目的 3
第二章 文獻回顧 4
2-1 持久性有機污染物（POPs） 4
2-2 多氯聯苯 12
2-3 多氯聯苯的特性 17
2-3-1 物理特性 17
2-3-2 化學特性 17
2-3-3 生物特性 18
2-4 多氯聯苯的毒性 21
2-5 多氯聯苯的案例 22
2-6 多氯聯苯的來源.23
2-7 多氯聯苯的傳播途徑 28
2-8 研究區域 29
2-8-1 高屏海域 29
2-8-2 蘭嶼 38
第三章 研究方法 39
3-1 材料與儀器 39
3-1-1 材料 39
3-1-2 儀器設備 40
3-2 試藥及器具前處理 40
3-3 採樣地點、時間與保存 40
3-4 樣品前處理 49
3-5 多氯聯苯分析 49
3-5-1 樣品淨化 49
3-5-2 GC-ECD 設定操作條件51
3-5-3 定量方法－內標準法51
3-6 品管與品保（QA-QC） 52
3-6-1 方法回收率 52
3-6-2 空白實驗分析 57
3-6-3 方法偵測極限 57
3-7 群集分析（Hierarchical Cluster Analysis, HCA） 57
3-8 主成分分析（Principal Components Analysis, PCA） 58
3-9 毒性當量（Toxic Equivalent Quantities, TEQ） 59
3-10 水氣交換 62
3-11 亨利定律 67
3-12 水氣交換計算之傳輸誤差 69
第四章 結果與討論 70
4-1 多氯聯苯濃度分布 70
4-1-1 多氯聯苯在空氣氣相濃度分布 71
4-1-2 多氯聯苯在水體溶解相濃度分布 77
4-2 多氯聯苯化合物同族物濃度分析 84
4-2-1 多氯聯苯於空氣氣相之同族物濃度分析 85
4-2-2 多氯聯苯於水體溶解相之同族物含量分析 94
4-3 階層群集分析（Hierarchical Cluster Analysis, HCA） 106
4-3-1 空氣氣態之群集分析 106
4-3-2 水樣溶解態之群集分析 109
4-3-3 以Aroclor商業產物判別多氯聯苯之污染來源 112
4-4 主成分分析（Principal Components Analysis, PCA） 117
4-4-1 空氣氣相 117
4-4-2 水樣溶解相 123
4-5 多氯聯苯之逆軌跡（back trajectory analysis 129
4-6 多氯聯苯之總毒性當量（Toxic Equivalent Quantities, TEQ） 131
4-7 多氯聯苯之文獻比較 135
4-7-1 空氣氣相與國內文獻之比較 135
4-7-2 空氣氣相與國外文獻之比較 137
4-7-3 水樣溶解相與國內文獻之比較 140
4-7-4 水樣溶解相與國外文獻之比較 140
4-8 多氯聯苯之水氣交換 145
4-8-1 水氣交換通量 145
4-8-2 水氣交換之全年通量 157
4-8-3 水氣交換與國內外文獻比較 162
4-9 大氣與海水中顆粒相多氯聯苯濃度分布及乾沉降...167
4-9-1 空氣顆粒相濃度....167
4-9-2 水體顆粒相濃度 171
4-9-3 乾沉降 176
第五章 結論與建議 182
5-1 結論 182
5-2 建議 185
參考文獻 186
附錄196

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