本研究主要為測量多環芳香烴化合物(polycyclic aromatic hydrocarbons, PAHs)在恆春半島大氣和近岸海水中之濃度與分佈，及計算PAH的海-氣交換通量。研究結果顯示恆春半島大氣（包括氣相和固相）和海水（包括溶解相和顆粒相）中總PAH濃度分別為0.85～4.4 ng m-3和2.1 ~34.3 ng L-1。大氣和海水中總PAH濃度相較於台灣和其他國家測站是屬於背景濃度和低污染量。恆春半島大氣總PAH濃度有季節性的差異，東北季風(NE)季的總PAH濃度高於西南季風(SW)季，且固相的濃度在NE季也較高；海水總PAHs濃度在各測站表層水和深層水沒有顯著差異。季風型的氣候為影響恆春半島大氣總PAH濃度季節性變化的主要原因，而陸源沖刷則會影響後灣區海水中總PAH濃度變化。
由PAHs組成、主成分分析（PCA）和氣團逆軌跡分析結果顯示恆春半島大氣PAHs之主要來源為汽機車排放，PAHs的濃度和組成之季節性變化受到亞洲季風系統影響。過於平緩的氣-固分配係數(log Kp)與過冷飽和蒸汽壓(log PoL)之線性迴歸截距，顯示大氣顆粒中存在有不參與氣-固交換之PAHs，可能有似煤灰顆粒存在。水體之PAHs組成、特徵化指數和PCA結果顯示，水體之PAH主要來為石油來源，其春季和夏季顯示顯著空間上組成的差異，可能是受到陸源輸入和沿岸流的混和影響。水體有機碳液-固分配係數(log Koc)與log Kow之線性迴歸，顯示水體中之PAH與顆粒之間有很強的吸附性，可能有似煤灰顆粒存在。
利用Whitman’s thin-film模式計算恆春半島大氣和水體中4個主要PAH化合物的水氣交換通量，研究結果顯示高揮發性的phenanthrene和pyrene在恆春半島主要是由水體揮發(volatile)到大氣中，而低揮發性fluoranthene和不易揮發的chrysene則為由大氣沉降(absorptive)到水體。由年水氣交換通量結果，可以發現恆春半島近岸水體為大氣低分子量PAH的源；為高分子量PAH的匯。

The distribution, partitioning and air-water exchange fluxes of polycyclic aromatic hydrocarbons (PAHs) were determined in the Hengchun Peninsula of southern Taiwan. The concentrations of total PAH in atmosphere (t-PAH; gas + particulate) and seawater (dissolved + particulate) ranged from 0.43～4.40 ng m-3 and 2.1 ~34.3 ng L-1, respectively. The highest levels of t-PAH concentrations in atmosphere were found during the NE season. Long-range transport and rainfall scavenging mechanisms could contribute to seasonal variations atmospheric t-PAH concentrations. There was significant spatial difference in PAH concentrations in seawater among the sampling stations. The higher t-PAH concentrations were found in estuary stations of Hunwan. The variations of t-PAH concentrations in seawater of Hunwan were influenced by land runoff.
The PAH compositional pattern, principal component analysis (PCA) and results from back trajectories demonstrated the major sources of atmospheric PAHs in Hengchun Peninsula, southern Taiwan were vehicular emissions. The seasonal variations in PAH concentration and composition were influence by Asian monsoon system. Gas-particle partition coefficients (Kp) of PAHs were well-correlated with the sub-cooled liquid vapor pressures (PoL), suggesting that the gas-particle partition of PAHs follows the characteristic of PAHs. The shallower slopes of log Kp versus log PoL suggest the presence of non-exchangeable fraction of PAHs in particle, likely associated to the soot carbon phase. The PAH compositional pattern, isomeric ratios and PCA of the Hengchun Peninsula coasts suggested that the source of PAHs in the Hengchun Peninsula coastal waters mostly from petroleum. The significant spatial difference between the spring and summer samples might be affected by a combination of land runoff and coastal currents. The partition coefficients between the particulate and dissolved phase (logKoc) were positively correlated with their logKow values, and higher than predicted values. The results suggest that the PAH associated with particles are present the extremely strongly bound, which could be attributed to the present of soot-like particles.
Air–water exchange fluxes of 4 polycyclic aromatic hydrocarbons (PAHs) were simultaneously measured in air and water samples from two sites in Hengchun Peninsula, from January to December 2010. The net fluxes of phenanthrene and pyrene were volatilization from water to air, and fluoranthene and chrysene were absorption from air to water. Due to PAH annual fluxes though air-water exchange, the seawater in Hengchun Peninsula is a source of low molecular weight PAHs and a reservoir of high low molecular weight PAHs.

論文審定書 i
論文公開授權書 ii
謝誌 iii
中文摘要 iv
ABSTRACT vi
表目錄 x
圖目錄 xi
第1章 簡介Introduction 1
1.1 多環芳香烴（PAHs）的概述 1
1.2 多環芳香烴的來源(emission)、宿命(fate)和傳輸(transport) 3
1.3 氣-固分配係數 5
1.4 液-固分配係數 6
1.5 水氣交換通量計算 7
1.6 研究地點現況描述 8
1.7 研究目的 9
第2章 材料與方法 10
2.1 空氣樣品採集 10
2.2 水樣採集 11
2.3 氣象資料及水溫和鹽度測量 12
2.4 空氣樣品處理 12
2.5 水樣處理 12
2.6 水中顆粒性有機碳分析 13
2.7 儀器分析 14
2.8 定量分析 14
2.9 品保與品管 15
2.10 資料分析 16
第3章 結果與討論 21
3.1 大氣中多環芳香烴的濃度及氣固分配 21
3.1.1 TSP和PAHs的濃度 21
3.1.2 總PAH濃度與其他地區相比 22
3.1.3 造成大氣濃度季節性變化的原因 22
3.1.4 PAH組成與來源 24
3.1.4.1 主成分分析(principal component analysis, PCA) 24
3.1.4.2 氣團逆軌跡分析 25
3.1.4.3 氣-固分配 26
3.2 水體中多環芳香烴的濃度 36
3.2.1 水中顆粒特性 36
3.2.2 水中PAHs的濃度之時空變化 36
3.2.3 總PAHs濃度與其他地區相比 36
3.2.4 水中PAHs的組成與來源 37
3.2.5 PAHs在溶解相和固相之間的分配係數 38
3.3 多環芳香烴之水氣交換通量 47
3.3.1 溶解相和氣相濃度 47
3.3.2 水氣交換通量 47
3.3.3 年交換通量與其他研究相比 48
第4章 結論與建議 54
4.1 結論 54
4.2 建議 55
參考文獻 56
附錄一 64
鄭金娥個人簡歷 65

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