大氣中多環芳香烴化合物(polycyclic aromatic hydrocarbons, PAHs)為環境中常見的有機化合物，當PAHs排放至大氣時會藉由擴散、傳輸、分解及去除過程而讓PAHs分佈在大氣的濃度有所改變，從大氣中掃除的過程包括了乾沉降和濕沉降，此一過程也是PAHs進入陸地及水體環境的重要傳輸路徑。本研究的主旨在於建立高雄海岸地區大氣PAHs的乾濕沉降資料，並利用特徵比、群集分析與主成分分析等統計工具來判斷其可能來源，以供未來政府環保單位擬定PAHs管制策略之重要參考，且有助於瞭解大氣中PAHs之傳輸與掃除機制。
採樣期間(2010年1月到12月)總懸浮微粒的乾沉降通量年平均為44.3 (6.60-384) mg/m2d，總懸浮微粒的濕沉降通量年平均為211 (56.1-738) mg/m2d，整年總PAHs的乾沉降通量平均為1500 (749-3760) ng/m2d，總PAHs的濕沉降通量年平均為8470 (2280-46000) ng/m2d。研究結果顯示，大氣總懸浮微粒濃度與總懸浮微粒的乾沉降通量在沙塵暴期間明顯比其他時期高，中元節期間則無特別改變。與之前文獻比較，大氣總PAHs濃度在中元節期間相對較低，推測是風向不同以及降雨所造成。懸浮微粒PM2.5/PM10的比例在沙塵暴期間有變低的現象，顯示沙塵暴期間粗顆粒較平常採樣期間為多，總懸浮微粒乾沉降速度與總PAHs乾沉降速度在沙塵暴期間比平常採樣期間高。在乾沉降通量估算方面，文獻上常使用總懸浮微粒的乾沉降速度及大氣中PAHs的顆粒相濃度來估算總PAHs乾沉降通量，與本研究實際量測的通量值比較，發現使用文獻方法的估計通量會有高估的情形。
相關性分析結果中，總懸浮微粒乾沉降通量與大氣中總懸浮微粒濃度、總懸浮微粒乾沉降速度成正相關，與降雨強度則呈負相關。總懸浮微粒乾沉降速度亦與大氣中總懸浮微粒濃度呈正相關。總PAHs乾沉降通量與大氣總懸浮微粒濃度、總PAHs乾沉降速度呈正相關，與降雨強度及溫度則呈負相關。總懸浮微粒濕沉降通量和總PAHs濕沉降通量皆與降雨強度呈正相關。PAHs指紋鑑定來源分析推測本採樣地區主要受到柴油燃燒來源，而群集分析和主成分分析結果則說明主要是受到船隻航行，貨櫃車、重機具所使用的柴油、重油所影響，但是特殊節日 (沙塵暴期間、中元節期間)則有不同的來源影響。

Polycyclic aromatic hydrocarbons (PAHs) are one of major classes of organic pollutants. As semi-volatile organic compounds, PAHs can be transported in the atmosphere and scavenged according to various processes (dry and wet deposition). Atmospheric deposition is an important pathway for the transfer of pollutants from atmosphere to the terrestrial and water surfaces. The objective of this research is to quantify the dry and wet deposition of the atmospheric PAHs in the Kaohsiung coastal area. Principal component analysis (PCA) and hierarchical cluster analysis (HCA) were also performed with diagnostic ratios to determine the potential sources of PAHs.
The mean dry and wet deposition fluxes of atmospheric total suspended particles (TSP) during the study period (January-December 2010) were estimated to be 44.3 (6.60-384) and 211 (56.1-738) mg/m2d, respectively. The annual mean total PAH fluxes in dry and wet deposition were 1500 (749-3760) and 8470 (2280-46000) ng/m2d, respectively. Both concentrations and dry deposition fluxes of TSP were much higher during dust storm. During Ghost Month, however, they were comparable with other sampling events. By comparing with literatures, the total PAH concentrations of TSP were relatively low during Ghost Month, suggesting that wind direction and precipitation might be plausible. The ratio of PM2.5/PM10 had a relatively low value during dust storm, indicating that coarse particle might be predominant. In addition, during dust storm, both TSP dry deposition velocity and total PAH dry deposition velocity were higher than other sampling events. Our findings in this study showed that previous attempts in literature to estimate total PAH dry deposition fluxes by using TSP dry deposition velocity and PAH concentrations could lead to overestimate fluxes in the field.
TSP dry deposition fluxes were positively correlated with atmospheric total TSP concentrations and TSP dry deposition velocity, but were correlated negatively with intensity of precipitation. In addition, TSP dry deposition velocity showed a positive correlation with TSP concentrations. Total PAH dry deposition fluxes were correlated positively with atmospheric total particulate concentrations and total PAH dry deposition velocity, but negatively with intensity of precipitation and temperature. However, TSP and total PAH fluxes in wet deposition were both correlated positively with intensity of precipitation. Diagnostic ratios showed that diesel exhaust was the main source of combustion-derived PAHs in the study. HCA and PCA analysis indicated that emissions from the ships and vehicles, and fuel used were the main sources of combustion-derived PAHs, while during special events, such as dust storm and Ghost Month, suggesting a different source of PAHs.

論文審定書......... i
謝誌........... ii
摘要................ iii
Abstract ............. v
目錄...... vii
圖目錄....... x
表目錄........ xii
附錄目錄...... xiii
第一章 前言 1
1-1 研究動機 1
1-2 研究內容及目的 1
第二章 文獻回顧 3
2-1 PAHs介紹 3
2-1-1 物理化學的特性 3
2-1-2 PAHs之形成機制 7
2-1-3 大氣中的來源 8
2-1-4 PAHs對人體的毒性 9
2-2 懸浮微粒 11
2-2-1 形成及來源 11
2-2-2 懸浮微粒對人體的影響 11
2-2-3 粒徑分佈 12
2-3 乾沉降 13
2-3-1 測量乾沉降的方法 13
2-3-2 影響大氣中乾沉降的因素 14
2-4 濕沉降 14
2-4-1 濕沉降的機制 14
2-4-2 PAHs的濕沉降 15
2-5 PAHs的化學指紋鑑定 16
第三章 實驗方法及步驟 17
3-1 材料與儀器 17
3-1-1 材料 17
3-1-2 試藥及器具的前處理 17
3-2 採樣步驟 18
3-2-1 採樣地點 18
3-2-2 採樣設備 19
3-2-3 採樣方法 20
3-3 PAHs分析 21
3-3-1 樣品前處理 21
3-3-2 氣相層析質譜儀分析 22
3-4 品保及品管 (QA/QC) 23
3-5 主成分及群集分析 24
第四章 結果與討論 33
4-1大氣中的懸浮微粒及總PAHs濃度 33
4-1-1 大氣中懸浮微粒濃度逐月變化趨勢 33
4-1-2 大氣中總PAHs濃度逐月變化趨勢 39
4-2 乾沉降通量 45
4-2-1 總懸浮微粒乾沉降通量及乾沉降速度 45
4-2-2 總PAHs乾沉降通量及乾沉降速度 49
4-2-3 海岸地區總PAHs乾沉降通量的估計值與實際值的比較 52
4-3 濕沉降 54
4-3-1 總懸浮微粒濕沉降通量 54
4-3-2 總PAHs的濕沉降通量 55
4-3-3 總PAHs的濕沉降掃除率 56
4-4 相關性分析 63
4-5 大氣中PAHs來源分析 66
4-5-1 化學指紋鑑定 66
4-5-2 主成分及群集分析 68
第五章 結論與建議 87
5-1 結論 87
5-2 建議 89
參考文獻 90
附錄 97

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