本研究於2012年12月至2013年11月期間，分別於高雄市內四個區域：南高雄(小港區：SG)、北高雄(左營區：FS)、高雄市市區(三民區：AG)，高雄海岸地區(鼓山區：NSYSU) 採集大氣懸浮微粒(PM2.5和PM2.5~10)與多環芳香烴化合物(Polycyclic aromatic hydrocarbons, PAHs)並量化其濃度，以探討高雄不同區域之大氣懸浮微粒與多環芳香烴污染物之時空變化，和可能之污染來源，進而了解高雄地區的污染情形。
本研究結果顯示SG、AG、FS以及NSYSU大氣中PM2.5的年平均濃度依序分別為65.1、62.8、68.6和60.9 μg m-3，而PM2.5~10的年平均濃度則分別為21.9、24.4、23.3和21.5 μg m-3，整體而言，PM2.5濃度以FS最高，其次為SG，濃度最低為NSYSU，本研究之PM2.5樣品大多數皆超過我國「空氣品質標準」之24小時標準值 (35 μg m-3)，而PM10大部分皆符合我國之空氣品質標準 (125 μg m-3)。大氣中SG、AG、FS以及NSYSU多環芳香烴濃度(氣相加顆粒相)依序為15.0、14.2、12.8、7.32 ng m-3，整體而言，以SG濃度最高，其次為AG，NSYSU濃度最低。
除了SG於11月第二次採樣之外，其餘BaP顆粒相濃度數據皆符合UK的標準制定值(0.25 ng m-3)。本研究使用毒性當量因子(toxic equivalent factors, TEF)將測得之多環芳香烴濃度轉換成BaP equivalents (BaPeq)，本研究之顆粒相平均BaPeq為0.20 ng m-3 (SG)、0.18 ng m-3 (AG)、0.18 ng m-3 (FS)以及0.11 ng m-3 (NSYSU)。
化學指紋特徵比、主成分分析以及群集分析判斷出不同區域可能之污染來源，本研究之氣相多環芳香烴來源以石油性以及石油性燃燒兩者為主。PM2.5多環芳香烴來源則是SG及NSYSU為汽油引擎排放及石油性燃燒之混和性來源，AG以汽油引擎排放為主，FS大多數為交通排放來源；PM2.5~10多環芳香烴來源SG則是大多數偏向以柴油引擎燃燒排放為主，AG以汽油引擎燃燒為主，FS大多數為交通排放來源；NSYSU大多數以柴油引擎燃燒為主。

Polycyclic aromatic hydrocarbons were collected in PM2.5 and PM2.5–10 samples for four regions in Kaohsiung from December 2012 to November 2013. The sampling sites included southern Kaohsiung (Siaogang District, SG), northern Kaohsiung (Zuoying District, FS), the downtown (Sanmin District, AG), and coastal area (Gushan District, NSYSU). Particulate matters, the gaseous and particulate polycyclic aromatic hydrocarbons (PAHs) were analyzed to explore the temporal and spatial variations of atmospheric pollution in Kaohsiung. Moreover, the potential sources of PAHs were identified as well.
The annual mean concentrations of atmospheric PM2.5 (PM2.5~10) at SG, AG, FS, and NSYSU were 65.1 (21.9), 62.8 (24.4), 68.6 (23.3), and 60.9 (21.5) μg m-3, respectively. The highest concentration of PM2.5 was found at FS, followed by SG, while the lowest one was found at NSYSU. Most samples exceeded the 24-hr air quality standards of PM2.5 (35 μg m-3); while only a few PM10 did not meet the standards (125 μg m-3). Atmospheric concentrations of total PAHs (gas + particulate phase) at SG, AG, FS, and NSYSU were 15.0, 14.2, 12.8, and 7.32 ng m-3, respectively. It was found that SG had the highest concentration of total PAHs, followed by AG, FS, and NSYSU.
In this study, the BaP concentrations in the particulate samples were all below the UK regulation (0.25 ng m-3) except for one sample in November at SG. The average BaP equivalents (BaPeq), used for the carcinogenic risk assessment of PAHs, in the particulate samples were 0.20 ng m-3 (SG), 0.18 ng m-3 (AG), 0.18 ng m-3 (FS), and 0.11 ng m-3 (NSYSU).
The results of diagnostic ratios, HCA and PCA demonstrated that petroleum combustion was the main sources of gaseous PAHs. For PM2.5, the results of HCA and PCA both suggested that sources of PAHs mainly came from the local gasoline engine emissions, with partially contribution of petroleum combustion in SG and NSYSU, gasoline gngine exhausts in AG, and vehicular emissions in FS; while the main source for PM2.5~10 was diesel engine exhausts for SG and NSYSU, gasoline engine exhausts for AG, and vehicular emissions for FS.

摘要 iii
Abstract iv
目錄 vi
表目錄 ix
圖目錄 xi
附表目錄 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多環芳香烴介紹 3
2-1-1多環芳香烴特性 3
2-1-2多環芳香烴來源 6
2-1-3多環芳香烴毒性 7
2-1-4多環芳香烴化學指紋特徵鑑定 11
2-2-1大氣中懸浮微粒形成及來源 13
2-2-2懸浮微粒對人體之影響 13
第三章 研究方法 15
3-1研究流程 15
3-2材料與儀器 16
3-2-1材料 16
3-2-2試藥及器具前處理。 16
3-3 採樣與保存 18
3-3-1採樣時間與地點 18
3-3-2設備與分析儀器 19
3-3-3採樣方法 20
3-4樣品分析 21
3-4-1 PAHs分析 21
3-5品保及品管(QA/QC) 23
3-5-1擬似標準品回收率 23
3-5-2實驗空白 23
3-5-3方法偵測極限(Method Detection Limit, MDL) 24
3-6主成分分析(Principal Components Analysis, PCA) 25
3-7群集分析(Hierarchical Cluster Analysis, HCA) 25
第四章、結果與討論 26
4-1 大氣中懸浮微粒濃度 26
4-1-1懸浮微粒濃度空間分布 26
4-1-2 懸浮微粒濃度季節性變化 33
4-2 大氣中多環芳香烴濃度 38
4-2-1 多環芳香烴濃度時空變化 38
4-2-2 氣相、顆粒相多環芳香烴濃度分佈 49
4-2-3 懸浮微粒與多環芳香烴之關係 61
4-3 大氣中多環芳香烴之毒性當量因子 62
4-3-1 大氣中BaP濃度時空變化 62
4-3-2 大氣中BaPeq時空變化 67
4-4 來源判斷分析 74
4-4-1 化學指紋特徵(diagnostic ratio) 74
4-4-2 主成分分析(Principal Component Analysis, PCA) 81
4-4-3 階層群集分析(Hierarchical Cluster Analysis, HCA) 97
第五章 結論與建議 121
5-1 結論 121
5-2 建議 123
參考文獻 124
附錄 130

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