本研究調查位於台灣南部高雄市內工業區附近四個採樣測站大氣細懸浮微粒(PM2.5)上多環芳香烴(PAHs)之濃度時空變化及可能來源。採樣測站包括大寮區(DL)、鳳山區(FS)、仁武區(RW)和橋頭區(CT)。於2016年9月至2017年8月期間共採集90份樣品，定量其PM2.5濃度，並透過氣相層析質譜儀(GC-MS)測定16種PM2.5上PAHs濃度(以下簡稱PM2.5-PAHs)。進一步使用特徵比、主成分分析(PCA)以及階層群集分析(HCA)來判別PAHs的潛在來源。研究結果顯示DL、FS、RW和CT測站之PM2.5年平均濃度分別為45.8 ± 16.3, 47.6 ± 21.0, 48.3 ± 17.2及51.4 ± 14.3 μg m-3，其對應之PAHs濃度分別為1.52 ± 0.79, 1.48 ± 1.03, 1.11 ± 0.68及1.35 ± 1.13 ng m-3。根據PM2.5-PAHs的物種組成比例，高分子量(HMW) PAHs比低分子量(LMW) PAHs在PM2.5上更佔優勢。而在DL、FS、RW和CT測站的毒性當量濃度(BaPeq)在年平均濃度分別為0.215 ± 0.116, 0.217 ± 0.145, 0.171 ± 0.094以及0.179 ± 0.130 ng m-3。四個測站的BaP濃度占總毒性當量濃度的49% ~ 52%。在本研究中PM2.5、PM2.5-PAHs和BaPeq呈現季節性變化，冬季濃度較高，夏季較低，且濃度皆與大氣溫度呈負相關。特徵比、PCA和HCA的分析結果亦顯示了不同季節PM2.5-PAHs的兩個主要來源，包括固定排放如煤炭燃燒和石油燃燒，與交通排放如汽油和柴油引擎車輛尾氣。在健康風險評估方面，暴露於本研究年平均毒性當量濃度(BaPeq)最高之FS測站PM2.5-PAHs之年平均吸入性增量終生癌症風險值(ILCR)為0.262×10-6，低於美國環境保護局所訂之一般民眾可允許暴露於致癌物質的危害風險之建議值(10-6)。

In this study, spatiotemporal variation and potential sources of PM2.5-bound polycyclic aromatic hydrocarbons (PAHs) were investigated for four sampling sites located close to air-polluting industrial area in Kaohsiung City, southern Taiwan. The sampling sites included Daliao (DL), Fongshan (FS), Renwu (RW) and Ciaotou District (CT). A total of 90 PM2.5 samples with 16 PAHs collected from September 2016 to August 2017 were analyzed. The concentrations of 16 PAHs were determined through gas chromatography–mass spectrometry. Diagnostic ratios, principle components analysis (PCA) and hierarchical cluster analysis (HCA) were applied to identify potential PAHs sources. The results revealed the annual mean PM2.5 concentrations were 45.8 ± 16.3, 47.6 ± 21.0, 48.3 ± 17.2 and 51.4 ± 14.3 μg m-3 for DL, FS, RW and CT sites, respectively, while their corresponding PAHs concentrations were 1.52 ± 0.79, 1.48 ± 1.03, 1.11 ± 0.68 and 1.35 ± 1.13 ng m-3. According to the component pattern of PM2.5-bound PAHs, the high molecular weight (HMW) PAHs were dominant on PM2.5 compared to the lower molecular weight (LMW) PAHs. The annual average benzo[a]pyrene equivalent (BaPeq) concentrations in PM2.5 at DL, FS, RW and CT sites were 0.215 ± 0.116, 0.217 ± 0.145, 0.161 ± 0.094 and 0.179 ± 0.130 ng m-3, respectively. BaP was found accounted for 49% to 52% of BaPeq concentrations in PM2.5 at four sites. In the present study, PM2.5, PM2.5-bound PAHs and BaPeq showed seasonal variations, the higher concentrations were found in winter while the lower ones were found in summer. There was a negative correlation between concentrations and atmospheric temperatures. The results of diagnostic ratios, PCA and HCA illustrated two major sources of PM2.5-bound PAHs in different seasons, including stationary emissions, such as coal combustion and petroleum burning, and vehicular emissions from gasoline and diesel engines. The annual average incremental lifetime cancer risk (ILCR) from inhaling exposure to PM2.5-bound PAHs at FS site was quantified as 0.262×10-6, which was lower than the criterion specified in the United States Environmental Protection Agency guidelines (10-6).

論文審定書 i
誌謝 ii
摘要 iii
Abstract iv
目錄 vi
圖目錄 ix
表目錄 xi
附表目錄 xiii
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 大氣懸浮微粒介紹 3
2-1-1 大氣懸浮微粒來源 3
2-1-2 懸浮微粒對人體之影響 3
2-2 多環芳香烴介紹 4
2-2-1 多環芳香烴特性 4
2-2-2 大氣中多環芳香烴之來源 7
2-2-3 多環芳香烴之化學指紋特徵鑑定 9
2-2-4 多環芳香烴之危害 10
2-3 大氣中細懸浮微粒與多環芳香烴之相關研究 13
第三章 研究方法 14
3-1 研究流程 14
3-2 材料與儀器 15
3-2-1 材料 15
3-2-2 試藥及器具前處理 16
3-2-3 設備與分析儀器 16
3-3 採樣與保存 17
3-3-1 採樣地點描述 17
3-3-2 採樣時間 18
3-3-3 採樣方法 18
3-4 樣品分析 20
3-4-1 PM2.5樣品分析 20
3-4-2 PAHs樣品分析 20
3-5 品質保證與品質管制(QA/QC) 22
3-5-1 空白試驗 22
3-5-2 方法偵測極限 22
3-5-3 擬似標準品回收率 22
3-6 資料分析 23
3-6-1 特徵比 23
3-6-2 主成分分析 23
3-6-3 階層群集分析 23
3-7 致癌風險計算 24
第四章 結果與討論 25
4-1 大氣中細懸浮微粒濃度 25
4-1-1 兩種採樣器之PM2.5實測濃度比較 25
4-1-2 PM2.5濃度空間分布 29
4-1-3 PM2.5濃度季節變化 33
4-2 大氣多環芳香烴濃度 35
4-2-1 兩種採樣器之PM2.5-PAHs實測濃度比較 35
4-2-2 PM2.5-PAHs濃度時空變化 37
4-2-3 PM2.5-PAHs之物種組成 43
4-2-4 PM2.5與PM2.5-PAHs之相關性 47
4-3 PAHs來源分析 50
4-3-1 特徵比 50
4-3-2 主成分分析 54
4-3-3 階層群集分析 60
4-4 大氣中多環芳香烴毒性當量因子 67
4-4-1 大氣中PM2.5-BaP濃度時空變化 67
4-4-2 大氣中毒性當量濃度(BaPeq) 70
4-4-3 致癌風險評估 73
第五章 結論與建議 74
5-1 結論 74
5-2 建議 76
參考文獻 77
附錄 86

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