本研究探討大台北地區大氣中細懸浮微粒(PM2.5)和多環芳香烴(PAHs)之時空變化，以及環境健康風險評估，於2015年1月至2016年4月期間，在大台北地區設置6個PM2.5採樣測站，分別有代表工業區的林口(LK)測站、商業區板橋(BQ)和萬華(WH)測站、住宅區的新店(XD)和松山(SS)測站及郊區的士林(SL)測站。研究結果顯示各測站PM2.5年平均濃度以BQ最高，SL最低；分別為LK(39.6±17.0 μg/m3)、BQ(44.0±15.2 μg/m3)、XD(39.1±17.8 μg/m3)、SL(36.5±14.3 μg/m3)、WH(41.0±13.9 μg/m3)和SS測站(36.8±13.9 μg/m3)。而在PAHs方面也是以BQ最高，但最低點為LK。各採樣測站PAHs年平均濃度分別為LK (0.99±0.65 ng/m3)、BQ (1.42±0.94 ng/m3)、XD (1.10±0.86 ng/m3)、SL (1.14±0.90 ng/m3)、WH (1.33±0.91 ng/m3)和SS (1.24±0.80 ng/m3)。PM2.5和PAHs有明顯的季節變化趨勢，大致上呈現夏季濃度較低，春、冬季濃度較高。和氣象因素的相關性分析結果，PM2.5的濃度和風速有顯著的負相關，PAHs則和溫度有顯著的負相關，顯示出風速較大有利於PM2.5的擴散與高溫利於PAHs的揮發。根據主成分分析(PCA)、階層群集分析(HCA)和特徵比(diagnostic ratio)發現，大台北地區6個採樣測站污染源皆以汽柴油混和的交通工具排放為主，顯示大台北地區的空氣受交通污染源影響高過於工業區影響。而在BQ、XD、SL、WH測站有些許廢棄物焚燒之特徵。環境健康風險評估方面，各採樣測站毒性當量(BaPeq)平均濃度為LK(0.09 ng/m3)、BQ(0.13 ng/m3)、XD(0.09 ng/m3)、SL(0.09 ng/m3)、WH(0.12 ng/m3)和SS(0.11 ng/m3)，而在計算個體終生致癌風險度時則需考慮個體差異及不確定因素。

This study aims to research spatial distribution and seasonal variation of 16 fine particulate matter (PM2.5) bound polycyclic aromatic hydrocarbons (PAHs) and their cancer risk assessments in Taipei ambient air. Ambient air samples of 6 sites including industrial area (LK), commercial areas (BQ, and WH), residential areas (XD, and SS) and suburban area (SL), were collected twice a month from January 2015 to April 2016. BQ exhibited the highest annual average PM2.5 concentration; while SL the lowest. The annual average concentrations of PM2.5 at LK, BQ, XD, SL, WH, and SS sites were 39.6±17.0, 44.0±15.2, 39.1±17.8, 36.5±14.3, 41.0±13.9, and 36.8±13.9 μg/m3, respectively. BQ also exhibited the highest annual mean PM2.5-PAHs concentration, while LK the lowest. Our result indicated the vehicle emission was dominant compared with industrial emission in the study area. Annual mean concentrations of PM2.5-PAHs were 0.99±0.65, 1.42±0.94, 1.10±0.86, 1.14±0.90, 1.33±0.91, and 1.24±0.80 ng/m3 at LK, BQ, XD, SL, WH, and SS sites, respectively. Significant seasonal variations were found in PM2.5 and PM2.5-PAHs in this study. In general, the concentrations were relatively low in summer and high in spring and winter. Correlation analysis with meteorological parameters indicated that PM2.5 was negatively correlated with wind speed; while PM2.5-PAHs was negatively correlated with temperature. Principle components analysis (PCA), hierarchical cluster analysis (HCA), and diagnostic ratio were performed to investigate the sources of PM2.5-PAHs. Vehicle emission, including gasoline and diesel engines, was the predominant source in Taipei urban area; while incineration and coal combustion emissions were also found. In cancer risk assessments among 6 sites, the concentrations of BaPeq were 0.09, 0.13, 0.09, 0.09, 0.12 and 0.11 ng/m3 at LK, BQ, XD, SL, WH, and SS, respectively. Individual differences and other conditions should be concerned when cancer risk assessment was calculated.

目錄
論文審定書 i
誌謝 ii
摘要 iii
Abstract iv
圖目錄 ix
表目錄 xi
附表 xii
第一章 前言 1
1-1 研究背景 1
1-2 研究目的 3
第二章 文獻回顧 4
2-1 懸浮微粒(Particulate matter)介紹 4
2-1-1 大氣環境中PM來源 4
2-1-2 PM2.5對人體健康之影響 5
2-2 多環芳香烴類(PAHs)介紹 5
2-2-1 PAHs物化特性 5
2-2-2 PAHs對人體健康之影響 6
2-2-3 PAHs形成原因 9
2-2-4 大氣環境中PAHs來源 9
2-3 都市環境中的PM2.5、PM2.5-PAHs來源與其影響因素 12
第三章 研究方法 14
3-1 研究架構與流程 14
3-2 材料與儀器 15
3-2-1 材料 15
3-2-2 試藥器具及處理方法 16
3-2-3 設備與分析儀器 17
3-3 樣品採集 18
3-3-1 採樣時間與地點 18
3-3-2 採樣方法 20
3-4 樣品分析 20
3-4-1 PAHs分析 20
3-5 品保及品管(QA/QC) 23
3-5-1 空白實驗 23
3-5-2 方法偵測極限 23
3-5-3 擬似標準品回收率 23
3-6 統計方法及來源分析 24
3-6-1 主成分分析(Principle Components Analysis, PCA) 24
3-6-2 階層群集分析(Hierarchical Cluster Analysis, HCA) 24
3-6-3 特徵比(Diagnostic ratio) 25
3-7 致癌風險評估(Cancer risk assessment) 25
第四章 結果與討論 26
4-1 大氣中PM2.5濃度 26
4-1-1 PM2.5濃度空間分布 26
4-1-2 PM2.5濃度季節差異 31
4-2 大氣中PM2.5-PAHs濃度 35
4-2-1 大氣中PM2.5-PAHs濃度分布 35
4-2-2 大氣中PM2.5-PAHs成分組成 41
4-2-3 PM2.5與PM2.5-PAHs之關係 47
4-3 PAHs來源判斷分析 48
4-3-1 主成分分析(Principle Components Analysis, PCA) 48
4-3-2 階層群集分析(Hierarchical Cluster Analysis, HCA) 59
4-3-3 特徵比(Diagnostic Ratio) 66
4-4 大氣環境中PM2.5-PAHs致癌風險評估 68
4-4-1 大氣環境中PM2.5-BaP濃度時空變化 68
4-4-2 大氣環境致癌風險評估 69
第五章 結論與建議 71
5-1 結論 71
5-2 建議 72
參考文獻 73

圖目錄
圖2-1 PAHs之分子結構 8
圖3-1 研究架構流程圖 14
圖3-2 採樣位置圖 19
圖3-3 PAHs實驗分析流程 22
圖4-1 各採樣測站PM2.5濃度趨勢圖 31
圖4-2 採樣測站PM2.5平均濃度和風速 32
圖4-3 本研究和環保署(EPA)空氣品質監測站逐月濃度趨勢比較 34
圖4-4 採樣測站PM2.5-PAHs平均濃度和溫度 39
圖4-5 各採樣測站PM2.5-PAHs濃度逐月變化 40
圖4-6 各採樣測站PM2.5-PAHs濃度四季差異 40
圖4-7 各採樣測站PM2.5-PAHs環數分布比例(%) 42
圖4-8 各採樣測站PM2.5-PAHs物種差異分布(%) 43
圖4-9 測站平均PM2.5與PM2.5-PAHs濃度趨勢 47
圖4-10 LK測站PAHs主成分分析分數圖(PC1 vs PC2) 53
圖4-11 BQ測站PAHs主成分分析分數圖(PC1 vs PC2) 53
圖4-12 XD測站PAHs主成分分析分數圖(PC1 vs PC2) 54
圖4-13 SL測站PAHs主成分分析分數圖(PC1 vs PC2) 54
圖4-14 WH測站PAHs主成分分析分數圖(PC1 vs PC2) 55
圖4-15 SS測站PAHs主成分分析分數圖(PC1 vs PC2) 55
圖4-16 LK測站PAHs主成分分析分數圖(PC2 vs PC3) 56
圖4-17 BQ測站PAHs主成分分析分數圖(PC2 vs PC3) 56
圖4-18 XD測站PAHs主成分分析分數圖(PC2 vs PC3) 57
圖4-19 SL測站PAHs主成分分析分數圖(PC2 vs PC3) 57
圖4-20 WH測站PAHs主成分分析分數圖(PC2 vs PC3) 58
圖4-21 SS測站PAHs主成分分析分數圖(PC2 vs PC3) 58
圖4-22 LK測站群集分析和Cluster相對濃度分布 60
圖4-23 BQ測站群集分析和Cluster相對濃度分布 61
圖4-24 XD測站群集分析和Cluster相對濃度分布 62
圖4-25 SL測站群集分析和Cluster相對濃度分布 63
圖4-26 WH測站群集分析和Cluster相對濃度分布 64
圖4-27 SS測站群集分析和Cluster相對濃度分布 65
圖4-28 特徵比分析(以測站劃分) 67
圖4-29 特徵比分析(以季節劃分) 67

表目錄
表2-1 美國環保署列出的16種優先管制PAHs及其物化特性 7
表4-1 各採樣測站PM2.5濃度(μg/m3) 27
表4-2 國內外PM2.5濃度比較(μg/m3) 29
表4-3 PM2.5實測值和氣候因素相關性 32
表4-4 本研究PM2.5實測值和環保署測站(EPA)監測值之相關性 33
表4-5 各採樣測站PM2.5-PAHs平均濃度(ng/m3) 36
表4-6 國內外PM2.5-PAHs濃度比較(ng/m3) 37
表4-7 PM2.5-PAHs實測值和氣候因素相關性 41
表4-8 各採樣站PM2.5-16PAH濃度季節變化(ng/m3) 44
表4-9 各採樣測站PAHs環數高低分布所佔比例(%) 46
表4-10 各採樣測站PAHs轉軸後主成分分析因素負荷表 50
表4-11 國際間PM2.5-BaP相關標準規範 68
表4-12 本研究各測站四季BaP濃度(ng/m3) 68
表4-13 PAHs物種毒性當量係數(Nisbet & Lagoy, 1992) 69
表4-14 各採樣測站BaPeq濃度(ng/m3) 70

附表
附表1 空白實驗及偵測極限(MDL)(ng) 81
附表2 擬似標準品回收率 82
附表3 LK測站PAHs濃度(ng/m3) 83
附表4 BQ測站PAHs濃度(ng/m3) 86
附表5 XD測站PAHs濃度(ng/m3) 89
附表6 SL測站PAHs濃度(ng/m3) 92
附表7 WH測站PAHs濃度(ng/m3) 95
附表8 SS測站PAHs濃度(ng/m3) 98
附表9 各測站採樣期間平均溫度(℃) 101
附表10 各測站採樣期間平均相對濕度(%) 102
附表11 各測站採樣期間平均風向(degress) 103
附表12 各測站採樣期間平均風速(m/sec) 104

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