本研究利用高流量空氣採樣器 (PS-1)及階段式衝擊器 (MOUDI)分析高雄市（左營站及小港站）四季大氣中多環芳香烴 (PAHs)之濃度特徵，並藉由粒徑分析探討多環芳香烴濃度於不同粒徑之分佈，最後利用受體模式 (CMB)分析高雄市境內之可能污染來源。

左營站之PAHs濃度以夏季 (81.4 ng/m3)為最低，以冬季 (143.9 ng/m3)濃度為最高；小港站之PAHs濃度亦以夏季 (95.2 ng/m3)為最低，以冬季 (182.9 ng/m3)濃度為最高。左營站及小港站之低分子量PAHs (LW-PAHs)大多以氣相為主，其所佔百比分別為55.89 - 95.89 ％及67.07 - 96.61 ％。高分子量PAHs (HW-PAHs)以顆粒相為主，所佔比例分別為55.24 - 83.50 ％及46.87 - 77.26 ％。

在PAHs之粒徑分佈上，左營站及小港站之d50分別為0.89 μm及0.35 μm，顯示左營站及小港站附著於懸浮微粒上之PAHs以細微粒 (＜1.0 μm)為主。

利用化學質量平衡 (CMB)，以20種PAHs（除NaP外）模擬污染來源結果顯示，左營站PAHs排放來源最高為移動源 (49 - 62 ％)；小港站PAHs排放來源最高為燃燒源 (49 - 64 ％)。

The high-volume air sampling (PS-1) and micro-orifice uniform deposit impactor (MOUDI) were used to measure the concentrations of polycyclic aromatic hydrocarbons (PAHs) in the atmosphere for four seasons at Zuoying and Siaogang in Kaohsiung city, together with the size distributions. Also, the CMB (Chemical Mass Balance) receptor model was employed to determine the potential sources of PAHs.

The results show that the highest concentrations of PAHs occurred in winter, being 143.9 ng/m3 and 182.9 ng/m3 at Zuoying and Siaogang, respectively; while the lowest concentrations of PAHs occurred in summer, being 81.4 ng/m3 and 95.2 ng/m3. The low-weight PAHs in the two sites were abundant in gaseous phase, being 55.89 - 95.89 % and 67.07 - 96.61 % at Zuoying and Siaogang, respectively. Meanwhile, the high-weight PAHs were almost present in particulate phase, being 55.24 - 83.50 % and 46.87 - 77.26 % at Zuoying and Siaogang, respectively.

The sizes of 50th percentile of cumulative size distribution, d50 of Zuoying and Siaogang were 0.89 μm and 0.35 μm, respectively. Hence, most atmospheric PAHs existed in fine-particle ranges (＜1.0μm).

The results of by CMB receptor modeling indicated that the major sources of pollution was exhaust emission (49 - 62 %) in Zuoying, and was burning source (49 - 64 %) in Siaogang.

總目錄
頁碼
中文摘要 Ⅰ
總目錄 Ⅱ
表目錄 Ⅴ
圖目錄 Ⅶ
附表目錄 Ⅷ

第一章 前言 1-1
1-1 研究緣起 1-1
1-2 研究目標 1-1

第二章 相關研究及文獻回顧 2-1
2-1 高雄市近年空氣及氣象背景資料概述 2-1
2-1-1 空氣品質PSI變化趨勢 2-1
2-1-2 各空氣污染物濃度變化趨勢 2-3
2-1-3 高雄市空氣污染物排放量概估 2-7
2-1-4 高雄地區歷年氣象概述 2-10
2-2 多環芳香烴化合物 (PAHs) 2-13
2-2-1 多環芳香烴化合物特性 2-13
2-2-2 PAHs之危害 2-17
2-2-3 PAHs之來源 2-21
2-2-4 多環芳香烴化合物濃度變化特性解析 2-25
2-2-5 多環芳香烴化合物粒徑分佈特性 2-25
2-3 多環芳香烴化合物之乾沉降 2-27
2-3-1 乾沉降機制 2-27
2-3-2 大氣中影響乾沉降之因素 2-28
2-3-3 乾沉降速度與乾沉降通量 2-28
2-4 懸浮微粒簡介 2-29
2-4-1 懸浮微粒定義 2-29
2-4-2 懸浮微粒形成及來源 2-30

第三章 研究方法與步驟 3-1
3-1 研究架構與流程 3-1
3-2 現場採樣 3-2
3-2-1 大氣中多環芳香烴化合物採樣規劃 3-2
3-3 採樣方法與設備 3-3
3-3-1 大氣採樣濃度 3-3
3-3-2 乾沉降採樣 3-5
3-3-3 懸浮微粒粒徑分析 3-6
3-3-4 樣品分析 3-7
3-4 多環芳香烴化合物之來源分析 3-9
3-4-1 CMB8模式理論基礎 3-9
3-4-2多環芳香烴化合物之污染來源分析 3-13
3-5 多環芳香烴化合物分析之品質保證與品質控制 3-13
3-5-1 空白試驗 3-13
3-5-2 方法偵測極限 3-14
3-5-3 減量線之配置 3-14
3-5-4 準確度 3-15
3-5-5 精密度(RSD) 3-16

第四章 結果與討論 4-1
4-1 大氣中多環芳香烴化合物(PAHs)濃度 4-1
4-1-1 採樣時間之氣象資料 4-1
4-1-2 大氣中懸浮微粒濃度 4-3
4-1-3 大氣中PAHs濃度 4-4
4-1-4 大氣中各環數PAHs分佈濃度 4-8
4-1-5 大氣中PAHs之氣/顆粒相分佈 4-10
4-2 乾沉降 4-12
4-2-1 總懸浮微粒乾沉降通量 4-12
4-2-1 總懸浮微粒乾沉降速度 4-13
4-3 粒徑分析 4-14
4-3-1 總懸浮微粒濃度 4-15
4-3-2 大氣中總PAHs之粒徑分佈 4-17
4-3-3 總懸浮微粒及總PAHs濃度之累積百分比 4-19
4-4 受體模式(CMB)模擬結果 4-21
4-4-1 CMB模式指紋資料之建立 4-21
4-4-2 大氣中PAHs污染源排放量推估 4-27
4-4-3 大氣中PAHs污染源貢獻百分比 4-32
4-5 PAHs之特徵比值及毒性等値因子 4-34
4-5-1 大氣中PAHs之污染來源 4-34
4-5-2 大氣中PAHs之毒性等値因子 4-35

第五章 結論與建議 5-1
5-1 結論 5-1
5-2 建議 5-3

參考文獻 ..參-1

附錄A 多環芳香烴化合物濃度採樣原始數據表…………...…附A-1






表目錄
頁碼
表2-1-1.1 民國86-94年高雄市四空品測站臭氧 (O3)事件日每年之天數 2-2
表2-1-1.2 民國86-94年高雄市四空品測站懸浮微粒 (PM10)事件日每年之天數 2-2
表 2.1-3 民國89年高雄市各污染源排放總表 2-9
表2-1-4 高雄地區近十年各月份平均氣象資料統計表 2-12
表2-2-1.1 21種PAHs之分子量、結構式及物理特性 2-14
表2-2-1.2 PAHs之蒸氣壓於25 ℃水中之溶解度與親電性反應 (Eπ) 2-16
表2-2-2 21種PAHs 之致癌性 2-20
表2-2-3 各污染源所產生的PAHs物種 2-22
表3-2-1 採樣日期 3-3
表3-3-3 MOUDI各階層截取粒徑 3-7
表3-4-1 CMB8模式統計指標判定準則 3-13
表3-5-3.1 PAHs標準品之成分及濃度 (Supelco) 3-17
表3-5-3.2 PAHs標準品之成分及濃度(Chem Service) 3-17
表3-5-3.3 PAHs標準品之成分及濃度 (Riedel-de Haёn) 3-17
表3-5-3.4 PAHs 標準品之成分及濃度 (Accu Standard) 3-17
表3-5-3.5 21種PAHs標準品原液稀釋成10 μg/ml之GC/FID圖譜積分面積 3-18
表3-5-3.6 21種PAHs標準品原液稀釋成10 μg/ml之GC/FID圖譜積分面積平均值、標準偏差及相對標準偏差 3-19
表3-5-3.7 標準品檢量線 3-20
表3-5-3.8 21種PAHs標準品於GC/FID之滯留時間 (min) 3-21
表3-5-3.9 21種PAHs標準品GC/FID滯留時間之平均值及標準偏差 3-22
表3-5-4.1 21種標準品之回收率 3-23
表3-5-5.1 標準品回收率之精密度及準確度 3-24
表4-1-1.1 左營站採樣時間氣象資料 4-2
表4-1-1.2 小港站採樣時間氣象資料 4-2
表4-1-2.1 左營站懸浮微粒濃度 4-3
表4-1-2.2 小港站懸浮微粒濃度 4-4
表4-1-3.1 PAHs環數之分佈 4-5
表4-1-3.2 左營站PAHs濃度 4-6
表4-1-3.3 小港站PAHs濃度 4-7
表4-1-3.4 左營站及小港站四季PAHs濃度 (ng/m3) 4-8
表4-1-3.5 台灣其他地區大氣中PAHs濃度 ( ng/m3 ) 4-8
表4-3 左營站及小港站PAHs氣粒相比 (％) 4-11
表4-2-1 各文獻懸浮微粒沉降通量 (mg/m2 day) 4-13
表4-2-2 各文獻懸浮微粒乾沉降速度 (cm/s) 4-14
表4-4-1 固定源及移動源PAHs之指紋資料 4-25
表4-4-2.1 左營站之燃燒源、餐飲排放及移動源佔大氣中PAHs之濃度分佈 4-29
表4-4-2.2 小港站之燃燒源、餐飲排放及移動源佔大氣中PAHs之濃度分佈 4-30
表4-4-2.3 左營站及小港站之燃燒源、餐飲排放及移動源佔大氣中PAHs季平均之濃度分佈 4-31
表4-5-1 PAHs之特徵比值 4-34
表4-5-1.1 國外BaP濃度容許值或建議值 4-36
表4-1-1.2 國內BaP以及BaPeq濃度值 (ng/m3) 4-37
表4-5-2 毒性當量係數 (Toxicology Equivalent Factor) 4-37




圖目錄
頁碼
圖2-1-1 高屏地區空氣品質現況(84 - 94) 2-1
圖2-1-2.1 高雄市各測站PM10逐月濃度變化趨勢 2-4
圖2-1-2.2 高雄市各測站SO2逐月濃度變化趨勢 2-5
圖2-1-2.3 高雄市各測站O3逐月濃度變化趨勢 2-6
圖2-4-2 大氣氣膠表面積粒徑分佈 2-32
圖3-1-1 研究架構流程圖 3-1
圖3-2-1 高雄市地區PAHs採樣點周界環境示意圖 3-2
圖3-3-1 高流量PS-1空氣採樣器 3-4
圖3-3-2 乾沈降採樣器 3-5
圖3-3-3 MOUDI階段式衝擊器 3-6
圖4-1-4.1 左營站及小港站低分子量PAHs (LW-PAHs)之四季濃度變化 4-9
圖4-1-4.2 左營站及小港站中分子量PAHs (MW-PAHs)之四季濃度變化 4-9
圖4-1-4.3 左營站及小港站高分子量PAHs (HW-PAHs)之四季濃度變化 4-10
圖4-1-4.4 左營站及小港站之總PAHs (TPAHs)之四季濃度變化 4-10
圖4-3-1.1 左營站總懸浮微粒之粒徑濃度 4-16
圖4-3-1.2 小港站總懸浮微粒之粒徑濃度 4-16
圖4-3-1.3 左營站總PAHs之粒徑濃度分佈 4-18
圖4-3-1.4 小港站總PAHs之粒徑濃度分佈 4-18
圖4-3-3.1 左營站及小港站不同粒徑總懸浮微粒濃度之累積百分比 4-20
圖4-3-3.2 左營站及小港站不同粒徑總PAHs濃度之累積百分比 4-20
圖4-4-3 各污染源四季之PAHs平均貢獻百分比(A)左營站 (B)小港站 4-33
圖4-5-1.1 左營站不同型態PAHs之氣顆粒相分佈 4-38
圖4-5-1.2 小港站不同型態PAHs之氣顆粒相分佈 4-38


附表目錄
頁碼
附表A-1 夏季左營站及小港站PAHs大氣採樣濃度表 附A-1
附表A-2 秋季左營站及小港站PAHs大氣採樣濃度表 附A-3
附表A-3 冬季左營站及小港站PAHs大氣採樣濃度表 附A-6
附表A-4 春季左營站及小港站PAHs大氣採樣濃度表 附A-10

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