臺灣博碩士論文加值系統

奈米微粒，亦可稱之為超細微粒(Ultrafine Particles, UP < 100 nm)在相同質量下比大微粒具有更大的表面積，誘發之氧化壓力效應相對較大，有研究指出空氣中的半揮發有機物(Semi-Volatile Organic Compounds, SVOCs)易吸附於奈米微粒上，而SVOCs中的多環芳香碳氫化合物(Polycyclic Aromatic Hydrocarbons, PAHs)因具有突變性與致癌性，特別受到學者重視；人體受PAHs之危害決定於PAHs之氣相/粒狀物相分佈及粒狀物相PAHs之粒徑分佈，因此有必要瞭解PAHs之氣相/粒狀物相分佈與不同粒徑大小微粒之PAHs含量。
本研究開發一套可降低量測誤差之空氣奈米微粒中PAHs濃度之系統AD-MOUDI-PUF，此系統利用環形擴散採樣管(Annual denuder, AD)填充XAD-4吸附劑，裝設於微孔均勻沈積衝擊器(Micro-Orifice Uniform Deposit Impactor, MOUDI)前端，先吸附氣相PAHs，排除氣相PAHs對後端微孔均勻沈積衝擊器所採集微粒之採樣誤差，並於最後端裝設聚氨基甲酸酯泡棉(polyurethane foam, PUF)檢視微粒上PAHs之揮發採樣誤差。研究結果顯示，使用8個通道，長度為60 cm的環形擴散採樣管，以流量30 L/min可有效吸附(移除)氣相PAHs，而AD-MOUDI-PUF系統使用鐵氟龍濾紙與石英濾紙檢測之PM0.1 PAHs濃度分別為1.87 ± 0.03 ng/m3與2.01 ± 0.08 ng/m3；若使用環形擴散採樣管移除氣相PAHs時，會使得MOUDI的PM0.1濾紙上15種PAHs濃度採樣結果較為正確，但若未經環形擴散採樣管移除氣相PAHs時會使得氣相PAHs進入濾紙後端的PUF，造成採樣之負向偏差。將AD-MOUDI-PUF系統與傳統式MOUDI-PUF系統進行比較，傳統式MOUDI-PUF使用石英濾紙採集PAHs約有50% 的正向偏差，顯示過去學者研究明顯高估粒狀物相PAHs濃度。

Several studies have concluded that nano particulates or ultra-fine particulates (< 0.1 μm in diameter, UPs) disproportionately induce oxidative stress in cells and are more toxic than larger particles of similar composition. It is also found that semi-volatile organic compounds (SVOCs) tend to adsorb on UPs. Among the SVOCs, polycyclic aromatic hydrocarbons (PAHs) are of particular concern because several PAHs are potent mutagens and carcinogens. It is important to measure the real concentrations of atmospheric ultra-fine PAHs for the assessment of their health effects.
A PAH sampling system which composed of annual denuder (AD), micro-orifice uniform deposit impactor (MOUDI) and polyurethane foam (PUF) in series is developed in this study. The collection efficiency of gaseous PAHs, positive and negative artifacts and particle loss for the AD and the sampling performance of the AD-MOUDI-PUF were evaluated. The annular denuder is 60 cm in length with 8 annuli. The results show that the annular denuder coated with ground XAD-4 at the flow rate of 30 L/min can trap the gaseous PAHs effectively. The average PAH concentrations of PM0.1 were 1.87 ± 0.03 and 2.01 ± 0.08 ng/m3 for AD-MOUDI-PUF sampler using Teflon filter and quartz filter. AD can remove PAHs effectively. A large amount of gaseous PAHs will absorb by the PUF and further lead to the positive artifacts without the AD. For example, 50% positive artifacts will be caused while quartz fiber filter was used.

總目錄
摘要 I
Abstract III
誌謝 IV
總目錄 IV
表目錄 IX
圖目錄 X
第一章 前言 1
1-1 研究動機 1
1-2 研究目標 2
第二章 文獻回顧 3
2-1 大氣奈米微粒特徵 3
2-1-1 懸浮微粒之定義 3
2-1-2 大氣微粒生成機制 3
2-1-3 奈米微粒特性 6
2-1-4 懸浮微粒粒徑分佈 10
2-1-5 奈米微粒採樣技術 12
2-1-6 奈米微粒之毒性效應 13
2-1-7 環境奈米微粒研究 15
2-1-7-1 典型都會區排放 15
2-1-7-2 交通源排放 16
2-2 多環芳香碳氫化合物(Polycyclic aromatic hydrocarbons,PAHs)17
2-2-1 PAHs生成機制 17
2-2-2 PAHs排放來源特徵 19
2-2-3 PAHs理化特性 21
2-2-4 PAHs之毒性效應 22
2-2-5 大氣環境PAHs之研究 29
2-3 PAHs採樣技術 31
2-3-1 傳統PAHs採樣器及採樣誤差 31
2-3-2 環形擴散採樣器 32
2-3-3 環形擴散採樣管構造與原理 33
2-3-3-1 環形擴散採樣管對氣相PAHs之收集效率 33
2-3-3-2 環形擴散採樣管微粒損失 35
2-3-3-3 環形擴散採樣管應用於大氣PAHs量測相關研究 36
第三章 實驗設備與方法 38
3-1 實驗設計 38
3-2 實驗設備與採樣方法 39
3-2-1 環形擴散採樣管 39
3-2-1-1 Amberlite XAD Resin吸附劑 39
3-2-1-2 塗敷溶液 41
3-2-1-3 環形擴散採樣管採樣前處理流程 41
3-2-2 微孔均勻沈積衝擊器 43
3-2-2-1 濾紙調理 45
3-2-2-2 微粒稱重 45
3-2-2-3 流量校正 46
3-3 採樣規劃 46
3-4 PAHs分析設備與方法 47
3-5 環形擴散採樣管微粒損失 51
第四章 結果與討論 53
4-1 大氣微粒濃度與粒徑分佈 53
4-2 環形擴散採樣管對氣相PAHs之收集效率 56
4-3 大氣PAHs濃度 59
4-3-1 大氣氣相PAHs濃度 59
4-3-2 大氣粒狀物相PAHs濃度與粒徑分佈 60
4-3-3 MOUDI-PUF採樣系統PAHs環數分佈之情形 63
4-3-4 AD-MOUDI-PUF採樣系統PAHs環數分佈之情形 65
4-4 奈米微粒PAHs之採樣偏差 67
4-4-1 正向偏差 67
4-4-2 負向偏差 69
4-5 環形擴散採樣管微粒損失 71
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 PAHs分析之品質保證與品質控制 90


表目錄
表2-1奈米微粒來源 ........................................................................................................ 7
表2-1奈米微粒來源 (續) ................................................................................................ 8
表2-1奈米微粒來源 (續) ................................................................................................ 9
表2-2各式多階衝擊器及其截取直徑 ...................................................................... 13
表2-3 16種PAHs之分子量、結構式及物理特性 .............................................. 24
表2-4 16種PAHs之蒸氣壓於25度C水中之溶解度與親電性反應 ............... 25
表2-5 PAHs毒性當量係數 (Toxicology Equivalent Factor, TEF) .................... 26
表2-6 16種PAHs之致癌性 ........................................................................................ 28
表2-7環形擴散採樣管常用之吸收劑及其可吸收之氣體 ................................ 32
表3-1 XAD種類及其物理特性 .................................................................................. 40
表3-2 MOUDI各階段之截取粒徑 ............................................................................ 44
表4-1大氣各粒徑微粒質量濃度 ............................................................................... 54
表4-2大氣各粒徑粒狀物相PAHs質量濃度 ......................................................... 61
表4-3 PAHs於各採樣串連組件所佔比例 .............................................................. 70
表4-4環形擴散採樣管各種粒徑之微粒數與損失百分比 ................................ 73


圖目錄
圖2-1各粒徑微粒之定義 ............................................................................................... 4
圖2-2各粒徑微粒之基本特性 ...................................................................................... 5
圖2-3大氣微粒之形成機制、來源及去除機制 ..................................................... 5
圖2-4環境中奈米微粒來源 .......................................................................................... 6
圖2-5典型大氣懸浮微粒之粒徑分佈圖 ................................................................. 11
圖2-6典型大氣與交通相關微粒之粒徑分佈圖 ................................................... 11
圖2-7微粒進入人體呼吸系統沉積位置及機制示意圖 ..................................... 14
圖2-8自由基生成PAHs之反應機制 ....................................................................... 18
圖2-9 Bap代謝活化及DNA鍵結之過程............................................................... 27
圖2-10 PAHs傳統採樣之誤差 ................................................................................... 31
圖2-11擴散採樣管採樣原理剖面圖 ........................................................................ 33
圖2-12 Denuder-MOUDI與MOUDI兩種系統15種PAHs濃度之差異 .... 36
圖3-1奈米微粒PAHs採樣系統配置圖 .................................................................. 38
圖3-2擴散管內磨砂玻璃管壁 .................................................................................... 41
圖3-3樹脂塗敷於磨砂玻璃管壁內 .......................................................................... 41
圖3-4微孔均勻沈積衝擊器 ........................................................................................ 44
圖3-5階段式衝擊器 ...................................................................................................... 44
圖3-6 MOUDI採樣器流量校正圖 ............................................................................ 47
圖3-7 PAHs分析流程圖 ............................................................................................... 50
圖3-8環形擴散採樣管微粒損失實驗系統圖 ........................................................ 52
圖4-1大氣微粒各粒徑範圍與PM10之比值 .......................................................... 55
圖4-2各種氣相PAHs以環形擴散採樣管採樣之實測吸附率 ........................ 58
圖4-3環形擴散採樣管於大氣採集之PAHs濃度 ............................................... 60
圖4-4大氣PAHs各粒徑範圍與PM10之比值 ...................................................... 62
圖4-5 MOUDI-PUF (Teflon) 系統各粒徑上低、中、高分子量PAHs之平均質量濃度 ............................................................................................................................. 64
圖4-6 MOUDI-PUF (Quartz) 系統各粒徑上低、中、高分子量PAHs之平均質量濃度 ............................................................................................................................. 64
圖4-7 AD-MOUDI-PUF (Teflon) 系統各粒徑上低、中、高分子量PAHs之平均質量濃度.................................................................................................................... 66
圖4-8 AD-MOUDI-PUF (Quartz) 系統各粒徑上低、中、高分子量PAHs之平均質量濃度.................................................................................................................... 66
圖4-9 MOUDI-PUF與AD-MOUDI-PUF使用鐵氟龍濾紙採集大氣15種PAHs PM0.1平均濃度 ...................................................................................................... 67
圖4-10 MOUDI-PUF、AD-MOUDI-PUF (Teflon、Quartz) 系統大氣PAHs PM0.1實測濃度 .................................................................................................................. 68
圖4-11 MOUDI-PUF與AD-MOUDI-PUF使用石英濾紙採集大氣15種
PAHs PM0.1平均濃度 ...................................................................................................... 69
圖4-12環形擴散採樣管各種粒徑之微粒數與損失變化圖 .............................. 71

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