臺灣博碩士論文加值系統

大氣季節性變化常影響大氣微粒組成與微粒所含PAHs濃度分佈，台灣位處亞熱帶氣候區，冬季乾燥少雨，夏季高溫多雨的氣候型態，明顯與歐美等溫帶國家有所不同，本研究以冬、夏季微粒濃度差異較大的台灣中南部為探討區域，採用相似流量採樣器 ( PS-1、UAS ) 採集三種不同粒徑範圍微粒 ( PM<2.5、PM2.5-10、TSP ) 與微粒所含十五種3-6環PAHs化合物，解析季節性差異對大氣PAHs粒子特徵的影響性。 研究結果顯示季節影響懸浮微粒質量濃度 ( μg m-3 )，PM<2.5、PM2.5-10、PM>10 的夏/冬微粒質量濃度比值分別為0.65、0.82、0.62，整體而言，顯示夏季受沈降等因子影響，使得夏季懸浮微粒質量濃度較冬季減少約三分之一。 不同粒徑微粒所含Σ PAHs濃度值皆以冬季較高，夏季Σ PAHs濃度僅為冬季的5∼6成，而兩季中則以PM<2.5細粒徑微粒具有最高的Σ PAHs濃度值，其冬、夏季濃度分別為14.34、8.29 ng m-3，顯示PAHs在大氣中的濃度分佈是以< 2.5μm細微粒為主。
大氣PAHs化合物氣/固分佈特徵，隨微粒粒徑大小而有所不同，研究結果發現 > 10 μm 微粒在log Kp vs log PL 圖上的斜率 ( m ) 與截距 ( b ) 明顯與 < 10 μm 微粒有所差異，冬季PM>10 與PM>2.5 的斜率與截距分別為-0.29、-4.11；-0.32、-4.05，此與不同粒徑微粒對PAHs涵容 ( Sorption ) 能力的差別有關。 三種粒徑粒子夏季氣/固分佈迴歸線的斜率 ( m ) 均大於冬季，截距 ( b ) 則較冬季為小，可能與夏季高濕度環境使微粒表面形成水膜，提升微粒吸附能力有關。
本研究以多點採樣迴歸分析 ( Pankow, 1992 )，求得各粒徑微粒在冬、夏季節的理論共同交點 ( Common Interception Point )，兩季的共同交點值以 < 10 μm微粒的差異較大，其中又以PM<2.5細微粒較明顯，PM<2.5粒子PAHs冬、夏季共同交點值 ( logPL, logKp ) 分別為 ( -5.69, -2.16 ) 與 ( -2.23, -3.01 )，顯示季節性差異對PAHs氣/固分佈特徵的影響以細微粒為主。 本研究與國內相關研究 ( 陳瑞仁, 1998 ) 實測所得PAHs固相分率 (ψ) 分佈趨勢相似，但ψ值大小並不相同，應是與地區污染源排放特性有關。 若將野外採樣實測ψ值與Jungle-Pankow理論模式相較，本研究大環PAHsψ值有低估的現象，小環PAHs則有高估趨勢，這可能是受到採樣流量差異與採樣非置換因子 ( X ) 的影響所致；研究數據顯示固相分率 (ψ) 與採樣非置換因子 ( X ) 間具有相關性，TSP微粒中r2分別為0.96、0.99，即除採樣流量外，採樣非置換因子也是造成固相分率 (ψ) 實測值與大氣理想ψ值差異的主要因子之一。 PAHs的固相分率 (ψ) 隨化合物的分子量而增加，顯示大環PAHs較易與微粒相結合，而由於受到採樣流量、吸附介質、地區粒子特性的影響，使得各地PAHs的ψ值不盡相同。

Seasonal variation affected both the particle size composition and the adsorption of particles on polycyclic aromatic hydrocarbons (PAHs) in atmospheres. The study was chosen summer and winter seasons in the southern part of Taiwan to represent substantial variation of particle concentration in regions. Several samplers with similar flow rate were simultaneously conducted to collect the mass concentration of various particles, and also to measure the gas and particle concentrations on fifteen PAHs at traffic circumstance in urban areas. We tried to investigate the seasonal differences of concentration and composition ratios in particle size distributions、gas / particle phase partitioning and particulate fraction (ψ) on semi-volatile PAHs components.
Results were shown that mass concentration of particles was almost 50% more in winter season. But, the composition ratios from different size particles (included PM<2.5, PM2.5-10, and PM>10) were similar in both seasons. From the view of PAHs concentrations ( ng m-3 ), the summer / winter ratios of PAHs among PM<2.5, PM2.5-10, and PM>10 were 0.65, 0.82, 0.62. The PM<2.5 particle has the highest value of PAHs concentrations in winter and summer seasons.
Those experimental data were verified by the correlation of the volatility with gas/particle partitioning coefficient (Kp) on 3-4 rings of PAHs components. Applying the sub-cooled vapor pressure (PL) of PAHs rather than solid vapor pressure (Ps) would contribute a good correlation (r2=0.97) to prove the evidence of adsorptive characteristics in atmospheric particles. The non-exchangeable factors (X, %) in various particles have shown a promising correlation with PL parameter. Because of low humidity causing the less water competition at adsorptive site in particles, data from winter season offered a good correlation between the non-exchangeable factors and PL vapor pressure of PAHs. The Jungle-Pankow model gives particulate fraction (ψ) for 3-ring PAHs (AcPy、AcP) which was underestimated. Filtration air samplers are subject to “blow-off” artifacts, which result in loss of semivolatile compounds from filtered particles. The gas/particle distribution of PAH is underpredicted, this may be related to the presence of sampling non-exchangeable PAHs or due to the long times required for aerosol-air reequilibration.

一、緒論--------------------------------1-1
二、文獻回顧----------------------------2-1
2.1PAHs化合物特性----------------------2-1
2.2大氣中PAHs來源與濃度特徵------------2-5
2.3PAHs粒徑分佈特性 -------------------2-8
2.4PAHs氣/固相分佈模式-----------------2-8
2.5PAHs採樣數據之迴歸分析--------------2-18
2.6大氣半揮發性物質的固相分率----------2-22
三、實驗設備及方法----------------------3-1
3.1採樣條件-------------------------3-1
3.2採樣裝置----------------------------3-2
3.3樣品分析---------------------------3-3
四、結果與討論------------------------4-1
4.1大氣PAHs化合物在不同季節中的濃度分佈特性-4-1
4.2不同粒徑微粒的氣/固分佈特徵的季節性差異--4-3
4.3不同季節中PAHs理論共同交點迴歸分析-------4-6
4.4大氣中PAHs固相分率 （ψ）實測值與Jungle-
Pankow 理論模式的比較--------------------4-8
五、結論--------------------------------5-1
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