近年來東亞地區經濟及工業快速成長，化石燃料消耗量及人為污染物排放量均大幅增加，導致能源的大量消耗及空氣污染物的大量排放，再加上中南半島區域性生質燃燒所排放的空氣污染物，伴隨著東北季風的影響下，也會將中國大陸華北地區發生的灰霾(以PM2.5為主)吹送至中國大陸華南、琉球、台灣、菲律賓，導致下風處國家或地區的空氣品質不良，再加上跨境長程傳輸(long-range transport)而造成空氣品質劣化，對巴士海峽、台灣海峽及南海交界區域產生一定程度的影響。本研究旨在針對該區域之細懸浮微粒污染來源及交互影響加以探討。
本研究於2016年7月至2017年3月期間，分別於台灣南部（屏東車城）、菲律賓北部（佬沃）、東沙群島（東沙島）等三處設置PM2.5採樣點，同步進行細懸浮微粒（PM2.5）採樣，再進行PM2.5的化學成份分析（包括水溶性離子成份、金屬元素成份、碳成份、脫水醣成份、有機酸成份），藉以瞭解此區域PM2.5的化學特徵。此外，為釐清該區域之污染源種類及貢獻率，本研究亦利用主成份分析法、化學質量平衡受體模式、逆軌跡模擬等方法，進行該區域PM2.5污染源種類及貢獻率之解析。
由PM2.5質量濃度季節變化得知，高濃度PM2.5好發於冬、春季，主要受到源自中國大陸華北、華東地區及中南半島的人為污染物隨污染氣團向下風處傳輸，導致PM2.5濃度明顯上升。夏、秋及春季期間，日間PM2.5濃度高於夜間濃度之情形較為普遍，而冬季較則常發生夜間濃度高於日間情形。
另由化學成份分析結果顯示，各季節水溶性離子成份均以二次無機性氣膠(SO42-、NO3-、NH4+)為主，約佔水溶性離子成份的50.7~71.5%。PM2.5的金屬元素成份以K、Ca、Mg、Fe、Al為主，而人為微量金屬元素(如：Cd、As、Ni及Cr)濃度在風向轉為東北季風時呈現明顯上升趨勢。富集因子分析結果顯示，秋、冬季採樣期間Ti、Cr、Mn、Ni、Cu、Zn等的富集因子（EF）大於10，三處採樣點除受地表逸散揚塵之影響外，亦受到跨境傳輸的人為污染源之影響，且隨PM2.5濃度逐漸升高，金屬元素種類逐漸趨於多元。不同季節PM2.5的碳成份中有機碳(OC)濃度均高於元素碳(EC)，且秋季起二次有機碳(SOC)濃度有明顯升高的趨勢。三處採樣點的甘露糖及半乳糖皆未檢出，左旋葡萄糖濃度趨勢呈現冬、春季大於夏、秋季的現象。透過逆軌跡圖和衛星火點圖發現，冬、春季期間污染氣團主要來自北方及中南半島，受到生質燃燒的影響較為嚴重。車城、佬沃、東沙三處採樣點PM2.5中有機酸濃度季節變化趨勢與PM2.5濃度相似，草酸、 丙二酸及琥珀酸濃度皆於冬、春季期間明顯升高，且在本研究採樣期間三處採樣點的丙二酸/琥珀酸比值（M/S）均大於1，顯示本研究採樣期間有較多的二次有機性氣膠（SOA）的產生。
就污染源種類及貢獻率而言，燃油鍋爐、逸散揚塵、衍生性硫酸鹽、交通運輸、海鹽飛沫為主要的穩定污染源，秋季過後生質燃燒貢獻率呈上升趨勢。屏東車城的境外傳輸比例介於41~80%之間，菲律賓佬沃的境外傳輸比例介於26~75%之間，而東沙群島的境外傳輸比例介於25%~83%之間，自秋季起跨境傳輸之貢獻率呈明顯上升趨勢，顯示受到境外長程傳輸污染物移入之影響甚鉅，此計算所得之境外傳輸貢獻率與本研究團隊在台灣海峽西岸、東岸、及海島地區之境外傳輸貢獻率爲44.9%、57.3%、39.8%相似(Li et al., 2016)。在污染源種類及其貢獻率日夜差異方面，交通運輸、生質燃燒等日間活動污染源及焚化燃燒、燃油鍋爐、鋼鐵廠等工業性污染源的貢獻率大致呈現日間高於夜間之趨勢。

In recent years, the rapid economic and industrial development of East Asia has significantly increased the consumption of fossil fuel and the emissions of anthropogenic sources causing severe environmental problems. Furthermore, biomass burning often occurs in southeastern Asia and southwestern China in spring. The ambient air quality becomes worse possibly due to long-range transport from Chinese haze during the northeastern monsoon periods. The objectives of this study was to collect PM2.5 at intersection of Bashi Channel, Taiwan Strait, and South China Sea, characterize their chemical fingerprint, and identify their potential sources and contributions.
This study collected PM2.5 in four seasons from July 2016 to March 2017 at Che-cheng (Taiwan), Laoag (Philippines), and Dongsha Islands (South China Sea) simultaneously. After sampling, Conditioning, and Weighing, water-soluble ionic species, metallic elements, carbonaceous contents, anhydrosugars, and organic acids of PM2.5 were then analyzed to figure out the chemical fingerprint of PM2.5 sampled at Che-cheng, Laoag, and Dongsha Islands. Furthermore, chemical mass balance (CMB) receptor modelling and backward trajectory simulation were further used to identify the potential sources of PM2.5 and their contributions in different seasons.
Field measurement results showed that high PM2.5 concentrations were observed in winter and spring. During the northeastern monsoons periods, the impacts of Asian dusts, biomass burning, and Northeast Monsoons on ambient air quality commonly occurred, which lead high PM2.5 contributions from long-range transport toward the target area. From the perspective of diurnal variation, we found that showed that PM2.5 concentration in the daytime was generally higher than those at nighttime except in winter at all sites.
Chemical analysis showed that the most abundant water-soluble ionic species of PM2.5 were secondary inorganic aerosols (SO42-, NO3-, and NH4+) which accounted for 50.7~71.5% of total ions. The metallic elements K, Ca, Mg, Fe, and Al dominated the chemical species of PM2.5, while the concentrations of other trace metals (eg: Cd, A, Ni, and Cr) increased during the northeastern monsoon periods. Organic carbon (OC) was the main carbonaceous species in all seasons, and OC/EC ratios and secondary organic carbon (SOC) increased during the northeastern monsoon periods. The levoglucosan concentrations in summer and fall were commonly lower than those in winter and spring, showing that PM2.5 concentrations were highly influenced by biomass burning in winter and spring. In spring, three sampling sites were influenced by long-range transport and biomass burning since the concentrations of levoglucosan in spring were higher than other seasons. Oxalic acid was the most abundant organic acid, and followed by succinic acid and malonic acid. Organic acids of PM2.5 at Laoag were commonly higher than those at Che-cheng and Dongsha Islands. The mass ratio of malonic and succinic acids (M/S ratio) in PM2.5 showed that PM2.5 were mainly attributed by secondary organic aerosols. High M/S ratios in this study showed that PM2.5 was mainly contributed from secondary organic aerosols. Daytime organic acid concentrations were always higher than nighttime organic acid concentration except in winter.
Results obtained from CMB receptor modeling showed that major sources of PM2.5 at three sites were sea salts, fugitive dusts, mobile sources, secondary sulfate, biomass burning, secondary nitrate. The concentration trend of biomass burning increased since fall. Overall, long-range transport accounted for 41~80%, 26~75%, and 25%~83% in Checheng, Laoag, and Dongsha Islands, showing that the three sampling sites was significantly influenced by the long-range transport. It was similar to our past researches that the average long-range transport distributions accounted for 44.9%, 57.3%, and 39.8% at the west-side sites, east-side sites, and offshore site of the Taiwan Strait, respectively (Li et al., 2016).
The trend of mobile sources, biomass burning, industrial process, boilers, incinerator, and steel plants was generally higher in the daytime than those of nighttime. Biomass burning in winter and spring contributed were than in other seasons.

學位論文審定書 i
論文公開授權書 ii
誌謝 iii
中文摘要 iv
英文摘要 vi
目錄 ix
圖目錄 xii
表目錄 xvi
第一章 前言 1
1-1研究緣起 1
1-2研究目的 1
1-3研究範圍與架構 2
第二章 文獻回顧 4
2-1 巴士海峽、台灣海峽及南海交界區域環境概況 4
2-1-1 屏東地區 4
2-1-2 菲律賓佬沃 7
2-1-3 東沙群島 9
2-2 懸浮微粒之物化特性 11
2-2-1 懸浮微粒之分類 12
2-2-2 懸浮微粒之粒徑分佈 14
2-3 懸浮微粒之化學組成 15
2-3-1 懸浮微粒之水溶性離子成份 15
2-3-2 懸浮微粒之金屬元素成份 22
2-3-3 懸浮微粒之碳成份 27
2-3-4 懸浮微粒之脫水醣成份 31
2-3-5 懸浮微粒之有機酸成份 33
2-4 懸浮微粒濃度之日夜變化 35
2-5 污染源解析模式 38
2-5-1逆軌跡模式 38
2-5-2富集因子分析法 39
2-5-3主成份分析法 41
2-5-4化學質量平衡受體模式 43
第三章 研究方法 45
3-1 細懸浮微粒之採樣規劃 45
3-1-1 採樣地點規劃 45
3-1-2 採樣時間規劃 45
3-2細懸浮微粒之採樣方法及濃度量測 48
3-2-1 PQ-200型PM2.5採樣器 48
3-2-2 質量濃度量測方法 49
3-3細懸浮微粒之化學成份分析方法 50
3-3-1 水溶性離子成份分析方法 50
3-3-2 金屬元素成份分析方法 52
3-3-3 碳成份分析方法 53
3-3-4 脫水醣、有機酸成份分析方法 54
3-4 品保與品管 56
3-4-1 採樣方法之品保與品管 56
3-4-2 分析方法之品保與品管 57
3-5 細懸浮微粒之污染源解析方法 59
3-5-1 逆軌跡模式模擬 59
3-5-2 富集因子分析法 59
3-5-3 化學質量平衡受體模式 60
第四章 結果與討論 62
4-1 採樣期間氣象條件分析 62
4-1-1 相對濕度 62
4-1-2 氣溫 63
4-1-3 雨量 63
4-2 細懸浮微粒濃度之變化趨勢分析 64
4-2-1 細懸浮微粒濃度季節變化趨勢 65
4-2-2 細懸浮微粒濃度日夜變化趨勢 66
4-2-3 不同傳輸路徑細懸浮微粒濃度之差異分析 68
4-3 細懸浮微粒化學成份分析 72
4-3-1 水溶性離子成份季節及日夜變化趨勢 72
4-3-2 金屬元素成份季節變及日夜變化趨勢 83
4-3-3 碳成份季節及日夜變化趨勢 92
4-3-4 脫水醣濃度之季節及日夜變化趨勢 96
4-3-5 有機酸濃度之季節及日夜變化趨勢 98
4-3-6 不同傳輸路徑PM2.5化學成份之差異分析 104
4-4細懸浮微粒之污染源解析結果 106
4-4-1 富集因子分析結果 106
4-4-2 主成分分析結果 107
4-4-3 化學質量平衡受體模式解析結果 119
第五章 結論與建議 138
5-1 結論 138
5-2 建議 141
參考文獻 142
附錄A 分析儀器之檢量線 155
附錄B 分析儀器之品保品管 166
附錄C PM2.5分析數據 173

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