隨著東亞地區各國的工、商業崛起，化石燃料使用量及人為污染物排放均呈現大幅增加，此舉導致能源劇烈消耗與產生大量污染物，導致東亞各國空氣品質均受到影響。台灣海峽(Taiwan Strait)及南海(South China Sea)位處台灣、中國大陸、菲律賓及中南半島之間，因冬、春兩季盛行東北季風而挾帶空氣污染物(如:灰霾)及亞洲沙塵(Asian dusts)的影響，再加上東南亞地區於春耕時期使用火耕(slash-and-burn)所造成之生質燃燒日趨嚴重，使得人為及自然污染物藉由長程傳輸跨越台灣海峽及南海，進而使得下風處國家或地區的空氣品質劣化，也會對於此兩海域的空氣品質造成一定程度的影響。
有鑑於此，本研究旨在探討東亞地區細懸浮微粒時空分佈、化學指紋特徵、污染來源及交互影響。本研究於2017年8月至2018年4月期間，分別於澎湖群島、東沙群島及南沙群島，同步執行PM2.5採樣，並進行化學成份(水溶性離子成份、金屬元素成份、碳成份、脫水醣成份及有機酸成份)分析，藉以瞭解東亞地區PM2.5的化學指紋特徵。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。
本研究結果顯示，高濃度PM2.5好發於冬、春季，主要受到源自於北方地區的人為污染物隨氣團南下傳輸所致，導致PM2.5濃度明顯上升，在日夜變化方面，四季採樣期間多半屬於日間高於夜間之情形。由化學成份分析結果顯示，PM2.5的水溶性離子成份以二次無機性氣膠(NO3-、SO42-、NH4+)為主，約佔水溶性離子成份(SIAs/WSI)的42.4~79.9%，且以冬、春季較為明顯，多半呈現日間高於夜間之趨勢。金屬元素成份皆以Ca、K、Mg、Fe、Al等地殼元素為主，而自秋季起微量金屬元素(如：V、Cr、Mn、Ni、Cu、Zn、As、Cd)濃度逐漸升高，富集因子結果顯示，秋、冬、春季採樣期間Ti、Cr、Mn、Ni、Cu、Zn等的EF值大於10，顯示三處採樣點除受土壤逸散揚塵貢獻外，亦受到跨境傳輸人為污染物之影響。碳成份方面，四季採樣期間有機碳(OC)濃度均高於元素碳(EC)，且於秋季起，二次有機碳濃度有明顯上升的趨勢。就脫水醣分析而言，三處採樣點除左旋葡萄糖外，半乳醣及甘露醣皆未檢出，左旋葡萄糖濃度於冬、春季濃度明顯高於夏、秋季，經由逆軌跡圖及四季火點圖發現，冬、春季期間污染氣團主要來自於中國大陸華北、華中地區等生質燃燒發生較為頻繁區域，而夏季採樣期間南沙群島受到印尼地區森林火災影響較澎湖群島及東沙群島嚴重，導致左旋葡萄糖濃度高於另外兩處採樣點。三處採樣點之有機酸濃度與PM2.5濃度呈現相同的變化趨勢，草酸、丙二酸及琥珀酸濃度皆於冬、春兩季採樣期間有明顯升高趨勢，採樣期間三處採樣點的丙二酸與琥珀酸比值(M/S)均大於1.0，其M/S比值依序為南沙群島>東沙群島>澎湖群島，顯示在採樣期間，有機酸主要來自二次有機氣膠的生成。
就污染源種類及其貢獻率而言，主要以海鹽飛沫、逸散揚塵、燃油鍋爐、交通運輸及衍生性硫酸鹽為主，夏季於南方帶來較為潔淨的氣團，故此時PM2.5濃度相對較低，污染源種類及其貢獻率與背景日較為相似。自秋季起，污染源種類逐漸增加且貢獻率亦逐漸上升，增加的污染源種類以人為污染源居多，包括石化業、鋼鐵業及生質燃燒等。整體而言，澎湖群島四季境外傳輸比例介於14~56%之間，東沙群島四季境外傳輸比例介於29~72%之間，而南沙群島四季境外傳輸比例介於18~60%之間。在污染源種類及其貢獻率的日夜差異方面，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、石化業、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。

Over the past decades, the industries and commerce rose up fastly in East Asian countries. The increase of fuel consumption and pollution emission lead to poor air quality in the region. Taiwan Strait and South China Sea are surrounded by Taiwan, China, Philippine, and Indochina Peninsula. The northeastern monsoons in winter and spring bring air pollutants (such as haze) and Asian dust to downwind region coupled with the growth of slash-and-burn in the spring in the Southeast Asia, which cause the deteroiation of ambient air across the Taiwan Strait and South China Sea via long-range transport.
Accordingly, this study aims to explore the spatiotemporal variation, chemical characteristics, and source apportionment of PM2.5 in East Asia. PM2.5 samples were collected simultaneously at the Penghu Islands, the Dongsha Islands, the Nansha Islands from August 2017 to April 2018. After sampling, PM2.5 filters were carried back to the laboratory for further conditioning, weighing, and chemical analysis. Water-soluble ions, metallic elements, carbonaceous contents, anhydrosugars, and organic acids were then analyzed to charactaize the chemical fingerprint of PM2.5 in East Asia. Furthermore, backward trajectory simulation and chemical mass balance (CMB) receptor modelling were applied to identify the potential sources of PM2.5 and their contribution in each season.Field sampling results indicated that high concentrations of PM2.5 were observed mainly in winter and spring. During the northeastern monsoons periods, anthropogenic pollutants from northern region were brought to the target area, resulting in significant increase of PM2.5 concentration. From the perspective of diurnal variation, the concentration of daytime PM2.5 was generally higher than those at nighttime at all sites in all seasons.
Chemical analytical results showed that secondary inorganic aerosols (NO3-, SO42-, and NH4+) dominated water-soluble ions, accounting for 42.4-79.9% of water-soluble ions particularly in winter and spring. Daytime PM2.5 concentration was commonly higher than that at nighttime. Crustal elements (Ca, K, Mg, Fe, Al) dominated the metallic elements in PM2.5. The concentration of hazardous metals (V, Cr, Mn, Ni, Zn, and Cd) came mainly from anthropogenic sources since fall. Moreover, organic carbon (OC) was the dominant carbonaceous species during the sampling periods, and OC/EC ratio increased during the northeastern monsoon periods. The concentrations of levoglucosan at the sampling sites were ordered as PH>DS>NS. The highest levoglucosan concentrations of 23.54 ng/m3 were observed at the Penghu Islands. Organic acids of PM2.5 at the Penghu Islands were commonly higher than those at the Dongsha Islands and the Nansha Islands. Oxalic acid was the abundant organic acids in PM2.5. The concentrations of oxalic acid at all sampling sites ranged from 5.1 to 246.2 ng/m3. The mass ratios of malonic and succinic acids (M/S ratio) in PM2.5 ranged from 0.95 to 1.41, showing that PM2.5 was mainly attributed from secondary organic aerosols (SOAs). Daytime organic acid concentrations were always higher than those at nighttime.
Results obtained from CMB receptor modeling showed that the major sources of PM2.5 at the three sampling sites were sea salts, fugitive dusts, mobile sources, secondary sulfate, and secondary nitrate. Since fall, the contribution of anthropogenic sources (incinerators, petrochemical plants, industrial boilers, secondary sulfate, secondary nnitrate) and biomass burning increased gradually. Overall, the contribution of long-range transport at the Penghu Islands, the Dongsha Islands, and the Nansha Islands accounted for 14~56%, 29~72%, and 18~60%, respectively. The contribution of anthropogenic sources (mobile sources, industrial process, industrial boilers, incinerators, and steel plants) and biomass burning in the daytime was generally higher than those at nighttime. The contribution of biomass burning to PM2.5 in winter and spring were generally higher than those in other seasons.

學位論文審定書 i
論文公開授權書 ii
誌謝 iii
摘要 iv
Abstract vi
目錄 ix
表目錄 xii
圖目錄 xiv
第一章 前言 1
1-1研究緣起 1
1-2研究目的 2
1-3研究範圍與架構 2
第二章 文獻回顧 5
2-1 台灣海峽與南海區域環境概況 5
2-1-1 澎湖群島 5
2-1-2 東沙群島 7
2-1-2 南沙群島 9
2-2 懸浮微粒的特性 10
2-2-1 懸浮微粒的形成機制及粒徑分佈 12
2-3 懸浮微粒的化學特性 15
2-3-1 懸浮微粒的水溶性離子成份 15
2-3-2 懸浮微粒的金屬元素成份 20
2-3-3 懸浮微粒的碳成份 24
2-3-4 懸浮微粒的脫水醣成份 29
2-3-5 懸浮微粒的有機酸成份 34
2-3-6 懸浮微粒濃度季節及日夜變化趨勢 38
2-3-7 臨海地區相關研究 42
2-4 污染源解析模式之應用 44
2-4-1 富集因子 44
2-4-2 化學質量平衡受體模式 47
2-4-4 逆軌跡模式 49
第三章 研究方法 51
3-1 細懸浮微粒之採樣規劃 51
3-1-1 採樣地點規劃 51
3-1-2 採樣時間規劃 51
3-2 細懸浮微粒之採樣方法及濃度量測 54
3-2-1 PQ-200型PM2.5採樣器 54
3-2-2質量濃度量測方法 55
3-3 細懸浮微粒之化學成份分析方法 56
3-3-1 水溶性離子成份分析方法 56
3-3-2 金屬元素成份分析方法 58
3-3-3 碳成份分析方法 59
3-3-4 脫水醣、有機酸成份分析方法 61
3-4 品保與品管 63
3-4-1 採樣方法之品保與品管 63
3-4-2 分析方法之品保與品管 64
3-5 細懸浮微粒之污染源解析方法 65
3-5-1 富集因子分析法 65
3-5-2 逆軌跡模式模擬 66
3-5-3 化學質量平衡受體模式 67
第四章 結果與討論 69
4-1台灣海峽與南海區域氣象條件分析 69
4-1-1相對溼度 69
4-1-2大氣溫度(氣溫) 70
4-1-3降雨量 71
4-2細懸浮微粒濃度時空變化趨勢分析 72
4-2-1細懸浮微粒濃度季節變化趨勢 72
4-2-2 細懸浮微粒濃度日夜變化趨勢 74
4-2-3不同傳輸路徑細懸浮微粒濃度之聚類分析 76
4-3 細懸浮微粒化學成份分析 80
4-3-1 水溶性離子成份季節及日夜變化趨勢分析 80
4-3-2 金屬元素成份季節及日夜變化趨勢分析 94
4-3-3 碳成份季節變化及日夜趨勢分析 107
4-3-4 脫水醣成份季節及日夜變化趨勢分析 112
4-3-5 有機酸成份季節及日夜變化趨勢分析 119
4-3-6 不同傳輸路徑化學成份之聚類分析 123
4-4 細懸浮微粒污染源解析 125
4-4-1 富集因子解析結果 125
4-4-2 化學質量平衡受體模式解析結果 131
第五章 結論與建議 146
5-1結論 146
5-2建議 149
參考文獻 150
附錄A分析儀器之檢量線 163
附錄B分析儀器之品保品管 174
附錄C PM2.5濃度及化學成份之原始數據 181

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