台灣海峽兩岸空氣品質的惡化(如：中國大陸灰霾、亞洲沙塵暴及中南半島生質燃燒)，與工業污染排放、自然揚沙及農廢燃燒具有高度的相關性。在特定氣象條件下，從上述污染源所排放的空氣污染物被吹向下風處的國家或地區，造成空氣品質劣化。過去文獻指出，東北季風會將中國華北地區發生的灰霾吹向華中、華南地區及台灣，甚至遠至南海北部的東沙群島。因此，位於下風處的台灣海峽南部及南海北部交界區域，是我國研究境外傳輸現象重要的空氣品質監測區域。
本研究於2015年夏季至2016年春季期間，於台灣海峽南部及南海北部交界區域，設置二處PM2.5採樣站，分別架設於澎湖群島(PH)及東沙群島(DS)，PM2.5的採樣均為同步採樣，每個季節採樣時間為連續14天，每天進行24小時的連續採樣。細懸浮微粒採樣器為BGI-PQ200型之PM2.5採樣器，樣品採集後經由密閉封存後，攜回實驗室進行物化特徵分析，包括質量濃度、水溶性離子成份、金屬元素成份、碳成份及脫水醣成份，並以主成份分析法(PCA)及化學質量平衡受體模式(CMB)，針對污染源種類及貢獻率加以解析及探討。
本研究採樣結果顯示，台灣海峽南部及南海北部交界區域PM2.5濃度空間分佈大致呈現北高南低的趨勢，夏季採樣期間澎湖群島及東沙群島PM2.5濃度均為四個季節中最低，自秋季起PM2.5濃度逐漸上升，推測主要受到東北季風影響，北方的人為污染物南下經由台灣海峽而到達澎湖群島，甚至影響到東沙群島。夏季期間來自南方的海上氣團明顯較秋、冬、春季來自的北方的氣團更為乾淨。
由化學指紋特徵結果顯示，PM2.5的水溶性離子成份除Cl-及Na+海鹽成份外，以SO42-、NO3-及NH4+所組成的二次無機性氣膠(SIAs)為主要物種，約佔水溶性離子成份的50~70%之間。金屬元素成份以Mg、K、Ca、Fe、Al為主要物種，自秋季起來自工業污染源的人為金屬元素(如：V、Cr、Mn、Ni、As、Cd、Pb)有顯著的上升趨勢。碳成份中於不同季節均以有機碳(OC)為主要物種，OC/EC比值自東北季風盛行期間起亦呈現上升趨勢。脫水醣濃度趨勢呈現冬、春季大於夏、秋季的現象，顯示冬、春季節受到生質燃燒的影響較為嚴重。
由成對T檢定相關性結果顯示，澎湖群島及東沙群島全年PM2.5濃度及化學成份p value分別為0.001及0.004，顯示採樣期間整年度有良好的相關性，而採樣期間各季節的PM2.5濃度及化學成份相關性結果，除春季採樣期間不具相關性外，夏、秋及冬季的PM2.5濃度及化學成份均有高度的相關性，原因為春季採樣期間兩站污染傳輸路徑較不相似。而兩站不同傳輸路徑PM2.5濃度相關性為南方傳輸型>北方傳輸型，化學成份相關性為北方傳輸型>南方傳輸型，且南方傳輸型不具相關性，顯示兩站南方傳輸型的路徑較不一致。
由污染源種類及貢獻率解析結果顯示，澎湖群島及東沙群島均以海鹽飛沫、逸散揚塵、燃油鍋爐、交通運輸及二次衍生性氣膠為主要污染源。自秋季起，污染源種類逐漸增多及貢獻量亦逐漸上升，且以人為污染源較多，包括石化業、鋼鐵業及生質燃燒等，其中秋季工業型污染源(如：焚化燃燒、石化業、鋼鐵業及水泥業)較夏季工業型污染源多了一倍。而冬、春季採樣期間，澎湖群島及東沙群島受生質燃燒污染的影響，則有不同的季節趨勢，澎湖群島為春季>冬季，東沙群島則為冬季>春季，推測兩處的生質燃燒來源不盡相同。整體而言，澎湖群島四季境外傳輸比例介於28.4~61.0%之間，而東沙群島四季境外傳輸比例介於36.4%~76.8%之間，顯示兩處均明顯受到境外傳輸污染的影響，其中東沙群島的境外傳輸污染比澎湖群島更高。

The deterioration of ambient air quality across the Taiwan strait, including Chinese haze, Asian duststorms and Indochina biomass burning, is highly correlated with industrial emissions, natural soil weathering and swidden agriculture. Under certain meteorological conditions, air pollutants could be blown to the downwind countries/regions and cause poor ambient air quality. Previous literature reported that the northern prevailing winds commonly blow the haze originated from northern China to central and southern China, Taiwan, and even Dongsha Islands. Therefore, the intersectional region of Taiwan Strait and South China Sea is an important air quality monitoring site for long-range transportation.
This study selected two PM2.5 sampling sites (i.e. Penghu Islands and Dongsha Islands) located at the intersectional region of Taiwan Strait and South China Sea. Twenty-four hour sampling of PM2.5 was simultaneously collected at Penghu Islands and Dongsha Islands for continuous 14 days in four seasons from summer 2015 to spring 2016. PM2.5 samples were simultaneously collected with BGI-PQ200. After sampling, PM2.5 samples were carried back to the laboratory for conditioning, weighing, and chemical analysis. The chemical composition of PM2.5 including water-soluble ionic species, metallic elements, carbonaceous contents, and anhydrosugar. Moreover, the potential sources of PM2.5 and their contribution were further identified by principal component analysis (PCA) and chemical mass balance (CMB) receptor model.
Field sampling results indicated that the spatial distribution of PM2.5 concentration increased from south to north. The lowest seasonal averaged PM2.5 concentrations were observed in summer at both Penghu Islands and Dongsha Islands. PM2.5 concentrations increased gradually since fall, which might be influenced by the northeastern monsoons since air masses could be transported from the north toward Penghu Islands and Dongsha Islands. Air masses blown from South China Sea in summer were much cleaner than those blown from the north in fall, winter, and spring.
Chemical analysis results showed that the most abundant water-soluble ionic species of PM2.5 were secondary inorganic aerosols (SIAs) including SO42-, NO3-, and NH4+ which accounted for 50~70% of water-soluble ions (WSIs). The most abundant metallic elements of PM2.5 were crustal elements (Mg, K, Ca, Fe, and Al), while anthropogenic elements (V, Cr, Mn, Ni, As, Cd, and Pb) concentration increased since fall. Organic carbon (OC) was the main species in all seasons, and OC/EC ratios 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.
Correlation analysis results obtained from paired t test showed that the p values of PM2.5 concentration and chemical composition were 0.001 and 0.004, respectively, between two subtropic islands, showing that they had high correlation. In addition to spring, both PM2.5 concentration and chemical composition had high correlation in summer, fall, and winter, because the transportation routes toward these two Islands were not similar in spring. The correlation of PM2.5 concentration for different routes showed that the southern routes were generally lower than the northern routes. Oppositely, the correlation of chemical composition for different routes showed that the northern routes were higher than the southern routes and the southern routes was not correlated, showing that the transportation routes were different toward the two Islands for the southern routes.
Results from PCA and CMB receptor modeling showed that major sources of PM2.5 concentrations were at Penghu Islands and Dongsha Islands were sea salts, soil dusts, fuel burning, mobile sources, and secondary aerosols. Since fall, both pollutant sources and their contributions increased, especially for anthropogenic sources including petrochemical plants, steel plants, biomass burning and etc. The contributions of industrial sources (e.g. incinerators, petrochemical, steel, and cement industries) increased almost twice from summer to fall. In winter and spring, biomass burning caused different seasonal trends between Penghu Islands and Dongsha Islands. Levoglucosan concentrations in spring were higher than those in winter at Penghu Islands, while levoglucosan concentrations in winter were higher than those in spring at Dongsha islands, showing that the sources of biomass burning might be different at Penghu Islands and Dongsha Islands. Overall, cross-boundary transport accounted for 28.4~61.0% at Penghu Islands and 36.4~76.8% at Dongsha Islands, respectively, showing that both islands were highly influenced by the cross-boundary transport, especially at Dongsha Islands.

目 錄
學位論文審定書…………………………………………………………………i
誌謝………………………………………………………………………………ii
中文摘要…………………………………………………………………………iii
英文摘要…………………………………………………………………………v
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………………………………………………………………... 1
1-3 研究範圍與架構………………………………………………………... 2
第二章 文獻回顧…..…………………………………………………………… 4
2-1台灣海峽南部與南海交界區域環境概況……………………………… 4
2-1-1 澎湖群島………………………………………….……………….. 4
2-1-2 東沙群島…………………………………………………………... 8
2-2 懸浮微粒特性…………………………………………………………... 10
2-2-1 懸浮微粒形成機制………………………………………………... 13
2-2-2 懸浮微粒濃度之季節變化趨勢……………….………………….. 14
2-3 懸浮微粒化學特性…………………………………..…………………. 16
2-3-1 水溶性離子成份…………………………...…………...…………. 16
2-3-2 金屬元素成份……………………………………………………... 18
2-3-3 碳成份…………………………………………………..…………. 20
2-3-4 脫水醣成份………………………………………………………... 22
2-4 鄰海地區懸浮微粒相關研究………………………………...………… 24
2-5 污染源解析模式之應用………………………………………………... 26
2-5-1 富集因子…………………………………...…………...…………. 26
2-5-2 主成份分析………………………………………………………... 27
2-5-3 化學質量平衡受體模式………………………………..…………. 28
2-5-4 逆軌跡模式………………………………………………………... 29
第三章 研究方法…………………………………………………………..…… 31
3-1 採樣規劃……………………...………………………………………… 31
3-1-1 採樣地點規劃…………………………………….……………….. 31
3-1-2 採樣時間規劃…………………………………….……………….. 32
3-2 細懸浮微粒採樣方法與原理…………………………………………... 33
3-2-1細懸浮微粒採樣器……………………...…………………………. 33
3-2-2 細懸浮微粒採樣方法及步驟……………………………………... 34
3-3 細懸浮微粒質量濃度量測及化學成份分析方法……………………... 35
3-3-1 質量濃度量測方法………………………………………………..... 35
3-3-2 水溶性離子成份分析方法………………………………………... 36
3-3-3 金屬元素成份分析方法…………………………………………... 37
3-3-4 碳成份分析方法…………………………………………………... 39
3-3-5 脫水醣成份分析方法……………………………………………... 40
3-4 品保與品管……………………………………………………………... 42
3-4-1 採樣方法之品保與品管……………………………………….…... 42
3-4-2 分析方法之品保與品管……………………………………….…... 43
3-5 大氣懸浮微粒之污染源解析….……………………………………….. 44
3-5-1 富集因子分析法..…………………………………………………. 44
3-5-2 主成份分析法………..………………………………………….…. 45
3-5-3 化學質量平衡受體模式………………………………………….... 46
3-5-4 逆軌跡模式……………………………………………………….... 47
第四章　結果與討論………………………………………………................48
4-1台灣海峽南部與南海北部區域氣象條件分析….……………………... 48
4-1-1大氣溫度……………………………………………………………. 48
4-1-2相對濕度……………………………………………………………. 48
4-1-3降雨量………………………………………………………………. 49
4-2細懸浮微粒濃度時空變化趨勢分析…………………………………… 50
4-2-1細懸浮微粒濃度季節變化趨勢……....…………………………… ........50
4-2-2不同傳輸路徑細懸浮微粒濃度之差異分析………………………. 53
4-3 細懸浮微粒化學成份分析…………………………………………….. 62
4-3-1 水溶性離子成份季節變化趨勢分析…………...….……………... 62
4-3-2 金屬元素成份季節變化趨勢分析………………………………... 72
4-3-3 碳成份季節變化趨勢分析……………………………………….... 78
4-3-4 脫水醣成份季節變化趨勢分析………………………………….... 82
4-3-5 不同傳輸路徑化學成份之差異分析……………………………... 87
4-4 澎湖群島及東沙群島細懸浮微粒相關性分析………………………... 89
4-4-1 不同季節PM2.5質量濃度及化學成份之相關性分析……………. 89
4-4-2 不同傳輸路徑PM2.5質量濃度及化學成份之相關性分析………. 94
4-5 細懸浮微粒污染源解析…………………………………………….….. 95
4-5-1 富集因子解析結果……………………………………………….... 95
4-5-2 主成份分析結果…………………………………………………... 96
4-5-3 化學質量平衡受體模式解析結果………………………………... 99
第五章 結論與建議…………………………………………………………….. 110
5-1 結論……………………………………………………………………. 110
5-2 建議……………………………………………………………………. 113
參考文獻…………………………………………………………………………114
附錄A 分析物種之檢量線………………………………………………….… 123
附錄B 分析方法之品保品管數據…………………………………….……… 133
附錄C 相關性分析之四季矩陣數據………………………………………... 141

表目錄
表2-1 澎湖地區人口統計表(2015年)…….…………………………………... 5
表2-2 澎湖地區氣候資料彙整表(2015年)…………….……….......................6
表2-3 澎湖地區歷年空氣品質彙整表(2011-2015年).......…………………….7
表2-4 東沙地區氣候資料彙整表……………………………………………… 9
表2-5 國際各國及組織PM2.5法規標準………………………..………………12
表2-6 大氣懸浮微粒粒徑分類表……………………………………………… 12
表2-7 不同生質燃燒源的levoglucosan、mannson及galactosan濃度彙整表24
表3-1 採樣站位置、經緯度及高程彙整圖…………………………………….31
表3-2 細懸浮微粒採樣時間規劃表…………………………………………… 32
表3-3 元素分析儀操作參數一覽表…………………………………………… 40
表3-4 ICS-5000+型高效能離子層析儀操作參數一覽表……….................41
表4-1 採樣期間季節平均溫度彙整表………………………………………….48
表4-2 採樣期間季節平均相對溼度彙整表…………………………………….49
表4-3 採樣期間季節平均降雨量彙整表……………………………………….50
表4-4 採樣期間不同採樣點PM2.5濃度彙整表…………………………..…..53
表4-5 澎湖群島不同傳輸路徑PM2.5濃度彙整表……………....……………..59
表4-5 不同傳輸路徑PM2.5濃度彙整表………………………………………..59
表4-6 東沙群島不同傳輸路徑PM2.5濃度彙整表……………..………………61
表4-7 夏季採樣期間PM2.5中水溶性離子濃度彙整表………………………..64
表4-8 秋季採樣期間PM2.5中水溶性離子濃度彙整表………………………..64
表4-9 冬季採樣期間PM2.5中水溶性離子濃度彙整表………………………..65
表4-10春季採樣期間PM2.5中水溶性離子濃度彙整表……………………… 65
表4-11 不同季節之二次無機性氣膠(SIAs)彙整表………………...………… 67
表4-12 不同季節細懸浮微粒之氯損失彙整表…………………….…………. 68
表4-13 不同季節之硫氧化率及氮氧化率彙整表……………………………. 71
表4-14 不同季節PM2.5中地殼元素濃度彙整表……………………...……….74
表4-15 夏季採樣期間PM2.5中金屬元素濃度彙整表…………………………75
表4-16 秋季採樣期間PM2.5中金屬元素濃度彙整表………………….……..75
表4-17 冬季採樣期間PM2.5中金屬元素濃度彙整表…………………….…..76
表4-18 春季採樣期間PM2.5中金屬元素濃度彙整表…………………..……..76
表4-19 採樣期間PM2.5中碳成份濃度彙整表………………………..………..81
表4-20 採樣期間PM2.5中脫水醣成份濃度彙整表…………………..………..84
表4-21 不同海島地區左旋葡萄糖濃度比較表……………………………….. 86
表4-22 不同季節及傳輸路徑的PM2.5濃度及化學成份p value彙整表………95
表4-23 夏季採樣期間主成份分析彙整表…………………………………….. 102
表4-24 秋季採樣期間主成份分析彙整表…………………………………….. 102
表4-25 冬季採樣期間主成份分析彙整表…………………………………….. 103
表4-26 春季採樣期間主成份分析彙整表…………………………………….. 103
表4-27 受體模式解析之PM2.5指紋資料庫彙整表…………………..……….105
表4-28 澎湖群島及東沙群島夏季採樣期間污染源解析結果……………….. 106
表4-29 澎湖群島及東沙群島秋季採樣期間污染源解析結果……………….. 106
表4-30 澎湖群島及東沙群島冬季採樣期間污染源解析結果……………….. 107
表4-31 澎湖群島及東沙群島春季採樣期間污染源解析結果……………….. 107

圖目錄
圖 1-1 研究架構流程圖………………………………………………………... 3
圖 2-1 澎湖群島地理位置圖…………………………………………………... 4
圖 2-2 澎湖地區四季風玫圖(2015年)………………………………………… 7
圖 2-3 澎湖地區歷年PM2.5濃度逐月變化趨勢圖…………………………….8
圖 2-4 東沙地區四季風玫圖(2015年)………………………………………… 10
圖 2-5 東沙地區PM2.5濃度逐月變化趨勢圖…………………....................11
圖 2-6 大氣懸浮微粒粒徑分佈圖…………………………...………………… 12
圖 2-7 Chuncheon市及Yeongwol郡的PM2.5季節濃度變化趨勢圖…..….…16
圖 2-8 上海市2011-2013年PM2.5濃度逐月變化趨勢圖……………………..16
圖 2-9 西安市冬季PM1及SO42-質量濃度逐日變化趨勢圖………………….17
圖 2-10 PM2.5及水溶性離子年平均濃度分佈圖…………...…..…….……..18
圖 2-11 新德里地區夏季及冬季碳成份12小時濃度圖……………………… 22
圖 2-12 橡木及黃松木在燃燒及悶燒下脫水醣類濃度比值圖…………..…...23
圖 3-1 南海及台灣海峽交界海域細懸浮微粒採樣站位置圖…….………….. 32
圖 3-2 PM2.5採樣器及微粒分徑器組合圖………………………………….. 33
圖 3-3 微粒分徑器氣流流路示意圖………………………………………….. 34
圖 3-4 微量分析天平………………………………………………………….. 36
圖 3-5 DX-120型離子層析儀(IC)………………………..………………….. 37
圖 3-6 ICS-1100型高效能離子層析儀(HPIC)………………………….…… 37
圖 3-7 感應耦合電漿原子發射光譜儀(ICP-AES)……..……………………...38
圖 3-8 元素分析儀(EA)………………………………………………………... 39
圖 3-9 ICS-5000+型高效能離子層析儀(HPIC)……………..……………….41
圖 4-1 澎湖群島採樣期間PM2.5濃度分佈圖…………….………………….. 52
圖 4-2 東沙群島採樣期間PM2.5濃度分佈圖………………………………….52
圖 4-3 不同季節PM2.5質量濃度之時間序列圖……………………………… 53
圖 4-4 澎湖群島四季採樣期間正向軌跡路徑圖…………...………………… 54
圖 4-5 澎湖群島夏、秋季採樣期間逆軌跡圖……………………………….. 55
圖 4-6 澎湖群島冬、春季採樣期間逆軌跡圖…………………………………56
圖 4-7 東沙群島夏、秋季採樣期間逆軌跡圖…………………………………57
圖 4-8 東沙群島冬、春季採樣期間逆軌跡圖…………………………………58
圖 4-9 澎湖群島不同類型之傳輸路徑圖……………………………………... 59
圖 4-10澎湖群島不同傳輸路徑之PM2.5濃度圖……………………………. 59
圖 4-11 東沙群島不同類型之傳輸路徑圖………………………………….... 60
圖 4-12 東沙群島不同傳輸路徑之PM2.5濃度圖……………………………..61
圖 4-13 不同季節PM2.5中水溶性離子濃度分佈圖……..………...…………66
圖 4-14 不同季節細懸浮微粒氯損失及氯鈉比比較圖……..………………...68
圖 4-15 PM2.5中[NH4+]及[nss-SO42-]+[NO3-]之關係圖………….………69
圖 4-16 採樣期間澎湖群島不同季節之硫氧化率(SOR)變化趨勢圖..……… 71
圖 4-17 採樣期間澎湖群島不同季節之氮氧化率(NOR)變化趨勢圖…..…... 72
圖 4-18不同採樣季節PM2.5之金屬元素濃度分佈圖……….………………..77
圖 4-19 採樣期間澎湖群島碳成份濃度季節變化圖…………………..…….. 80
圖 4-20 採樣期間東沙群島碳成份濃度季節變化圖……………………..….. 80
圖 4-21 OC與EC之相關趨勢及最小OC/EC值………………..…………….. 82
圖 4-22 OC與O3之相關趨勢圖……………..………………………………… 82
圖 4-23 採樣期間脫水醣成份濃度季節變化趨勢圖….…………..…………..83
圖 4-24 澎湖群島鉀離子與左旋葡萄糖之時間序列圖………………………. 85
圖 4-25 東沙群島鉀離子與左旋葡萄糖之時間序列圖………………………. 86
圖 4-26 澎湖群島及東沙群島鉀離子與左旋葡萄糖之相關性………………. 86
圖 4-27 澎湖群島不同污染氣團傳輸路徑圖…………………………………. 87
圖 4-28 東沙群島不同污染氣團傳輸路徑圖…………………………………. 87
圖 4-29 澎湖群島不同傳輸路徑之水溶性離子濃度分佈圖……………….… 90
圖 4-30 東沙群島不同傳輸路徑之水溶性離子濃度分佈圖……………….… 90
圖 4-31 澎湖群島不同傳輸路徑之金屬元素濃度分佈圖……………………. 91
圖 4-32 東沙群島不同傳輸路徑之金屬元素濃度分佈圖……………………. 91
圖 4-33 澎湖群島不同傳輸路徑之碳成份濃度分佈圖………………………. 92
圖 4-34 東沙群島不同傳輸路徑之碳成份濃度分佈圖………………………. 92
圖 4-35 澎湖群島不同傳輸路徑之左旋葡萄糖濃度分佈圖………………… 92
圖 4-36 東沙群島不同傳輸路徑之左旋葡萄糖濃度分佈圖………………… 93
圖 4-37 不同季節以Fe為參考元素之富集因子圖…………………..………. 101
圖 4-38 東沙群島不同季節PM2.5污染源種類及貢獻率圖…………..………108
圖 4-39 澎湖群島不同季節PM2.5污染源種類及貢獻率圖……………..……108
圖 4-40 東沙群島不同季節PM2.5境外傳輸比例圖…………..………………109
圖 4-41 澎湖群島不同季節PM2.5境外傳輸比例圖………………..…………109

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