本研究旨在針對台灣海峽之海岸、海域及海島地區進行細懸浮微粒同步採樣，本研究於2013年至2015年在台灣海峽設置六處細懸浮微粒，分別於台灣海峽西岸兩處(廈門及福州)、海島地區一處 (澎湖)及台灣海峽東岸三處(台北、台中及高雄)採樣站進行同步細懸浮微粒採樣，並針對所採集之細懸浮微粒樣本進行化學特性分析，藉以探討此台灣海峽區域內細懸浮微粒的時空分佈、化學指紋特徵、污染貢獻來源及種類、跨境傳輸路徑之影響。
台灣海峽細懸浮微粒時空分佈結果顯示，台灣海峽之細懸浮微粒濃度呈現西岸普遍高於東岸及海島地區，且細懸浮微粒濃度有北向南遞增的趨勢。細懸浮微粒(PM2.5)及粗微粒(PM2.5-10)於冬、春兩季平均濃度明顯高於春、夏兩季。化學成分結果顯示，主要的化學組成以水溶性離子成份中以二次無機性氣膠(SO42-、NO3-、NH4+)、地殼金屬元素(Mg, Ca, AL, K, 及Fe)及人為污染金屬元素(Pb, Ni,及Zn)為主。此外，高OC/EC普遍發現於台灣海峽西岸主要之固定污染源(電廠、石化廠及工業區)下風處之採樣點。
本研究針對細懸浮微粒之傳輸途徑及可能污染來源進行進一步解析，高污染氣團傳輸軌跡主要來自於華北、中國大陸東部沿海、朝顯半島或南日本島。污染氣團主要藉由長程傳輸從此區域中大規模燃煤燃燒及生質燃燒取暖傳輸至此區域所造成。由不同傳輸途徑細懸浮微粒之受體模式模擬結果顯示，二次衍生性污染源貢獻率主要呈現由西岸往海島及東岸有逐漸上升之趨勢，可能原因為高衍生性氣膠累積生成主要因長傳輸距離及花費較長時間傳輸至台灣海峽東岸所致。另外，本研究利用所採集之細懸浮微粒扣除背景日之境外傳輸推估方式結果顯示，台灣海峽西岸、東岸及海島地區之境外傳輸貢獻率分別為44.9%、57.3%及39.8%。
本研究利用海研三號在高細懸浮微粒污染季節期間，於台灣海峽上海島及海面上所採集細懸浮微粒採樣結果顯示，海面及海島上所採集之懸浮微粒均以細微粒為主。將海面上及海島地區所採集之細懸浮微粒進行化學特性分析結果顯示，非海鹽水溶性離子佔細懸浮微粒貢獻率於海島地區明顯高於海面上，而海鹽類水溶性離子成分佔細懸浮微粒貢獻率則呈現海面上明顯高於海島地區。
台灣海峽三個主要島嶼及鄰近陸地之地面風場氣象模式模擬結果顯示，馬祖群島之地表氣流場主要受到由北風傳輸所影響，此結果顯示馬祖地區污染來源主要受到北方污染物長程傳輸之影響；金門群島之地表氣流場主要受到高壓反氣旋系統造成污染物易於累積於廈門灣內；澎湖群島西岸之地面風場主要受到季節風影響，而東岸則受到及海陸風交互影響，此結果顯示澎湖群島氣流場主要受到長程傳輸及海陸風效應之影響。

This study aims to investigate the spatiotemporal distribution, chemical characteristics, source apportionment, and the contribution of transportation routes of atmospheric fine particle (PM2.5) over the coastal, sea, and offshore areas of the Taiwan Strait. Fine particles (PM2.5) were simultaneously collected at six sites including two sites (Xiamen and Fuzhou) on the west-side of the Taiwan Strait, one site (Penghu Islands) at an offshore site, and three sites (Kaohsiung, Taichung, and Taipei) on the east-side of the Taiwan Strait in the years of 2013-2015.
Field sampling of PM2.5 at large scale coastal and islands areas around the Taiwan Strait indicated that the average PM2.5 concentrations at the west-side sites were generally higher than those at the east-side sites, while those increased significantly from the north sites to the south sites at both sides of the Taiwan Strait, respectively. PM2.5 and PM2.5-10 concentrations in winter and spring were generally higher than those in summer and fall. The most abundant chemical composition were secondary inorganic aerosols (SO42-, NO3-, and NH4+), natural crustal (Mg, Ca, AL, K, and Fe), and anthropogenic metals (Pb, Ni, and Zn). Moreover, high OC/EC ratios of PM2.5 were commonly observed at the west-side sites located at the downwind of major stationary sources, such as utility power plants, petrochemical plants, and industrial complexes.
Results obtained from the transportation routes and potential sources of PM2.5 at the Taiwan Strait, clustered transportation routes based on backward of trajectory simulation indicated that PM2.5 could be transported from North China, eastern coast of China, Korea Peninsula, or South Japan, suggesting that it was mainly attributed to the combination of the relatively elevated emissions from fossil fuel (e.g. coals) combustion and biomass (e.g. woods) burning for space heating, long-range transport (LRT) of air pollutants. Results obtained from CMB receptor modeling showed that the source apportionment of secondary sources were in order of east-side sites > offshore site > west-side site, suggesting aged secondary particles could be formed during the transportation process by long longer range and duration toward the east-side sites and the offshore site. Result obtained from cross-boundary contributions of PM2.5 around the Taiwan Strait showed that the average cross-boundary transportation contributions 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.
Results obtained from the chemical characteristics over sea and offshore site in the Taiwan Strait for sampling cruises indicated that fine particles were generally higher than those of coarse particles over sea than those at the offshore site. Moreover, the contributions of nss-WSI for PM2.5 at the offshore site were obviously higher than those over sea, while the contributions of ss-WSI for PM2.5 at the offshore site were generally lower than those over sea during the high pollution episodes seasons.
The simulated surface wind fields showed that northerly winds blew atmospheric particles from long-range transportation toward the northwestern Taiwan Strait in the Matsu Islands domain, while high pressure anticyclonic systems caused the accumulation of atmospheric particles at the Xiamen Bay in the Kinmen Islands domain, and the prevailing winds and sea-land breezes highly influenced the surface wind fields over the island and coastal regions caused by the combination of local sources and northward long-range transportation in the Penghu Islands domain.

論文審定書……………………………………………………………………….……. i
誌謝………………………………………………………..…………………………… ii
中文摘要……..……………………………………………………..……...............… iii
ABSTRACT………………………………………………………………………….... v
TABLE OF CONTENTS……………………………………………………………... vii
LIST OF TABLES…………………………………………………………………….. xi
LIST OF FIGUARES………………………………………………………………..... xiv
CHAPTER ONE Introduction….…………………………………………….....…... 1
1.1 Background ………………….…………………………………………….………. 1
1.2 Objectives………………………………………………………………….……….. 3
1.3 Scope…………………………………………………………………….…………. 3
CHAPTER TWO Review of Literatures…………….……………………………….. 6
2.1 Background of Coastal and Offshore Regions around the Taiwan Strait……….. 6
2.1.1 Fuzhou Region……………………………………………………………..…... 6
2.1.2 Xiamen Region…………………………………………………………..…….. 7
2.1.3 Penghu Islands…………………………………………………………..……. ........ 9
2.1.4 Kaohsiung Region……………………………………………………..………... 10
2.1.5 Taichung Region………………………………………………………....……... 11
2.1.6 Taipei Region……………………………………………………………...…..... 11
2.2 Physicochemical Characteristics of Atmospheric Particles…………………….…..12
2.3 Size Distribution of Atmospheric Particles…………………………………….…... 12
2.4 Chemical Characteristic and Fingerprint of Atmospheric Particles…………….…..13
2.4.1 Water-soluble Ionic Species of Atmospheric Particles……………………….. 13
2.4.2 Metallic Elements of Atmospheric Particles…………………………………. 15
2.4.3 Enrichment Factors of PM2.5 Metallic Elements……………………..………. 16
2.4.4 Carbonaceous Species of Atmospheric Particles…………………………..… 17
2.5 Overview of the Coastal Areas of Particulate Matter over the World………….… 18
2.6 Long-Range Transportation of Particulate Matter over the World…...………….. 19
2.7 Overview of the Sea Salts of Particulate Matter over Ocean and Coastal Region 21
CHAPTER THREE Methodologies………………………………………………….. 24
3.1 Sampling Protocol…………………………………………………………….……. 24
3.2 Chemical Analysis…………………………………………………………….……. 25
3.2.1 Analysis of Water-Soluble Ionic Species…………………………………...… 25
3.2.2 Analysis of Metallic Elements…..………………………………………..…... 26
3.2.3 Analysis of Carbonaceous Species……………………………………..…….. 26
3.3 Quality Assurance and Quality Control………………………………………..…… 28
3.4 Chemical Transformation of SO2 and NOX……………………………………..….. 28
3.5 Chemical Mass Balanced (CMB) Receptor Model…………………………….…... 29
3.6 Transportation Routes of Air Masses………………………………………….…… 30
CHAPTER FOUR Spatiotemporal Distribution and Chemical Characteristic of PM2.5 around the Taiwan Strait………...……….……………. 32
4.1 Spatiotemporal Variation of PM2.5 Concentration…………………………………. 32
4.2 Chemical Characteristic of PM2.5……………………………………………….….. 37
4.2.1 Water-soluble Ionic Species of PM2.5 ……………….……………………..… 37
4.2.2 Metallic Elements of PM2.5…………………………………………………… 43
4.2.3 Carbonaceous Species of PM2.5………………………………………..……... 44
4.3 Source Indicators of PM2.5………………………..………………………..………. 50
4.4 Distribution of PM2.5 Chemical Composition…………………………………..….. 51
4.5 Reconstruction of PM2.5 Mass...……………………………………………............ 53
4.6 Chemical Transformation of SO2 and NOX…………………………………..….…. 55
4.7 Enrichment Factors of Metallic Elements for PM2.5………………….……….…… 58
4.8 Chemical forms of SO4 2-, NO3– and NH4+ particulate……………………...…… 59
CHAPTER FIVE Transportation Routes and Potential Sources of PM2.5 and Their Chemical Characteristics on Both Sides of the Taiwan Strait………………………………………………………..…… 62
5.1 Clustered Transportation Routes of Air Masses…………...…………………..……62
5.2 Seasonal Variation of PM2.5 for Clustered Transportation Routes……………..…66
5.3 Chemical Characteristics of PM2.5 for Clustered Transportation Routes……..…71
5.3.1 Water-soluble Ionic Species of PM2.5 for Clustered Transportation Routes… 71
5.3.1.1 Inorganic Ionic Species of PM2.5 for Clustered Transportation Routes….. 71
5.3.1.2 The Distribution of Sea Salts in PM2.5 for Clustered Transportation Routes…………………………………………………………………… 76
5.3.2 Metallic Elements of PM2.5 for Clustered Transportation Routes…………… 81
5.3.2.1 Metallic Elements of PM2.5……………………………………………… . 81
5.3.2.2 Enrichment Factors of Metallic Elements for PM2.5……………………... 83
5.3.3 Carbonaceous Species of PM2.5 for Clustered Transportation Routes………. 85
5.3.4 Chemical Transformation of SO2 and NOX for Clustered Transportation Routes…………………………………………………………………………. 86
5.4 Source Apportionment of PM2.5 for Clustered Transportation Routes………… . 88
5.5 Background and Cross-boundary Contributions of PM2.5 of the Taiwan Strait… 96
5.5.1 Cross-boundary Contributions of PM2.5 around the Taiwan Strait…………… 96
5.5.2 Cross-boundary Contributions of Water-soluble Ionic Species in PM2.5 around the Taiwan Strait……………………………………………………… 99
5.5.3 Cross-boundary Contributions of Metallic Elements in PM2.5 around the Taiwan Strait…………………………………………………………………. 101
5.5.4 Cross-boundary Contributions of Carbonaceous Species in PM2.5 around the Taiwan Strait…………………………………………………………………. 103
Chapter SIX Chemical Characteristics and Spatial Variation of Atmospheric Fine Particles over Sea and Islands in the Taiwan Strait for Sampling Cruises………………………………………………… 104
6.1 Sampling Protocol of Atmospheric Aerosol Particles…………………………… 104
6.2 Spatiotemporal Variation of PM2.5 Concentrations over Sea and Islands…… 105
6.3 Water-soluble Ionic Species of PM2.5 over Sea and Islands……………………108
6.4 Contribution of Sea Salts to PM2.5 over Sea and Islands……………………… 108
6.5 Ratio of Chloride to Sodium and Chloride Deficit of PM2.5……………......…… 114
6.6 Spatial Variations of Water-soluble Ionic Species of PM2.5 for Various Routes of Cruise………………………………………………………………………………. 117
6.7 Metallic Elements of PM2.5 for Various Routes of Cruises……………………… 119
6.8 Carbonaceous Species of PM2.5 for Various Routes of Cruise…………………. 122
CHAPTER SEVEN Seasonal Variation and Chemical Characteristics of Atmospheric Particles at Three Islands in the Taiwan Strait………………………………………………………… 126
7.1 Introduction………………………………………….. ………….………………… 126
7.2 Selection and Description of Sampling Location…………………..………………. 130
7.3 Spatiotemporal Variation of PM10 Concentration…………………..……………… 134
7.4 Chemical Characteristics of PM10 at Three Islands in the Taiwan Strait…….… 136
7.4.1 Water-Soluble Ionic Species of PM10 at Three Islands in the Taiwan Strait…. 136
7.4.2 Metallic Elements of PM10 at Three Islands in the Taiwan Strait………..…... 139
7.4.3 Carbonaceous Species of PM10 at Three Islands in the Taiwan Strait…...… 141
7.5 Source Apportionment of PM10………………………………………………..…… 144
7.6 Surface Wind Fields of Three Domains in the Taiwan Strait………………….……147
CHAPTER EIGHT Conclusions……….…………………………………………..… 149
REFERENCES……………………………………………………………………….. 153
APPENDIX A Clustered Backward Trajectory Routes at both Side Sites of the Taiwan Strait……………..…………………………………………. 181
APPENDIX B Calibration Curve of Chemical Analytical Data…………………… 186
APPENDIX C The Cross-boundary Contribution of PM2.5 at Both Side Sites of the Taiwan Strait……………………………………………………. 189
APPENDIX D Chemical Analytical Data of Atmospheric Fine Particle of the Taiwan Strait………………………………………………………… 193

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