本研究針對菲律賓北部及台灣南部交界區域之大氣汞污染物，分別選擇菲律賓佬沃(呂宋島北部地區)、屏東車城(台灣南部地區)、東沙群島(南海北部地區)三處地點，分別設置大氣汞採樣站，同步進行大氣環境中氣態汞(TGM)、氣態氧化汞(GOM)及顆粒汞(PHg)的採樣及分析。藉以探討菲律賓北部及台灣南部交界區域的大氣汞污染物(TGM、GOM、PHg)濃度的日夜及季節變化、污染源解析及長程傳輸之影響。有鑒於台灣南部、菲律賓北部及南中國海北部相關大氣汞研究較少，故實有必要針對此區域進行大氣汞採樣及分析研究，本研究亦利用HYSPLIT Model繪製採樣期間空氣污染氣團之逆軌跡圖，藉以瞭解污染氣團之可能來源，並以全球火點圖與各空氣污染物相關性進行大氣汞污染解析。最後，將本研究結果與世界各主要城市與海島之大氣汞濃度加以比較。
就菲律賓北部及台灣南部交界區域的GEM、GOM及PHg的空間分佈而言，菲律賓佬沃測站的平均濃度為3.00±0.69 ng/m3、26.69±9.23 pg/m3、0.22±0.046 ng/m3；屏東車城測站的平均濃度為2.26±0.68 ng/m3、19.57±7.83 pg/m3、0.12±0.035 ng/m3；東沙群島測站的平均濃度為2.20±0.76 ng/m3、15.41±5.23 pg/m3、0.12±0.029 ng/m3。菲律賓佬沃測站GEM、GOM及PHg的平均濃度值皆為最高， GEM及PHg濃度最高值皆出現在菲律賓佬沃的春季，分別為3.58±0.28及0.30±0.080 ng/m3，GOM濃度最高值出現在菲律賓佬沃的夏季(28.91±9.21 pg/m3)； GEM及PHg濃度最低值皆出現在東沙群島的夏季，分別為1.58±0.33 ng/m3及0.13±0.02 ng/m3， GOM濃度最低值出現在東沙群島的秋季(12.86±5.64 pg/m3)。
就不同型態汞的分佈而言，佬沃、車城及東沙群島大氣汞濃度皆以TGM為主要型態。就不同季節而言，TGM在TAM所佔比例為96.72%(夏季)、95.86%(秋季)、93.65%(冬季)、92.64%(春季)，全年TGM佔TAM的比例為92.64~96.72%；PHg佔TAM的比例為3.28%(夏季)、4.14%(秋季)、6.35%(冬季)、7.36%(春季)，全年PHg佔TAM的比例為3.28~7.36%。
由傳輸路徑彙整結果發現，污染氣團大多來自於中國華北、華中地區，然而發生頻率最低的中國華南及中南半島所量測GEM濃度值反而卻最高，其餘來自於太平洋、日本及韓國的GEM濃度值為最低。因此，可瞭解GEM長程傳輸之貢獻不容小覷及解析氣團所帶來之大氣汞污染，此三處背景站的大氣汞濃度，與歐美地區及大氣汞南、北半球背景值相比較高，但由於此三處皆無大型人為污染源，可能與境外傳輸或當地人為活動有關，因此對於大氣汞長程傳輸的影響實不容小覷。

In this study, we investigated the spatiotemporal variation and source identification speciated atmospheric mercury in the intersectional region of southern Taiwan (Checheng), northern Philippines (Laoag), and northern South China Sea (Dongsha Islands). At each sampling site, total gaseous mercury (TGM), gaseous oxidized mercury (GOM), and particle-bound mercury (PHg) were sampled simultaneously to discuss the spatiotemporal distribution, diurnal variation, potential sources and long-range transport of speciated atmospheric mercury. This study further applied HYSPLIT model to plot and cluster the trajectories of air masses during the sampling periods to identify the potential sources of speciated atmospheric mercury. The correlation of speciated atmospheric mercury concentrations with global fire maps and transportation routes was also conducted. Finally, the speciated atmospheric mercury concentrations measured in this study were compared with those in the world's major cities and islands.
The average concentrations of GEM, GOM, and PHg were 2.76±0.36 ng/m3, 23.14±8.67 pg/m3, and 0.23±0.058 ng/m3 at the three background sites, respectively. The highest concentrations of GEM and PHg occurred at Laoag in spring, while the highest GOM concentrations was observed at Laoag in summer. The lowest concentrations of GEM and PHg were occurred at Dongsha Islands in summer, while the lowest GOM concentration was observed at Dongsha Islands in fall. Overall, TGM accounted for 92.64-96.72% of total atmospheric mercury (TAM), while PHg accounted for 3.28-7.36% of TAM.
Backward trajectory simulation showed that the polluted air masses came mainly from North China and Central China. However, South China and Indochina Peninsula with the lowest frequency had the highest concentration of GEM. On the other hand, polluted air masses transported from the western Pacific Ocean, Japan Islands, and Korean Peninsula had the lowest GEM concentration. This study revealed that the concentrations of speciated atmospheric mercury at the three background sites were generally higher than those in Europe and the United States, but lower than those in Asia except Japan. It might be attributed to long-range transport or local human activities since there are no large-scale anthropogenic sources in the target area.

論文審定書…………………………………………………………………………….i
論文公開授權書………………………………………………………..……………..ii
中文摘要……………………………………………………………………………...iii
英文摘要……………………………………………………………………………....v
目錄…………………………………………………………………………………..vii
表目錄………………………………………………………………………...……….x
圖目錄……………………………………………………………………………..….xi
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……………………………………………………………3
第二章 文獻回顧…………………………………………………………………..…5
2.1 汞之背景介紹…………………………………………………….…………5
2.1.1 汞的基本特性………………………………………………..…………5
2.1.2 大氣汞的型態及組成特徵…………………………………………..…8
2.1.3 大氣汞的生成機制及全球循環機制…………………………………11
2.2 汞的健康風險…………………………………….………………………..16
2.2.1 汞的毒理性質………………………………………...……………….16
2.2.2 汞的暴露危害標準………………………………...………………….19
2.3 大氣汞量測方法…………………………………………………………... 21
2.3.1 大氣汞量測技術演進………………………...…………………….…21
2.3.2 不同型態大氣汞採樣及分析方法……………………………..……..24
2.4 污染源解析模式之原理及應用…………………………………………...27
2.4.1 逆軌跡模式之基本原理………………………………………………27
2.4.2 逆軌跡模式之應用……………………………………………………29
2.5 國內外大氣汞相關研究…………………………………………………...31
第三章 研究方法……………………………………………………………………38
3.1 大氣汞採樣規劃...…………………………………………………………38
3.1.1 大氣汞採樣地點.…………………………………………….…..……38
3.1.2 大氣汞採樣時間….…………………………………….……..………38
3.2 大氣汞採樣方法.………………………..…………………………………40
3.2.1 TGM採樣方法.…………………………………………………..……40
3.2.2 GOM採樣方法.………………………………………………….….…44
3.2.3 PHg採樣方法……………………………………………………….…47
3.3 大氣汞分析方法.…………………………………………………………..49
3.3.1 TGM分析方法及步驟.………………………………………………..50
3.3.2 GOM分析方法及步驟.………………………………………………..52
3.3.3 PHg分析方法及步驟.…………………………………………………52
3.4 大氣汞採樣及分析之品保及品管(QA/QC) .……………………………..53
3.4.1人員資格……………………………………………………………….53
3.4.2品保及品管樣品……………………………………………………….53
3.5 冷蒸氣原子螢光光譜儀(Cold Vapor Atomic Fluorescence Spectrometry,
CVAFS)…………………………..……………………………..…………57
3.6 污染源解析方法.………………………………………………..…………58
3.6.1 逆軌跡模式.……………………………………………………...……58
3.6.2 全球火點分佈.……………………………………...…………………58
第四章 結果與討論.…………………………………………………………..…….60
4.1 菲律賓北部與台灣南部區域之氣象條件分析.…………………………..60
4.1.1 風速及風向.……………………………………………………...……60
4.1.2 氣溫、濕度及降雨量.…………...……………………………………66
4.2 GOM擴散管驗證與測試.…………………………………………….……68
4.2.1 GOM擴散管空白測試.……………………………………..…………68
4.2.2 GOM擴散管穿透率測試.……………………………………………..69
4.2.3 GOM擴散管平行比對測試.……………………………..……………70
4.3 金汞齊的驗證與測試.……………………………………………………..71
4.3.1 金汞齊空白測試.……………………………………...………………71
4.3.2 金汞齊穿透率測試…….………………………………………...……72
4.3.3 金汞齊日夜採樣測試…………………………………………………73
4.4菲律賓北部與台灣南部交界區域大氣汞時空分佈.……………………...75
4.4.1 菲律賓北部及台灣南部交界區域不同型態汞之季節變化趨勢……76
4.4.2 菲律賓北部及台灣南部區域不同型態大氣汞之空間分佈………....79
4.4.3 菲律賓北部及台灣南部區域氣固相分佈特徵………………...…….80
4.4.4 菲律賓北部及台灣南部交界區域不同季節TGM及PHg發生頻率分
佈.……………………………………………………………………...83
4.4.5 菲律賓北部及台灣南部交界區域高污染季節TGM日夜濃度比較.85
4.4.6 菲律賓北部及台灣南部區域春、冬高污染季節PHg與PM2.5
日夜濃度相關性比較……………………………………………..…..85
4.5菲律賓北部及台灣南部交界區域大氣汞污染來源解析.……………...…87
4.5.1 污染氣團傳輸路徑聚類分析…………………………………....……87
4.5.2 全球火點分佈監測.…………………………………...………………95
4.5.3 大氣汞濃度、氣象參數及空氣污染物之相關性分析..……………..97
4.6與世界各地大氣汞濃度比較.……………………………………………...99
第五章 結論與建議.…………………………………………………….……..…..103
5.1 結論.…………………………………………………….……………..….103
5.2 建議.……………………………………………………………….…..….105
參考文獻.…………………………………………………………………….……..106
附錄A 汞標準品體積與溫度關係表…………………...………………………...122
附錄B 不同型態大氣汞量測數據表……………………..………………………125

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