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研究生：	鄭妙靜 Cheng, Miao-Ching
論文名稱：	利用主要元素、微量元素與鍶鉛同位素探討大氣中水溶性元素組成之傳輸與來源 Sources and Transportation Mechanism of Dissolved Elements in the Atmosphere: Major, trace elements and Sr-Pb isotopes
指導教授：	游鎮烽 You, Chen-Feng
學位類別：	博士 Doctor
系所名稱：	理學院 - 地球科學系 Department of Earth Sciences
論文出版年：	2010
畢業學年度：	98
語文別：	英文
論文頁數：	177
中文關鍵詞：	鍶同位素、鉛同位素、主要及微量元素、雨水、氣溶膠
外文關鍵詞：	Sr isotopes, Pb isotopes, major and trace elements, rainwater, aerosols
相關次數：	點閱：121 下載：2
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本研究中第一部分為短時間序列台南市雨水樣本，包括四個颱風事件。分析主要離子、重金屬和鉛同位素以了解颱風路徑其氣流路徑在短期內對化學組成的變化。颱風期間，銅鉛通量之遽烈增加強調沿海地區重金屬進出平衡的改變。結合氣流逆軌跡及主變量分析結果顯示同樣的氣流路徑可能會造成相似的雨水化學組成。
第二及第三部份以彭佳嶼47個月雨水樣品(1998-2001)，測量鍶鉛同位素、主要元素及微量元素以暸解雨水化學的空間和時間變化。鍶同位素結果顯示在冬季季風時期碳酸鹽貢獻高達 45％，但在其他季節海水是雨水中主要的鍶來源（> 50％）。整體主成分分析結果顯示地殼元素、工業污染及燃燒煉鋼業影響了雨水的化學組成。鉛同位素的相對貢獻計算顯示彭佳嶼雨水中的鉛在夏季主要受到台灣來源的影響，而來自中國大陸的鉛則在其他季節有明顯影響。
中國大陸14個城市氣溶膠中的水溶性成分有助於了解化學組成的季節和空間變化。主成分分析的結果顯示人為影響是最主要的來源。冬季水溶性鋁和鐵是由季風帶來並累積在氣溶膠中進而影響沿海地區的濃度分布。水溶性硫，鋅和鉛的濃度分佈則與大陸主要的工業區和地形有關。

A suite of time-series rain specimens including four typhoon events are collected from Tainan city, southern Taiwan and analyzed for major ions, heavy metals and Pb isotopes to elucidate mechanisms causing dissolved components variation in rainwater and to understand how heavy metals are transported by air-mass along typhoon pathways in short-term period. The Cu and Pb fluxes increase during typhoon events and thus impact importantly the chemical budgets of these metals in coastal ocean. Combining air-mass backward trajectories and PCA results demonstrates consistently that air-mass routes dictate critically the dissolved chemical characteristics in rains.
47 monthly rainwater samples for four years were measured Sr and Pb isotopes, major elements, as well as trace elements to understand spatial and temporal variations of chemical characteristics. Model results showed carbonate contributes up to 45% during the winter monsoon period, but seawater is the dominant Sr source in rainwater (>50%) at other times. Overall PCA results for trace elements show crustal materials, industrial pollution related, and combustion of steel making industry affect chemical compositions. The relative contributions calculations support that aerosols from Taiwan affect Pb isotopes ratios in summer and the sources from mainland China are observed in other seasons.
The water-soluble components in fine paricles in fourteen cities over China would help to understand the seasonal and spatial variations in a year. The PCA results show that anthropogenic materials are the most important sources of water-soluble contents in summer and winter. The water-soluble Al and Fe are brought by monsoon and accumulated in aerosols in winter. The distributions of water-soluble S, Zn and Pb are related to the industrial zones and topography.

Table of Contents
Abstract………………………………………………………………..I
Chapter 1. Introduction
1 General introduction……………………………………………….2
2 Applications of Sr isotopes in atmospheric chemistry……………..3
2.1 Basic introduction of Sr…………………………………………………3
2.2 Sr in atmospheric aerosols and rainwater………………………………4
3 Applications of Pb isotopes in atmospheric chemistry…………….4
3.1 Basic introduction of Pb………………………………………………...4
3.2. Pb in atmospheric aerosols and rainwater……………………………...8
4 The purposes of this study…………………………………………9
References…………………………………………………………..10
Chapter 2. Sources of Major Ions and Heavy Metals in Rainwater Associated with Typhoon Events in Southwestern Taiwan
Abstract…………………………………………………………………18
1 Introduction…………………………………………………………19
2. Sample collection and methodology………………………………..21
2.1. Rainwater…………………………………………………………………21
2.2 Typhoon events during the study periods…………………………………23
2.3. Analytical procedures…………………………………………………….24
2.4. Backward trajectory……………………………………………………...25
2.5. Statistical analysis………………………………………………………..25
3. Results and Discussion……………………………………………..25
3.1. Major elements concentrations…………………………………………..27
3.2 Trace elements concentrations and enrichment factors (EFs)…………….30
3.3. Principal component analysis……………………………………………33
3.3.1 Dissolved chemical elements……………………………………...33
3.3.2 Air-mass Pathways………………………………………………...36
3.4. Pb isotopes……………………………………………………………….37
3.5. Major ion and trace element fluxes………………………………………40
4. Conclusions………………………………………………………...45
References……………………………………………………………46
Chapter 3. Seasonal variation in long-range transported dust to a subtropical islet offshore northern Taiwan: Chemical composition and Sr isotopic evidence in rainwater
Abstract………………………………………………………………….52
1 Introduction…………………………………………………………53
2. Sampling and analytical methods…………………………………..54
2.1. Rainwater and aerosol dust collection……………………………………54
2.2. Analytical methods……………………………………………………….55
3. Results and Discussion……………………………………………..57
3.1. Dissolved chemical data………………………………………………….59
3.2. Sr isotopes in rainwater…………………………………………………..62
3.2.1 Seasonal variations………………………………………………...62
3.2.2 Contribution from volcanic eruptions……………………………..65
3.2.3 Estimated relative contributions…………………………………...70
4. Conclusion………………………………………………………….73
References…………………………………………………………....74
Chapter 4. Seasonal variations of long-range transport of pollutants in rainwater: Heavy metals and Pb isotopes evidences
Abstract…………………………………………………………………80
1 Introduction…………………………………………………………81
2. Sample location and analytical methods…………………………...82
2.1. Rainwater collection……………………………………………………..82
2.2. Analytical methods……………………………………………………….83
3. Results and Discussion……………………………………………..84
3.1. Chemical data…………………………………………………………….84
3.2. Principal component analysis (PCA)…………………………………….93
3.2.1 Trace elements…………………………………………………….93
3.2.2 Seasonal variations………………………………………………..94
3.3. Pb isotopes……………………………………………………………….98
3.3.1 Seasonal Variations………………………………………………..98
3.3.2 Three end-member contribution from Taiwan and mainland China..……………………………………………………………100
4. Conclusions……………………………………………………….106
References…………………………………………………………..107
Chapter 5. Spatial and seasonal variations of water-soluble components in fine aerosols over China
Abstract………………………………………………………………...115
1. Introduction……………………………………………………….116
2. Sample location and analytical methods…………………………..118
3. Results and Discussion……………………………………………122
3.1 Chemical Compositions…………………………………………………122
3.2 Spatial and Seasonal Variations of water-soluble contents……………...127
3.2.1 Major elements (Na, Ca, S and Cl)………………………………127
3.2.2 Heavy metals (Al, Fe, Ba, Zn, Pb and As)…….…………………143
3.3 Industrial zones and topography of China……………………….165
4. Conclusions……………………………………………………….166
References…………………………………………………………..167
Chapter 6. Conclusions and Future Prospects
1 Conclusions………………………………………………………..174
2 Future Prospects…………………………………………………...176
                                    

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