臺灣博碩士論文加值系統

本研究，在2005年1月至2006年11月期間，於國立海洋大學工學二館頂樓（北緯25度9分，東經121度46分），以高流量採樣器（TE-5170, Tish Enviromental, INC.）收集大氣懸浮微粒，共隨機選取193份氣膠樣本分析其中所含的主要水溶性離子和磷濃度，並以3-day氣流逆軌跡回推圖推測氣膠可能的來源地區。
對於大氣氣膠中磷濃度的分析，主要以連續萃取法（sequential extraction method，SEDEX）萃取總無機磷（total inorganic phosphorus, TIP）、有機磷（organic phosphorus, OP）和總磷（total phosphorus, TP）；另以Milli-Q水萃取氣膠中的溶解態無機磷（dissolved inorganic phosphorus, DIP），分析總無機磷（TIP）的溶解度（solubility）。萃取出的各相磷物種，以Murphy and Riley（1962）改良的磷鉬藍法（molybdate blue metod）進行濃度分析。
研究結果顯示，氣膠中總無機磷（TIP）在總磷（TP）中平均占約70±11 %，範圍40.6∼97.4 %；有機磷（OP）於總磷（TP）中的含量占2.4∼59.5 %，平均占約30±11 %；溶解度（solubility）平均為47±19 %。研究區域大氣中磷濃度分佈的強度為TIP＞OP＞DIP，其濃度關係為TIP/ TP＝0.80（r＝0.98）、OP / TP＝0.2019（r＝0.77）、DIP / TP＝0.20（r＝0.76）。本研究區域各相磷濃度分佈有明顯的季節性變化，Solubility、DIP/TP和 TIP/TP的高值出現在1月、3月、4月、7月、10月∼12月。主要水溶性離子的測定結果，指出本研究區域1∼5月及11和12月份的氣膠的來源以陸源性為主，9∼10月以海源性來源為為主。而主要陰陽離子與各相磷的主成份分析結果顯示，地殼、海洋和燃燒來源為採樣期間本研究區域大氣氣膠組成的三個主要控制因素。

We analyzed 193 aerosol samples, collected from January 2005 to November 2006 at a coastal site on the southern East China Sea at Keelung city, Taiwan, for phosphorus species, and water-soluble major ions. In addition, 3-day back trajectories of air masses arriving daily at the sampling site were calculated to determine the potential aerosol source regions.
In this study, we use a sequential extraction method to extract total inorganic phosphorus (TIP),organic phosphorus(OP),and total phosphorus
(TP) in the aerosol. Total phosphorus (TP) content was then calculated as the sum of total inorganic phosphorus (TIP) and organic phosphorus (OP). Addition, we use Milli-Q water to extract dissolved inorganic phosphorus (DIP) for analyzing solubility of total inorganic phosphorus (TIP). All phosphorus species use the molybdate blue method to analyze.
The result indicates that the average percentage concentrations of individual phosphorus species in TP were 70±11% (range 40.6∼97.4%) for TIP, 30±11% (range 2.4∼59.5%) for OP. The average value of the solubility is 47±19%. The strong correlations were apparent between TP, TIP, OP and DIP, suggesting the common sources and transport mechanisms for these species. The concentration relationships and regression coefficients between these species respectively are TIP/ TP＝0.80(r＝0.98), OP / TP＝0.2019(r＝0.77), DIP / TP＝0.20(r＝0.76).
The obtained concentrations of major ions indicate that a continental source was dominant from January to May and from November to December, and an oceanic source from September to October. The measured atmospheric concentrations of phosphorus species show clear seasonal variations, and correspond to the different sources and weather conditions. The results of a Principal Component Analysis of combined major ions and phosphorus species indicate that crustal sources, marine sources, and combustion sources are the three major controlling factors during the sampling period.

中文摘要.....................................................................................................I
英文摘要..................................................................................................III
表目錄......................................................................................................IX
圖目錄.....................................................................................................XII
第一章 ......................................................................................................1
1.1 簡介.....................................................................................................1
1.2 研究內容.............................................................................................2
1.3 研究目的.............................................................................................2
第二章 文獻回顧......................................................................................4
2.1 磷元素.................................................................................................4
2.1.1 磷的重要性...................................................................................4
2.1.2 磷在環境中的主要型態...............................................................4
2.2 磷的生物地球化學循環.....................................................................5
2.2.1 磷循環的特點...............................................................................5
2.2.2 磷循環之基本過程.......................................................................6
2.2.3 陸地生態系統中的磷循環...........................................................7
2.2.4 水生生態系統中的磷循環...........................................................8
2.3 磷在大氣中的行為...........................................................................12
2.3.1 大氣沉降在海洋生地化系統中扮演之角色.............................12
2.3.2 大氣氣膠輸入到海洋中的磷.....................................................13
2.4 大氣氣膠中磷物種的測定方法.......................................................14
第三章 研究方法....................................................................................18
3.1採樣地點.............................................................................................18
3.2使用儀器.............................................................................................19
3.2.1採樣儀器......................................................................................19
3.2.2分析儀器......................................................................................19
3.3氣膠樣本的前處理.............................................................................21
3.4化學分析.............................................................................................22
3.4.1化學分析的處理步驟..................................................................22
3.4.2分析方法......................................................................................25
3.4.2.1磷酸鹽分析方法.......................................................................25
3.4.2.2水溶性陰陽離子的分析方法...................................................29
3.4.3方法回收率..................................................................................32
3.4.4樣品查核......................................................................................34
第四章 結果和討論................................................................................35
4.1 研究區域的氣象資料.......................................................................35
4.1.1氣象資料統計..............................................................................35
4.1.2氣團來源統計..............................................................................36
4.2 研究區域氣膠的質量濃度分佈特性...............................................40
4.3 氣膠的中水溶性陰陽離子濃度分佈特性.......................................46
4.3.1 氣膠中水溶性陰陽離子的濃度分析結果.................................48
4.3.2 海鹽性Na+、非海鹽性nss-Ca2+和nss-SO42-的濃度分佈情形.
...............................................................................................................50
4.3.3 氣膠中水溶性陰陽離子濃度與質量濃度的相關性.................55
4.4 氣膠的DIP、TIP、OP和TP的濃度分佈特性...................................56
4.4.1 乾沉降的DIP、TIP、OP和TP的濃度分析結果.........................57
4.4.2 乾沉降的DIP、TIP、OP和TP的日濃度分佈變化.....................60
4.4.3 乾沉降的DIP、TIP、OP和TP的月平均濃度分佈變化.............62
4.4.4 氣膠中的DIP、TIP、OP和TP濃度與質量濃度的相關性.........75
4.4.5 氣膠中的DIP、TIP、OP和TP之間的濃度分佈關係.................77
4.4.6 氣膠中磷物種的溶解度及濃度相對百分比例分佈變化.........79
4.4.7 氣膠中DIP、TIP、OP和TP與主要陰陽離子的相關性分析.....84
4.4.8氣膠中DIP、TIP、OP和TP與主要陰陽離子的主成份分析.....86
第五章 結論............................................................................................91
參考文獻..................................................................................................95
附錄一 2005年1月至2006年11月磷物種濃度.................................102
附錄二 2005年1月至2005年12月3-day 氣流逆軌跡回推圖......108
附錄三 2006年1月至2006年11月3-day 氣流逆軌跡回推圖......115
表目錄
Table 1磷主要儲存庫和通量…...................................................……...11
Table 2人類增強的全球磷循環............................................…..….…...11
Table 3磷酸鹽分析試劑的配法..............................................................26
Table 4磷酸鹽分析檢量線的製作方式..................................................27
Table 5磷酸鹽化學分析數值的計算方式..............................................28
Table 6陰陽離子分析試劑的配法..........................................................29
Table 7陰陽離子分析檢量線的製作方式..............................................30
Table 8測量陰陽離子參數的設定..........................................................31
Table 9方法回收率_對照組(A組)實驗數據..........................................33
Table 10方法回收率_實驗組(B組)實驗數據........................................33
Table 11方法回收率_ 對照組(A組)與實驗組(B組)的實驗數據比較
..................................................................................................................33
Table 12磷物種樣本測定的查核............................................................34
Table 13磷物種與主要陰陽離子偵測極限............................................34
Table 14北部海域氣象資料....................................................................37
Table 15中央氣象局_基隆地區的氣象資料..........................................38
Table 16北部海域氣象資料統計............................................................38
Table 17本研究區域不同來源氣流逆軌跡回推圖資料統計................39
Table 18氣膠質量濃度的極大、極小值、中位數、年平均值和標準差..............................................................................................................40
Table 19氣膠的質量濃度月平均分佈和標準差....................................41
Table 20氣膠中主要陰陽離子月平均濃度............................................49
Table 21氣膠中主要陰陽離子的平均濃度與標準差............................49
Table 22不同時序的海鹽性Na+和非海鹽性nss-Ca2+、nss-SO42-、nss-K+的濃度的平均值......................................................................................54
Table 23氣膠中主要陰陽離子濃度與氣膠質量濃度的相關性矩陣....55
Table 24氣膠的DIP、TIP、OP和TP濃度的極大值、極小值、中位數、平均值和標準差..............................................................................59
Table 25氣膠所含各相磷物種濃度的月平均值....................................63
Table 26不同時序的氣膠所含各相磷物種濃度的平均值....................64
Table 27氣膠中DIP、TIP、OP和TP與質量濃度的相關性矩陣............76
Table 28無機磷溶解度及TIP、OP在TP中所占百分比例的基本統計量..............................................................................................................79
Table 29各月氣膠所含無機磷的溶解度及各磷物種所占百分比例....80
Table 30不同時序氣膠所含無機磷溶解度及各磷物種所占百分比例平均值..........................................................................................................80
Table 31氣膠中主要陰陽離子與磷物種的相關性矩陣........................85
Table 32氣膠中主要陰陽離子與磷物種的主成份特徵值與解釋變異比例..............................................................................................................89
Table 33前三項因素的因素負荷值........................................................90
圖目錄
Fig 1磷循環………..………………………….………………………..10
Fig 2採樣地點示意圖………………………….………………………18
Fig 3 Chen et al.（2006）的實驗流程圖…………………………………24
Fig 4本研究實驗流程圖..…….………..………………………………24
Fig 5氣膠日質量濃度時間分佈圖…………….………………………41
Fig 6氣膠月平均質量濃度分佈的時間趨勢圖……….………………42
Fig 7氣膠月平均質量濃度與Na2+月平均質量濃度………...……......52
Fig 8氣膠月平均質量濃度與nss-Ca2+月平均質量濃度時間趨勢圖...52
Fig 9氣膠月平均質量濃度與nss-SO42-月平均質量濃度時間趨勢圖..53
Fig 10氣膠月平均質量濃度與nss-K2+月平均質量濃度時間趨勢圖...53
Fig 11 DIP與TP的日濃度變化時間趨勢圖..........................................61
Fig 12 TIP與TP的日濃度變化時間趨勢圖...........................................61
Fig 13 OP與TP的日濃度變化時間趨勢圖............................................61
Fig 14氣膠中不同相磷物種月平均濃度時間趨勢圖...........................64
Fig 15氣膠中不同相磷物種在不同時序中的平均濃度分佈圖...........74
Fig 16氣膠日質量濃度與DIP的日濃度分佈趨勢................................75
Fig 17氣膠日質量濃度與TIP的日濃度分佈趨勢................................75
Fig 18氣膠日質量濃度與OP的日濃度分佈趨勢.................................76
Fig 19氣膠中DIP與TIP的濃度相關性.................................................78
Fig 20氣膠中DIP與OP的濃度相關性..................................................78
Fig 21氣膠中DIP與TP的濃度相關性..................................................78
Fig 22氣膠中TIP與TP的濃度相關性...................................................78
Fig 23氣膠中OP與TP的濃度相關性....................................................78
Fig 24各相磷物種在總磷中所佔百分比例的月平均分佈圖...............81
Fig 25 Solubility月平均分佈圖...............................................................81
Fig 26 Eigenvalues of each component in the principal component analysis.....................................................................................................88
Fig 27第一主成分與第二主成分的向量分佈.......................................89

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