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研究生:劉志虔
研究生(外文):Zhi-Chian Liu
論文名稱:垂直梯度法與替代表面法量測乾沈降速率之結果比較
論文名稱(外文):The comparison of dry deposition rates measured by vertical gradient method and surrogate surface method
指導教授:吳義林
指導教授(外文):Yee-Lin Wu
學位類別:碩士
校院名稱:國立成功大學
系所名稱:環境工程學系碩博士班
學門:工程學門
學類:環境工程學類
論文種類:學術論文
論文出版年:2002
畢業學年度:90
語文別:中文
論文頁數:98
中文關鍵詞:替代表面法垂直梯度法乾沈降結果比較
外文關鍵詞:surrogate surface methodvertical gradient methoddry depositioncomparison of results
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  乾沈降為污染物自大氣中被自然移除的重要機制之一,然而乾沈降量測技術發展至今數十年來,仍未有一套可廣泛被接受與使用的量測方法。環境的不確定性與大氣流場的複雜性使得各量測方法在評估乾沈降的結果差異可達一至兩個數量級以上。

  本研究選擇垂直梯度法與替代表面法於同時同地進行氣固相物種(HNO3、SO2、NH3、Cl-、NO3-、SO42-、Na+、NH4+、K+、Mg2+、Ca2+)乾沈降的實地量測,期望藉此評估此兩種方法於實地採樣的適用性,以及比較其採樣結果,找出相關性及差異性。所有的採樣均在日間進行,垂直梯度法的採樣高度為2、4、7、13、24公尺,採樣時間4小時;替代表面法之乾沈降平板架設於高7公尺的平台上,採樣時間8小時。針對不同物種使用適合的收集表面,鐵氟龍濾紙收集粒狀物;浸泡過K2CO3的石英濾紙收集氣相HNO3及SO2;浸泡過檸檬酸溶液的石英濾紙收集NH3氣體。

  由替代表面法上、下表面測得之通量結果發現,固相成份由於受重力影響較顯著,因此上表面通量往往大於下表面通量,粗微粒之差異又比細微粒來得大;氣相成份則是以分子擴散之形式在大氣中運動,而分子擴散在上、下表面發生之機率相同,因此並無明顯的上、下表面通量差異,HNO3、SO2及NH3之上下表面通量比值分別為1.0、0.95及1.04。在固相成份乾沈降通量的結果比較方面,垂直梯度法測得之結果均大於替代表面法,其中以NO3-、SO42-和NH4+的差異最大,達到一個數量級,其餘成份僅Ca2+的相關性較好,R2可達0.68。是否由於濃度梯度變化過於明顯導致計算上有高估的情形還有待釐清。氣相成份之差異則不若固相成份來得大,僅HNO3有約3.5倍的差距,SO2及HNO3的相關係數R2分別為0.63及0.65。
Dry deposition is the importance mechanism by which pollutants are removed from the atmosphere. The techniques for measuring dry deposition have been developed over the years. However, there is not a standard measurement method which can be accepted and used as yet. The divergency of results in estimates of dry deposition by each measurement method approach one or two order of magnitude, due to uncertainties of environment and complexities of atmospheric flow condition.

The dry deposition rates of gaseous and aerosol species was measured in field condition simultaneously by means of vertical gradient and surrogate surface method in this study. The objectives of this study are: (1) evaluate the applicability of the two methods, (2) compare measurement results to figure out the correlativity and differentiation between the two methods. All the sampling campaign was conducted in daytime. For vertical gradient method, sampling was performed at five heights(2, 4, 7, 13, 24 m). For surrogate surface method, the dry deposition flat plates were deployed at a 7-m platform. The sampling time is 4 hr and 8 hr for vertical gradient method and surrogate surface method, respectively. Particles were collected by teflon filters; gaseous HNO3 and SO2 were absorbed by quartz filters coating K2CO3 solution; NH3 was absorbed by quartz filters coating citric acid solution.

The measurement results of surrogate surface method show that the particle deposition flux to the upper surfaces is always higher than that to the lower surfaces, especially the coarse particle, due to gravity. Nevertheless, gaseous species in atmosphere are transported mainly by molecular diffusion, and molecular diffusion occurs independently of direction. Therefore, the deposition flux of gaseous species to the upper surface is almost equal to the lower surfaces. For HNO3, SO2 and NH3 the ratio of the upper surface flux to the lower surface flux is 1.0, 0.95 and 1.04, respectively. As for the comparison of dry deposition fluxes of aerosol species, the results of measured by vertical gradient method are always larger than that measured by surrogate surface method. Of all aerosol species, the divergency of NO3-, SO42- and NH4+ is one order of magnitude and only Ca2+ is well correlated, R2 is 0.68.The divergency of gaseous species is much smaller than aerosol species. The correlation coefficient R2 of SO2 and HNO3 is 0.63 and 0.65, respectively.
目錄
第一章 前言……………………………………………………… 1
1-1. 研究緣起…………………………………………………… 1
1-2. 研究目的…………………………………………………… 2
第二章 文獻回顧………………………………………………… 4
2-1. 乾沈降簡介…………………………………………… 4
2-1-1. 乾沈降的定義……………………………………… 4
2-1-2. 乾沈降的貢獻量…………………………………… 4
2-2. 乾沈降程序…………………………………………… 6
2-2-1. 氣動傳輸…………………………………………… 7
2-2-2. 邊界層傳輸………………………………………… 7
2-2-3. 表面反應…………………………………………… 8
2-3. 收集面邊界層簡介…………………………………… 9
2-4. 乾沈降阻抗的表示…………………………………… 12
2-4-1. 氣動阻力…………………………………………… 12
2-4-2. 邊界層阻力………………………………………… 13
2-4-3. 表面阻力…………………………………………… 14
2-5. 影響乾沈降的變數…………………………………… 14
2-5-1. 氣象條件…………………………………………… 14
2-5-2. 污染物特性………………………………………… 16
2-5-3. 受體表面特性……………………………………… 17
2-6. 乾沈降的測量方法…………………………………… 19
第三章 研究方法………………………………………………… 35
3-1. 採樣點設置…………………………………………… 35
3-2. 採樣方法……………………………………………… 35
3-2-1. 垂直梯度法…………………………………… 35
3-2-1. 替代表面法…………………………………… 37
3-3. 樣品分析……………………………………………… 39
3-3-1. 濾紙採樣前處理…………………………………… 39
3-3-2. 採樣及樣品運送系統……………………………… 39
3-3-3. 濾紙採樣後處理…………………………………… 39
3-3-4. 水溶性離子成份分析……………………………… 40
3-4. 數據分析…………………………………………………… 40
3-4-1. 垂直梯度法………………………………………… 40
3-4-2. 替代表面法………………………………………… 43
第四章 結果與討論……………………………………………… 49
4-1. 垂直梯度法之量測結果………………………………………49
4-1-1. 固相成份………………………………………………… 49
4-1-2. 氣相成份………………………………………………… 50
4-2. 替代表面法之量測結果………………………………………56
4-2-1. 固相成份……………………………………………………56
4-2-1-1. 鐵氟龍表面………………………………………… 56
4-2-1-2. 噴矽膠表面………………………………………… 57
4-2-2. 氣相成份……………………………………………………63
4-3. 垂直梯度法與替代表面法之結果比較………………………67
4-3-1. 固相成份……………………………………………………67
4-3-2. 氣相成份……………………………………………………76
第五章 結論與建議……………………………………………… 82
5-1. 結論………………………………………………………… 82
5-2. 建議………………………………………………………… 83
參考文獻…………………………………………………………… 84
附錄 採樣分析品保品管作業…………………………………… 90

表目錄
表2-1. 影響乾沈降速率的因子……………………………………… 26
表2-2. 重金屬乾沈降速度與相對濕度之關係……………………… 27
表2-3. 大氣中數種常見氣體的乾沈降速度………………………… 27
表2-4. 替代表面法的設計…………………………………………… 28
表2-5. 垂直梯度法與替代表面法量測SO2乾沈降速度一覽表…… 30
表2-6. 垂直梯度法與替代表面法量測SO42-乾沈降速度一覽表…… 31
表2-7. 垂直梯度法與替代表面法量測含氮物種乾沈降速度一覽表…… 32
表2-8. 乾沈降量測技術匯整………………………………………… 33
表3-1. 現場實驗設備及儀器一覽表………………………………… 48
表3-2. 離子層析儀型號及操作參數………………………………… 48
表4-1. 不同高度之固相成份懸浮濃度……………………………………… 52
表4-2. 不同高度之氣相成份懸浮濃度……………………………………… 52
表4-3. 文獻上之SO42-乾沈降通量………………………………………… 60
表4-4. 文獻上之粒狀物乾沈降通量………………………………………… 60
表4-5. 垂直梯度法與替代表面法之固相通量結果比值…………………… 69
表4-6. 文獻上之粒狀物懸浮濃度…………………………………………… 70
表4-7. 垂直梯度法與替代表面法量測固相成份之乾沈降速度…………… 70
表4-8. 垂直梯度法與替代表面法之固相通量結果比值…………………… 77
表4-9. 垂直梯度法與替代表面法量測氣相成份之乾沈降速度…………… 77
表一 離子層析儀精密度與準確度偏差…………………………………… 96
表二 離子層析儀方法偵測極限…………………………………………… 96
表三 離子層析儀檢量線公式及R2………………………………………… 97
表四 鐵氟龍濾紙回收率…………………………………………………… 97
表五 樣品與濾紙空白值(固相)……………………………………………98
表六 樣品與濾紙空白值(氣相)………………………………………… 98

圖目錄
圖1-1. 研究架構流程圖……………………………………………… 3
圖2-1. 邊界層傳輸四種機制………………………………………… 21
圖2-2. 不同雷諾數下的受體表面邊界層…………………………… 22
圖2-3. 流體質點在邊界層內運動之情形…………………………… 23
圖2-4. 典型的邊界層厚度…………………………………………… 23
圖2-5. 乾沈降阻抗類比示意圖……………………………………… 24
圖2-6. 不同粒徑下之乾沈降速度…………………………………… 25
圖3-1. 採樣地點位置圖……………………………………………… 44
圖3-2. 鐵架及平台現場外觀圖……………………………………… 45
圖3-3. (a)乾沈降採樣平板全貌……………………………………… 46
圖3-3. (b)乾沈降採樣平板規格……………………………………… 46
圖3-4. 實驗室內樣品後處理流程圖………………………………… 47
圖4-1. 固相陰離子成份之垂直濃度剖面圖………………………………… 53
圖4-2. 固相陽離子成份之垂直濃度剖面圖………………………………… 53
圖4-3. 垂直梯度法量測固相物種之傳輸通量結果………………………… 54
圖4-4. 氣相成份之垂直濃度剖面圖………………………………………… 54
圖4-5. 垂直梯度法量測氣相物種之傳輸通量結果………………………… 55
圖4-6. 實地採樣中濾紙匣與監測儀量測SO2濃度之結果比較…………… 55
圖4-7. 鐵氟龍上下表面之固相成份乾沈降通量值………………………… 61
圖4-8. 噴矽膠上下表面之固相成份乾沈降通量值………………………… 61
圖4-9. 固相成份之上下表面通量比值……………………………………… 62
圖4-10. 鐵氟龍與噴矽膠表面之淨傳輸通量值…………………………… 62
圖4-11. 氣相成份於上下表面之平均通量值……………………………… 65
圖4-12. 氣相成份於上下表面之平均通量值(上大於下表面時)…………65
圖4-13. 氣相成份於上下表面之平均通量值(下大於上表面時)…………66
圖4-14. 垂直梯度法與替代表面法上表面之固相通量結果比較………… 71
圖4-15. 垂直梯度法與替代表面法下表面之固相通量結果比較………… 71
圖4-16. 鉀離子之兩種通量結果相關性圖………………………………… 72
圖4-17. 鎂離子之兩種通量結果相關性圖………………………………… 72
圖4-18. 鈣離子之兩種通量結果相關性圖………………………………… 73
圖4-19. Cl-之梯度變化與懸浮濃度之相關性圖…………………………… 73
圖4-20. NO3-之梯度變化與懸浮濃度之相關性圖………………………… 74
圖4-21. SO42-之梯度變化與懸浮濃度之相關性圖………………………… 74
圖4-22. Na+之梯度變化與懸浮濃度之相關性圖…………………………… 75
圖4-23. NH4+之梯度變化與懸浮濃度之相關性圖………………………… 75
圖4-24. 垂直梯度法與替代表面法上表面之氣相通量結果比較………… 78
圖4-25. 垂直梯度法與替代表面法下表面之氣相通量結果比較………… 78
圖4-26. HNO3之垂直梯度法與替代表面法上表面通量結果相關性圖…… 79
圖4-27. HNO3之垂直梯度法與替代表面法下表面通量結果相關性圖…… 79
圖4-28. SO2之垂直梯度法與替代表面法上表面通量結果相關性圖……… 80
圖4-29. SO2之垂直梯度法與替代表面法下表面通量結果相關性圖……… 80
圖4-30. NH3之垂直梯度法與替代表面法上表面通量結果相關性圖…… 81
圖4-31. NH3之垂直梯度法與替代表面法下表面通量結果相關性圖…… 81
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