臺灣博碩士論文加值系統

微粒粒徑分布及散光係數深受相對濕度影響。而目前廣受應用之積分散光儀(integrating nephelometer)，在將其應用於高濕度環境之測定過程中，為避免水分附著於受測腔內壁，均將受測氣流加熱。此操作方式將使微粒失去水分，造成微粒粒徑分布向小粒徑方向偏移，並進而低估散光係數測值。由於我國台灣地區經常出現高相對濕度之情形，在受測大氣微粒樣品之相對濕度受積分散光儀加熱而減少的過程中，微粒所含水份亦隨之減少而使其粒徑變小，進而影響其散光係數之測值結果。有鑑於此，探討大氣微粒於積分散光儀內相對濕度變化過程所生之散光係數測值影響，為提供大氣微粒真實散光係數之重要研究課題。
本研究為釐清相對濕度對氣膠微粒散光係數之影響，分別就：大氣微粒在不同相對濕度下之吸濕成長性質、建置氣膠散光係數計算模式、以及求解積分散光儀中發生之散光係數變化等三大面向加以探討。其中大氣微粒吸濕成長性質測定係利用串聯式微分型移動度分析系統(Tandem Differential Mobility Analyzer, TDMA)配合不致稀釋大氣微粒樣品之微粒濕控系統加以測定。氣膠散光係數計算模式，則納入微粒之粒徑分布及足以反映微粒成分變化之成長熱力學函數予以建置，並配合自行製備微粒之測定結果予以檢討。在定量檢討積分散光儀中發生之散光係數變化上，則應用計算流體力學求解積分散光儀內受加熱影響所導致之流場及溫度變化，並據以計算各種不同粒徑、組成成分分布之微粒，在積分散光儀中發生之散光係數變化。
本研究成果顯示：大氣微粒中原落於狹窄粒徑範圍的部分，在吸濕成長後呈雙峰型態粒徑分布，顯現其組成成分之外部混合性質。在本研究探討之粒徑介於53至200 nm之大氣微粒，其粒徑成長較大之微粒個數比例及成長因子均隨起始粒徑增加而增加。硫酸銨與硝酸銨純物質微粒散光係數隨濕度變化之情形，均與本研究所建置之散光係數計算模式獲致結果相符。積分散光儀樣品氣流之相對濕度變化主要發生於加熱區，此區與樣品微粒受光照射之有效體積大抵重疊，因此積分散光儀內部之加熱機制，即使樣品氣流中微粒發生可觀之粒徑分布變化，進而影響其散光係數測值。當入流氣流相對濕度較高，使其在積分散光儀中受熱後仍未越過氣流中所含微粒結晶點時，微粒散光係數低估程度係隨入流氣流相對濕度減少而緩和減少。在入流氣流相對濕度為90%時，不同成分微粒散光係數低估程度落於41%至72%之間。當入流氣流相對濕度較低，使其在積分散光儀中受熱後越過氣流中所含微粒結晶點時，微粒散光係數低估程度即因微粒粒徑突減而更形顯著，此低估程度亦隨相對濕度減少而減少。

Size distribution and scattering coefficients of particles are significantly influenced by relative humidity (RH). The scattering coefficient change caused by particles’ size change is especially important for environments with high relative humidity. In order to quantify the effects of RH change on scattering coefficients of particles, the hygroscopic growth of particles and size change occurring in scattering measurement instrument, integrating nephelometer, are investigated in this study.
Hygroscopic growth of particles of different sizes and the resultant size distribution changes were observed as a function of the relative humidity (RH). A particle generation device, relative humidity module, and a Tandem Differential Mobility Analyzer system were set up to measure the particle size distributions under different RH conditions. Adopting Nafion as an RH adjusting module, the aerosol hygroscopic observations were successfully performed without the interference caused by blending sample stream with humidified air. The measured deliquescence humidity of model compounds, NaCl and (NH4)2SO4, agree with the theoretical values reported by other investigators. The particle growth factor is enhanced around the RH of 70%. In addition, particle size distribution behaves as two split groups of particles with the RH greater than 76%. The average growth factors of hygroscopic ambient particles in Taiwan are similar to those reported elsewhere. There are several hygroscopic salt compositions in ambient aerosols, (NH4)2SO4 is the most abundant one. Observed particle deliquescence behaviors showed limited alternation of organics on particle growth at higher RH.
Nephelometer is widely used to measure the scattering coefficient of ambient particles. The sample stream is heated in nephelometer to avoid the possible formation of water film on the inner wall of nephelometer. The relative humidity change of heated sample stream also alters particles’ size distribution. In order to clarify the meaning of scattering coefficient measured by nephelometer, it is necessary to quantify the difference of measured and true scattering coefficient of ambient particles. In this study, the flow field, temperature field, and relative humidity field of nephelometer’s test chamber are solved by computational fluid dynamics. The corresponding scattering coefficient changes are calculated for three different types of particles including typical urban particles, rural particles, and marine particles. For sample stream with 90% relative humidity, the measured particle scattering coefficient is 63.5%, 41.7%, and 72.5% lower than the ambient particle scattering coefficient for typical urban particles, rural particles, and marine particles, respectively. For typical urban particles and rural particles, the differences between measured and ambient particle scattering coefficients are larger in environments with higher relative humidity. The differences range from 23.8% to 63.5% for typical urban particles, from 8.4% to 41.7% for rural particles. For marine particles, this difference is about 70%, and not sensitive to relative humidity.

第一章　引言 1
1.1 研究背景 1
1.2 研究目標 2
第二章　文獻回顧 3
2.1 微粒散光係數影響機制 3
2.11 微粒散光之微觀物理模式 4
2.1.2 微粒散光現象巨觀解析 8
2.2 相對濕度對微粒粒徑分布之影響 9
2.2.1 微粒粒徑隨濕度變化測定方法 9
2.2.2 大氣微粒粒徑隨濕度變化現象 12
2.3 氣膠微粒散光係數測定方法探討 14
2.4 微粒散光係數計算模式 18
2.4.1 機制型模式 18
2.4.2 迴歸型模式 25
第三章　研究方法與實驗設備 31
3.1 濕度對微粒吸濕成長因子影響 33
3.1.1 研究流程 33
3.1.2 實驗設備 36
3.1.3 測定方法 44
3.1.4 測定結果計算 48
3.2 相對濕度對微粒群散光係數影響 50
3.2.1 研究流程 52
3.2.2 實驗設備 52
3.2.3 測試方法 61
3.2.4 測定結果應用於模式評估 62
3.2.5 大氣微粒散光係數計算模式建立及檢討 66
3.3 不同濕度下積分散光儀測值意義解析 74
3.3.1 研究流程 76
3.3.2 模式工具 76
第四章　結果與討論 83
4.1 濕度對微粒吸濕成長因子之影響 83
4.1.1 自行製備微粒測試 83
4.1.2 大氣微粒吸濕成長因子測定結果 88
4.2 相對濕度對微粒群散光係數影響 107
4.2.1 濕度對微粒粒徑分布之影響 107
4.2.2 濕度對微粒散光係數之影響 119
4.2.3 散光係數計算模式應用於大氣微粒 124
4.3 不同濕度下積分散光儀測值意義解析 129
4.3.1 積分散光儀邊界條件界定 129
4.3.2 積分散光儀流場及溫度模擬 131
4.3.3 相對濕度分布換算 140
4.3.4 微粒散光係數變化量計算 142
4.3.5 不同濕度下微粒散光係數變化量計算 152
第五章　結論與建議 155
5.1 結論 155
5.2 建議 156
參考文獻 158
圖目錄
圖2.1　積分散光儀示意圖 17
圖3.1　研究架構圖 32
圖3.2　濕度對微粒吸濕成長因子影響之資料流向圖 34
圖3.3　濕度對微粒吸濕成長因子影響之研究流程圖 35
圖3.4　相對濕度對微粒群分徑個數濃度影響之實驗設備圖 38
圖3.5　相對濕度對微粒吸濕成長因子影響氣膠流經設備示意圖 46
圖3.6　濕度對微粒粒徑分布及散光係數影響之資料流向圖 51
圖3.7　濕度對微粒粒徑分布及散光係數影響之研究流程圖 53
圖3.8　濕度對微粒粒徑分布及散光係數影響之實驗設備圖 58
圖3.9　濕度與大氣微粒散光係數關係解析之研究流程圖 68
圖3.10　大氣微粒散光係數計算模式建立及檢討之資料流向圖 69
圖3.11　不同濕度下積分散光儀測值意義解析之資料流向圖 75
圖3.12　不同濕度下積分散光儀測值意義解析之研究流程圖 77
圖4.1　100 nm純鹽類氯化鈉及硫酸銨微粒潮解曲線 84
圖4.2　100 nm硫酸銨及硝酸銨內部混合微粒潮解曲線 87
圖4.3　三維粒徑分布隨濕度變化圖 91
圖4.4　大氣微粒潮解曲線 97
圖4.5　微粒成長因子隨粒徑及相對濕之分布曲面 105
圖4.6　硫酸銨微粒在不同濕度下之粒徑分布 109
圖4.7　硝酸銨微粒在不同濕度下之粒徑分布 110
圖4.8　Glutaric acid微粒在不同濕度下之粒徑分布 112
圖4.9　硫酸銨、硝酸銨內部混合微粒在不同濕度下之粒徑分布 113
圖4.10　硝酸銨、Glutaric acid內部混合微粒在不同濕度下之粒徑分布 115
圖4.11　(4.1)式模式殘項之機率分布 128
圖4.12　積分散光儀內部納入求解結構示意圖 129
圖4.13　積分散光儀解析用之網格分布示意圖 130
圖4.14　正常操作狀態積分散光儀流場速度向量圖 132
圖4.15　正常操作狀態積分散光儀流場等速度線分布圖 135
圖4.16　正常操作狀態積分散光儀等溫度線分布圖 138
圖4.17　典型都會微粒在不同濕度下之粒徑分布 145
圖4.18　典型都會微粒在不同濕度下之表面積分布 146
圖4.19　郊區微粒在不同濕度下之粒徑分布 148
圖4.20　郊區微粒在不同濕度下之表面積分布 149
圖4.21　海鹽微粒在不同濕度下之粒徑分布 150
圖4.22　海鹽微粒在不同濕度下之表面積分布 151
表目錄
表2.1　微粒成長熱力學函數 23
表2.2　大氣微粒散光係數計算模式比較 29
表3.1　濕度對微粒吸濕成長因子探討使用儀器 36
表3.2　濕度對微粒粒徑分布及散光係數影響之研究變因 54
表3.3　受測微粒組成物質基本性質 56
表3.4　濕度對微粒粒徑分布及散光係數影響研究使用儀器 56
表3.5　大氣微粒散光係數計算模式建立及檢討之觀測變數 68
表3.6　大氣微粒散光係數計算模式建立及檢討所需儀器 70
表3.7　標準k-e紊流模式閉合常數 81
表3.8　本研究流場及溫度場求解所用之收斂條件 82
表4.1　較吸濕微粒及較不吸濕微粒之粒徑成長因子 102
表4.2　MOUDI採得微粒樣品之水溶性成分含量 103
表4.3　本研究所得微粒成長熱力學函數與類似研究比較 106
表4.4　各濕度微粒粒徑分布差異t檢定之P值 116
表4.5　微粒粒徑分布模式值及實測值差值之95%信賴區間 118
表4.6　自行產製微粒綠光散光係數測定結果 120
表4.7　各濕度微粒散光係數差異t檢定之P值 121
表4.8　微粒散光係數模式值及實測值差值之95%信賴區間 123
表4.9　本研究所得大氣微粒散光係數模式 125
表4.10　散光係數模式值及實測值關係變異數分析表 127
表4.11　各溫度案例溫度場邊界條件 131
表4.12　各案例溫度場相應相對濕度分布 141
表4.13　典型都會微粒粒徑分布模式參數值 143
表4.14　郊區微粒粒徑分布模式參數值 147
表4.15　海鹽微粒粒徑分布模式參數值 149
表4.16　來自各地區微粒之散光係數測值低估程度 153

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