有機物自水中揮發之研究

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趙煥平(Huan-Ping Chao) 查詢紙本館藏

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環境工程研究所

論文名稱

有機物自水中揮發之研究
(Organic Solute Emissions from Various Dilute Solutions)

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摘要(中)

本研究主要內容包括建立新的揮發模式﹐解釋環境因子對揮發之影響及分析有機物在不同環境條件下的揮發特性。傳統以二層膜理論估算有機物之揮發量存在一些較不適用或無法精確估算的情形，包括擾流狀態、較適於估算高揮發性有機物、無法由物理化學性質解釋影響揮發之因子及對純物質揮發進行估算等四部份。為克服上述問題，本研究新提出之模式改以氣體動力學中估算有機物在真空下，單位時間內撞擊1 cm2平板的分子質量所用之方程式為基礎，並將氣相參數β與擾流參數α加入方程式中；其中β為風速與大氣壓力的函數，在相同的大氣條件下β接近常數，α為有機物在液體交界與溶液中濃度比值，其為擾流強度、亨利常數與化合物分子量的函數，此模式將原本以有機物在溶液中濃度為揮發量估算之方法轉變成以有機物在交界面濃度減少來決定揮發損失。此新提出之模式稱之表面損失揮發模式(surface depletion rate-limiting, SDRL)，另由實驗的結果證明了所提出揮發模式之有效性。
對揮發之影響因子部份，證實揮發是系統能量與溶質與溶液間親和力之競爭。以此為依據，增加溫度與擾流強度會使系統能量增加從而增加揮發速率﹔加入界面活性劑或大分子有機物後，則會增加溶質與溶液間的親和力，使有機物的揮發受到抑制。對於有機物的揮發特性部份﹐以不同物化性質有機物置於不同的環境條件下﹐觀察彼此間揮發速率的差異﹐並以傳統的質量傳送理論、所提出之表面損失模式與活化能反應速率方程式解釋選擇化合物所表現出的揮發特性﹐同時也詳細探討了三種模式的適用性。

摘要(英)

This study is to develop a new volatilization model and to elucidate volatilization characteristics of different organic compounds under various environmental conditions. The gas kinetic equation for the pure substance emission under the vacuum condition was extended to be the volatilization model by adding a gas parameter β and a liquid-turbulence coefficient α. The β value of different organic compounds at the given environmental condition was found to be a constant. The α is a function of the liquid turbulence, the wind speed, the Henry’s law constant and the molecular weight of the interested compounds.
The volatilization of an organic solute from a solution is the result of two competing factors. The first consists of accelerative effects that include the thermal energy and the mixing intensity. The second consists of inhibitive effects, namely, the affinity that exists between the solute and the solution. Consequently, the solute emission rates depend on the environmental conditions (such as the liquid temperatures and the mixing intensities), wind speeds, and the solute and solution properties. The effects of the above-mentioned environmental conditions on volatilization will be discussed with the physico-chemical properties of the selected organic compounds in the section. On the other hand, the ratio of the volatilization rate constant for the organic compound to that for the reference substance depicts volatilization characteristics under different environmental conditions. It was found that Henry’s law constant for stirred liquid, wind speed and aqueous solubilities of compounds for the surfactant in the solution can determine the volatilization diversity. The results revealed that the organic compounds with the similar physico-chemical properties exhibited the nearly identical volatilization characteristic in the various environments. To select the reference compound on the basis of their physico-chemical properties is a more effective method for estimating the volatilization rates of solutes under various environmental conditions.

關鍵字(中)

★ 揮發
★ 擾流
★ 風速
★ 界面活性劑
★ 表面損失揮發模式
★ 氣體動力學

關鍵字(英)

★ kinetic gas equation
★ surfactant
★ liquid stirring
★ wind speed
★ volatilization characteristic

論文目次

目錄 ……………………………………………………………… Ⅰ
圖目錄 ……………………………………………………………… VI
表目錄 ……………………………………………………………… VIII
第一章前言.……………………………………………………... 1
1-1 研究緣起.…………………………………………………….… 1
1-2 研究目的及內容.………………………………………………. 3
第二章文獻回顧.………………………………………………... 4
2-1 基本理論介紹…………………………………………………. 4
2-1-1 勞特定律…………………………………………………. 4
2-1-2 亨利定律…………………………………………………. 4
2-1-3 二層膜理論………………………………………………. 5
2-1-4 氣體動力學觀念…………………………………………. 7
2-1-5 增溶作用…………………………………………………. 8
2-1-6 Arrhenius活化能方程式...………………………………. 8
2-2 界面活性劑……………………………………………………. 9
2-2-1 界面活性劑之定義……………………………………….. 9
2-2-2 界面活性劑之分類………………………………………. 10
2-2-3 臨界微胞濃度(CMC)…………………………………….. 10
2-2-4 界面活性劑分子結構與CMC值之間的關係…………... 11
2-2-5 界面活性劑對疏水性有機污染物的增溶現象…………. 11
2-3 ＶＯＣs之定義與特性……………………………………….. 13
2-4 蒸汽壓與亨利常數之估算……………………………………. 15
2-4-1 蒸汽壓算…………………………………………………. 15
2-4-2 亨利常數估算……………………………………………. 16
2-5 ＶＯＣs逸散量的估算……………………………………….. 18
2-5-1 高濃度VOC之揮發量…………………………………… 18
2-5-2 VOC自稀薄溶液中的揮發量…………………………… 20
2-6 ＶＯＣs在廢水廠中損失的機制……………..………………. 25
2-6-1 揮發至大氣……………………………………………….. 26
2-6-2 吸附損失…………………………………………………. 29
2-6-3 生物分解損失……………………………………………. 30
2-7 各產業常見之VOC及溢散後之處理方式………………….. 31
2-7-1 各產業常見VOC………………………………………… 31
2-7-2 溢散VOC之處理方式…………………………………… 34
2-8 影響揮發的因子………………………………………………. 36
2-8-1 溫度影響…………………………………………………. 36
2-8-2 大分子有機物與界面活性劑……………………………. 37
2-8-3 有機物溶解度……………………………………………. 38
2-8-4 反應槽的尺寸……………………………………………. 38
2-8-5 氣、液相擾流……………………………………………. 39
2-8-6 化合物蒸汽壓……………………………………………. 41
第三章研究方法與實驗設備…………………………………... 43
3-1 研究流程………………………………………………………. 43
3-1-1 選定不同亨利常數之化合物……………………………. 45
3-1-2 收集選擇化合物的物理化學性質……………………….. 45
3-1-3 選擇環境條件……………………………………………. 46
3-1-4 測定不同化合物在純物質時的揮發量………………….. 46
3-1-5 測有機物的揮發速率常數………………………………. 47
3-1-6 計算α值…………………………………………………. 48
3-1-7 求α值與其他相關參數間之關係式……………………. 48
3-1-8 探討揮發之影響因子……………………………………. 49
3-1-9 選擇參考化合物…………………………………………. 49
3-1-10 比較選擇化合物與參考化合物揮發差異……………… 50
3-1-11 推測在廢水處理時有機物之揮發量……………………. 50
3-2 實驗設備………………………………………………………. 51
3-3 實驗材料…………………………………..………………….. 53
3-3-1 有機物之物化特性………………………………………. 53
3-3-2 選擇之界面活性劑……………………………………….. 56
3-3-3 大分子有機物與高分子聚合物………………………….. 56
3-4 實驗控制條件………………………………………………….. 56
3-4-1 溫度控制………………………………………….………. 56
3-4-2 擾流強度…………………………………………………. 57
3-4-3 氣相擾動控制……………………………………………. 57
3-4-4 溶液配置濃度……………………………………………. 57
3-4-5 反應槽的尺寸……………………………………………. 58
3-4-6 反應時間…………………………………………………. 58
3-4-7 取樣時間…………………………………………………. 59
3-4-8 萃取的溶劑……………………………………………….. 59
3-4-9 分析不同化合物之檢知器………………………………. 60
3-5 實驗步驟………………………………………………………. 60
3-5-1 純物質揮發測定步驟……………………………………. 60
3-5-2 液相擾流下KOL測定步驟………………………….. 61
3-5-3 加入界面活性劑時KOL測定步驟………………..… 62
3-5-4 氣相擾流下KOL測定步驟……………………………… 62
3-5-5 模擬廢水處理廠之擾流…………………………………. 63
第四章表面損失揮發模式………………………………….…… 64
4-1 二層膜理論在估算揮發量之應用與問題…………………….. 64
4-1-1 二層膜理論的問題………………………………………. 64
4-1-2 對二層膜理論的修正方式……………………………….. 66
4-1-3 表面損失揮發模式與二層膜模式的差異性…………..… 67
4-2 純物質之揮發………………….…………………..………….. 71
4-2-1 靜止狀態下的β值………………..…………………….. 71
4-2-2 液相擾動狀態下的β值………………………………….. 73
4-2-3 不同風速下之β值………………………..……………… 74
4-2-4 同時氣、液相擾動下之β值…………………………….. 81
4-3 揮發速率常數k值在擾流下的變化特性……..…………….. 83
4-3-1 揮發速率常數在不同條件下之差異…………………… 83
4-3-2 攪拌系統下的揮發速率常數…………………………….. 88
4-3-3 攪拌對於不同揮發性化合物k值的變化……….…..….. 90
4-3-4 攪拌與靜止時質傳係數的比值(KOL/KOLo)變化………... 98
4-4 液相擾流因子α之探討……………………………………….. 100
4-4-1 α值與亨利常數之關係……………………….…………. 100
4-4-2 α值隨擾流強度之變化………………….……………….. 102
4-4-3 擾流強度對α/α0值變化……………..………………… 109
4-4-4 α值與分子量之關係…………………………………….. 110
4-4-5 α值與G、H、M之關係……………………………….. 113
第五章環境因子對揮發之影響…………………………..…….. 117
5-1 有機物揮發特性論述…….…………………..……………….. 117
5-1-1 亨利常數在揮發上之應用………………………………. 117
5-1-2 三種揮發模式對揮發特性之解釋………………………. 120
5-2 溶液性質對VOCs揮發之影響………………….…………….. 124
5-2-1 溶液溫度對VOCs揮發速率之影響…………………….. 124
5-2-2 界活性劑對VOCs揮發速率之影響…………………….. 127
5-2-3 形成微胞對揮發速率抑制情形……………………….. 130
5-2-4 VOCs在不同性質溶液之揮發特性……………………... 133
5-3 風速對於揮發速率之影響…………………………………….. 144
5-3-1 不同風速下有機物傳送係數……………..……..……. 144
5-3-2 有機物在風速與液相攪拌之KOL值變化..……….…….. 152
5-4 實際廢水處理模擬……………………………………………. 160
5-4-1 不同濃度混凝劑對有機物揮發之影響……….……..….. 160
5-4-2 Polymer濃度對揮發之影響………………………….….. 165
5-4-3 化學混凝程序中有機物的揮發特性……..…………….. 169
第六章結論與建議……………………………………………….. 171
參考文獻…………………………………………………………….. 173
附錄
附錄A亨利常數之單位換算…………………………………… 附1
附錄B純物質揮發試驗選擇化合物之蒸汽壓………………… 附4
附錄C參數計算…..…………………………………….……… 附5

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指導教授

李俊福(Jiunn-Fwu Lee)

審核日期

2003-12-8

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