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研究生：	陳彥伯 Chen, Yen-Po
論文名稱：	正丁醇蒸氣在帶高電量SiO2及TiO2奈米微粒上之非均勻相核凝現象 Heterogeneous nucleation of n-butanol vapor on highly charged nanoparticles of SiO2 and TiO2
指導教授：	陳進成 Chen, Chin-Cheng
學位類別：	碩士 Master
系所名稱：	工學院 - 化學工程學系 Department of Chemical Engineering
論文出版年：	2009
畢業學年度：	98
語文別：	中文
論文頁數：	129
中文關鍵詞：	非均勻相核凝、過飽和度、流動型雲霧室、帶高電量微粒、凝結電荷放大系統、正丁醇、二氧化矽、二氧化鈦
外文關鍵詞：	heterogeneous nucleation, supersaturation, flow cloud chamber, highly charged nanoparticles, condensation charge magnification system, n-butanol, SiO2, TiO2
相關次數：	點閱：102 下載：1
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奈米微粒因為粒徑很小有著和巨觀材料性質不同的差異。在大氣中因為天然及人為因素而產生相當多的奈米微粒，並且因為大氣中的自然輻射種種因素使微粒帶電，使微粒因為電荷影響改變蒸氣凝結的能力。
本研究以電噴霧法製備二氧化矽(SiO2)及二氧化鈦(TiO2)奈米微粒，配合凝結電荷放大系統，讓單一粒徑的15nm、20nm、25nm的奈米微粒，帶1-3個單位負電量，並以流動型雲霧室來探討帶高負電量SiO2及TiO2微粒在正丁醇蒸氣中所引起之非均勻相核凝機構。
粒徑效應方面二氧化矽(SiO2)及二氧化鈦(TiO2)微粒無論在過飽和水蒸氣或是正丁醇蒸氣中，臨界過飽和度的值皆隨著粒徑減小而提升，定性上與理論相符合，定量上則有一定的差距。
電荷電量效應方面，SiO2及TiO2微粒因為帶電量的提升，所需之臨界過飽和度降低，粒徑越小帶電量的影響越趨於明顯，其中本實驗以15nm的微粒所需的臨界過飽和度因為電荷量改變最為明顯。至於兩種不同微粒的臨界過飽和度值比較，實驗結果和先前論文相符合，TiO2微粒所需的臨界過飽和度值皆小於SiO2微粒。
實驗值和理論值的差距，推測可能原因為負離子附著在微粒表面之上，成為核凝程序發生之中心位置(site)，降低所需之臨界過飽和度。

Nanoparticles may have properties different from the bulk due to their small size. In the atmosphere, there are ions generated as a result of cosmic ray and natural radiolysis, and aerosol particles become charged due to the attachment of these ions. Charge on particle can affect the condensation of vapor .
In this study, an electrospray aerosol generator was used to generate SiO2 and TiO2 nanoparticles and highly charged nanoparticles were prepared by condensation charge magnification system. A flow cloud chamber(FCC) was employed to examine the effects of amount of charges each particle carried on the critical supersaturation requried for the condensation of the supersaturated n-butanol vapor on SiO2 and TiO2 nanoparticles with a diameter ranging from 15 nm to 25 nm, and each carrying 1 up to 3 unit negative charges.
The results show that the experimental critical supersaturation(Scr) decreases with increasing particle size, at a rate in reasonable agreement with that predicted by Fletcher’s version of Volmer’s theory of heterogeneous nucleation.
For SiO2 and TiO2 particles, the experiment results show that Scr decreases because of the charge effect. For 15 nm SiO2 particles, an obvious charge effect on Scr is observed, and the effect is much stronger than the prediction. This phenomenon may be caused by negative ion attached on particles surface to reduce the barrier of nucleation.

中文摘要..................Ⅰ 
英文摘要.................II 
誌謝....................III 
目錄..................IV 
表目錄...............VII 
圖目錄............... IX 
符號說明............XIV 

第一章 緒言 1 
1 簡介................1 
2 非均勻相核凝文獻回顧............5 
3 研究目標.......................9 

第二章 理論分析 14 
1 電噴霧法 ...............14 
2 電暈放電.................19 
3 核凝理論.................22 
4 不可溶中性微粒ΔG之計算...................24 
4.1 不可溶帶電微粒ΔG之計算...................29 
5 雲霧室中溫度、密度與過飽和度分佈.................30 

第三章 實驗系統及操作 34 
1 實驗系統.................34 
1.1 微粒產生器................38 
1.2 微粒電荷中和器...............42 
1.3 電力篩選器............44 
1.4凝結電荷放大系統..............49 
1.5 流動型雲霧室...............52 
1.6 超細微粒凝結核計數器..............55 
1.7 掃瞄式粒徑分析儀...........57 
2 實驗藥品.................59 
3 實驗步驟.................60 
3.1 電噴霧系統操作...............60 
3.2 去除效率實驗...............62 
4 理論模擬臨界過飽和度............67 

第四章 實驗結果及討論 68 
1 電噴霧法製備之微粒與微粒粒徑分析........69 
1.1 製備SiO2微粒之最佳操作條件及粒徑分析.......69 
1.2製備TiO2微粒之最佳操作條件及粒徑分析......71 
1.3單一粒徑SiO2和TiO2微粒之粒徑分析..... .......73 
2 凝結電荷放大系統實驗............77 
3 空白實驗..................85 
4 微粒去除效率實驗結果.............87 
5 帶高負電量微粒實驗值與理論值比較.......93 
6 帶高負電量微粒對臨界過飽和度之影響.......101 
7無機微粒SiO2和TiO2臨界過飽和度實驗值之比較........110 
8蒸氣分子對帶高電荷量微粒之臨界過飽和度的影響......113 

第五章 結論與未來研究方向 117 
1 結論................117 
2 未來研究方向...............120 
參考文獻 ...............121 


表目錄 

1 本實驗室歷年探討水蒸氣在有機與無機微粒上之非均勻相核凝...............11 
2 本實驗室歷年探討正丁醇蒸氣在有機與無機微粒上之非均勻相核凝..............12 
3 本實驗室歷年探討正壬烷蒸氣在有機與無機微粒上之非均勻相核凝............................12 
4 本實驗歷年探討水蒸氣在帶高電量奈米微粒上之非均勻相核凝之探討...............13 
5 本實驗探討正丁醇在帶高電量奈米微粒上之非均勻相核凝之探討..................13 
1 微粒之電荷Boltzmann平衡分佈表......43 
1 粒徑範圍5~25nm的微粒之slip correction以及帶一個、二個或三個單位電量之電移動度...................84 
2 雲霧室上下板液膜溫度與產生之最大過飽和度及最大過飽和度處之溫度關係表.....................92 
3 實驗所得帶高電量SiO2微粒臨界過飽和度........97 
4 實驗所得帶高電量TiO2微粒臨界過飽和度........97 
5 帶高負電量SiO2微粒在水蒸氣下之理論值與實驗值......98 
6 帶高負電量TiO2微粒在正丁醇蒸氣下之理論值與實驗值..99 
7 SiO2與TiO2微粒在正丁醇蒸氣中臨界過飽和度比較....112 
8 SiO2帶高電量微粒在水及正丁醇蒸氣中實驗值之臨界過飽和度比......................116 
9 SiO2帶高電量微粒在水及正丁醇蒸氣中之臨界過飽和度實驗值.....................116 

圖目錄 

1 液體吸附在不同微粒表面示意圖.......8 
2 液體吸附於混相式表面之活性位置示意圖.......8 
1 電噴霧示意圖.........................15 
2 液體錐內之受力情況....................15 
3 毛細管末端流體在不同電壓操作下形成不同操作模式.....16 
4 cone-jet mode崩潰機制示意圖..........17 
5 正電暈放電示意圖............21 
6 負電暈放電示意圖..............21 
7 微粒表面上之液體胚核................25 
8 平衡蒸氣壓(Pea)，蒸氣壓(a)，溫度(T)，過飽和度(S)，蒸氣密度(ρv)、載流氣體密度(ρc)及混合氣體密度(ρt, ρt=ρv+ρc)與無因次高度之關係............33 
1 奈米微粒之非均勻相核凝現象實驗裝置圖........37 
2 注射幫浦外觀圖................38 
3 電噴霧系統配置圖..............41 
4 加裝電暈放電裝置後之電噴霧系統配置圖........41 
5 微粒中和器之構造圖............42 
6 電力篩選器(3071)外觀圖.........47 
7 電力篩選器(3080)外觀圖.........48 
8 電力篩選儀之內部構造圖........48 
9 同軸噴射混合器外觀圖..........50 
10 同軸噴射混合器內軸外觀圖.............50 
11 同軸噴射混合器內部構造示意圖.........51 
12 流動型雲霧室之構造圖..........54 
13 超細微粒凝結核計數器構造圖...........56 
14 掃瞄式粒徑分析儀構造圖........58 
15 以He-Ne雷射觀察雲霧室中核凝現象示意圖......66 
1 電噴霧法製備SiO2微粒時尚未經過篩選前的粒徑分佈圖...70 
2 電噴霧法製備TiO2微粒時尚未經過篩選前的粒徑分佈圖...72 
3 單一粒徑之15nm SiO2奈米微粒的粒徑分佈圖....74 
4 單一粒徑之20nm SiO2奈米微粒的粒徑分佈圖....74 
5 單一粒徑之25nm SiO2奈米微粒的粒徑分佈圖....75 
6 單一粒徑之15nm TiO2奈米微粒的粒徑分佈圖....75 
7 單一粒徑之20nm TiO2奈米微粒的粒徑分佈圖....76 
8 單一粒徑之25nm TiO2奈米微粒的粒徑分佈圖....76 
9 帶高電量之單一粒徑20nm SiO2微粒的粒徑分佈圖.......81 
10 帶高電量之單一粒徑15nm SiO2微粒的粒徑分佈圖.....81 
11 帶高電量之單一粒徑25nm SiO2微粒的粒徑分佈圖.....82 
12 帶高電量之單一粒徑25nm TiO2微粒的粒徑分佈圖.....82 
13 帶高電量之單一粒徑20nm TiO2微粒的粒徑分佈圖.......83 
14 帶高電量之單一粒徑15nm TiO2微粒的粒徑分佈圖.......83 
15 正丁醇蒸氣中帶不同電量SiO2微粒空白實驗進出口比值與粒徑關係..............86 
16 正丁醇蒸氣中帶不同電量TiO2微粒空白實驗進出口比值與粒徑關係..............86 
17 帶不同負電量之25nm SiO2微粒在過飽和正丁醇蒸氣中之去除效率與過飽和度關係圖..............89 
18 帶不同負電量之20nm SiO2微粒在過飽和正丁醇蒸氣中之去除效率與過飽和度關係圖..............89 
19 帶不同負電量之15nm SiO2微粒在過飽和正丁醇蒸氣中之去除效率與過飽和度關係圖..............90 
20 帶不同負電量之25nm TiO2微粒在過飽和正丁醇蒸氣中之去除效率與過飽和度關係圖............90 
21 帶不同負電量之20nm TiO2微粒在過飽和正丁醇蒸氣中之去除效率與過飽和度關係圖..............91 
22 帶不同負電量之15nm TiO2微粒在過飽和正丁醇蒸氣中之去除效率與過飽和度關係圖.............91 
23 粒徑為15nm帶兩個單位負電量之SiO2微粒在正丁醇蒸氣中去除效率隨過飽和度變化之關係圖...........94 
24 SiO2微粒在正丁醇蒸氣下之臨界過飽和度實驗值.....95 
25 TiO2微粒在正丁醇蒸氣下之臨界過飽和度實驗值.....95 
26 帶高負電量SiO2微粒在正丁醇蒸氣下之理論值與實驗值比較.............................100 
27 帶高負電量TiO2微粒在正丁醇蒸氣下之理論值與實驗值比較..............................100 
28 胚核及電荷在微粒上之分佈情形................104 
29 正丁醇蒸氣之核凝臨界過飽和度理論值與帶高電量SiO2微粒之實驗值之比較.........................105 
30 正丁醇蒸氣之核凝臨界過飽和度理論值與帶高電量TiO2微粒之實驗值之比較.........................106 
31 負離子附著在微粒表面上之情形.................107 
32 負離子在微粒表面之核凝程序..............108 
33 電荷在微粒上之影響情形...............109 
34 正丁醇蒸氣在帶高負電量SiO2、TiO2不可溶奈米微粒上之臨界過飽和度圖.......................112 
35 中性SiO2微粒在三種工作液中過飽和度比實驗值與理論值對粒徑變化圖....................115
                                    

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