臺灣博碩士論文加值系統

本研究係於預混甲烷火焰，加入TTIP和HMDSO前置物以燃燒合成方式形成TiO2-SiO2之複合氧化物。實驗條件包括調整當量值、氧氮比和不同前置物濃度，從火焰觀察、火焰溫度、產物晶相和顆粒大小，探討TiO2-SiO2複合氧化物之形成機制。
在火焰觀察方面，可經由調整兩種前置物(Precursors)之不同比例得知火焰顏色變化，只受TTIP影響，火焰顏色會由藍色轉為紅色，而在燃燒反應中HMDSO並不會使火焰顏色變化。在火焰溫度方面，隨著兩前置物的添加，火焰溫度會比之前未加入前置物之火焰溫度還低，這是由於兩前置物之加入燃燒反應為吸熱反應，其中HMDSO之吸熱反應大於TTIP。
在晶相觀察方面，當固定兩前置物之流量比時，在任何當量值、氧氮比和收集高度時，燃燒合成TiO2-SiO2之複合氧化物在XRD之晶相觀察下可知TiO2-SiO2複合氧化物中之TiO2全為Rutile相，而在當量比、氧氮比和收集高度之提升時，則會造成合成TiO2-SiO2複合氧化物中Rutile的含量的增加。在TEM之觀察下，可知TiO2-SiO2複合氧化物中無定形的SiO2均勻地包覆在TiO2顆粒表面形成核殼結構，加入少許SiO2會有效抑制TiO2晶粒的成長，當量值和氧氮比之提升，而造成火焰溫度的提高，也都會使TiO2晶粒的粒徑變大，而收集高度的提高也會使TiO2晶粒的粒徑變大。

The study focuses on premixed CH4 +O2+N2 flame and adjusted ratio of TTIP/HMDSO for composing Titania/silica complex oxides (TiO2-SiO2). The experimental conditions include the equivalence ratio, the ratio of oxygen/nitrogen, the collecting height and the concentration of different precursors. The composing Titania/silica complex oxides mechanisms are studied by the flame observation, flame temperature, crystalline phase and particle sizes.
Flame color is affected by adjusting the ratio between two precursors. The main reason is that the TTIP changes the flame color from blue to red. However, HMDSO does not change the flame color. The higher equivalence ratio and the oxygen/nitrogen ratio cause higher flame temperatures. When two precursors are added, the flame temperature decreases due to both precursors causing endothermic reactions.
When the equivalence ratio, the ratio of oxygen/nitrogen and collecting height increase, the composite result of TiO2 phase of titania/silica complex oxides (TiO2-SiO2) is Rutile phase. Also, the amount of Rutile is increasing. In the aspect of particle size analysis, the higher equivalence ratio and the oxygen percentage cause temperature rise and more collision chances that lead to bigger particle size. Heterogeneous nucleation of SiO2 on the surface of TiO2 is the main reason of core-shell nanocmposites formation. In addition, the size of TiO2 nanoparticles of titania/silica complex oxides increases with the collecting height in the flame.

口試委員審定書 I
誌謝 II
中文摘要 III
Abstract IV
目錄 V
圖目錄 IX
表目錄 XII
符號表 XIII
第一章 導論 - 1 -
1.1前言 - 1 -
1.1.1 奈米材料種類及應用 - 1 -
1.1.2奈米材料特性 - 4 -
1.1.3 奈米複合材料種類及特性 - 6 -
1.1.4奈米科技產業 - 8 -
1.2研究背景 - 9 -
1.3研究目的 - 12 -
第二章 化學反應機構原理與相關文獻回顧 - 14 -
2.1 化學反應機構簡介 - 14 -
2.1.1化學反應機構的基本簡介 - 14 -
2.1.2反應機構與化學反應速率的關係 - 15 -
2.1.3甲烷燃燒化學反應機構的介紹 - 16 -
2.2 文獻回顧 - 18 -
2.2.1 二氧化鈦之相關文獻 - 18 -
2.2.2 二氧化矽之相關文獻 - 23 -
2.2.3二氧化鈦與二氧化矽複合氧化物之相關文獻 - 27 -
第三章 實驗研究方法 - 29 -
3.1實驗架構與說明 - 29 -
3.1.1實驗基本架構 - 29 -
3.1.2實驗操作參數 - 29 -
3.1.3 TTIP和HMDSO之介紹 - 31 -
3.2燃燒設備 - 31 -
3.2.1改良式預混式燃燒器 - 31 -
3.2.2 燃料輸送系統 - 32 -
3.2.3 其他儀器設備 - 33 -
3.3 儀器校正 - 34 -
3.3.1 浮球式流量計之校正 - 34 -
3.3.2 熱電偶之校正 - 35 -
3.4 實驗步驟 - 36 -
3.4.1實驗前之準備 - 36 -
3.4.2火焰溫度場之量測及現象觀察 - 37 -
3.4.3燃燒產物的收集與分析 - 37 -
第四章 結果與討論 - 38 -
4.1前置物之揮發量量測 - 38 -
4.2火焰之觀測 - 38 -
4.2.1未加入前置物之火焰觀測 - 38 -
4.2.2加入前置物之火焰觀測 - 39 -
4.3火焰溫度之分佈 - 40 -
4.3.1當量值對火焰溫度之影響 - 40 -
4.3.2氧氮比對火焰溫度之影響 - 41 -
4.3.3前置物對火焰溫度之影響 - 41 -
4.4產物晶相之分析 - 43 -
4.4.1 當量比和氧氮比對單一前置物之晶相分析 - 44 -
4.4.2調整前置物比例對產物晶相之影響 - 45 -
4.4.3當量值對產物晶相純度之影響 - 46 -
4.4.4氧氮比對產物晶相純度之影響 - 46 -
4.4.5產物收集高度對產物晶相之影響 - 47 -
4.5 產物粒徑之分析 - 47 -
4.5.1調整前置物比例對產物粒徑之分析 - 47 -
4.5.2當量值對產物粒徑之影響 - 49 -
4.5.3氧氮比對產物粒徑之影響 - 49 -
4.5.4 粉末收集高度對產物徑粒之影響 - 50 -
第五章 結論與建議 - 51 -
5.1結論 - 51 -
5.1.1前置物之揮發量量測 - 51 -
5.1.2 火焰之觀測 - 51 -
5.1.3 火焰溫度之量測 - 51 -
5.1.4產物晶相之分析 - 52 -
5.1.5產物之粒徑分析 - 52 -
5.2建議 - 53 -
參考文獻 - 54 -
圖目錄 - 61 -
表目錄 - 94 -
附錄 - 106 -
A.電子流量計之保證書 - 106 -
B.相關精密儀器的介紹 - 107 -
B.1 XRD，X-ray diffraction(X射線粉末繞射儀) - 107 -
B.2 TEM(穿透式電子顯微鏡) - 109 -

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