臺灣博碩士論文加值系統

本文利用共沈澱法合成一系列陰離子型Mg-Al和Zn-Al層狀無機水滑石（LDHs）；再用不同碳數之長鏈脂肪酸[CH3(CH2)nCOOH, n=10, 14, 16] 當作插層劑來改質水滑石。利用FT-IR、X-ray、 EA和 ICP等儀器鑑定這些改質過的水滑石，並且說明這些脂肪酸以成功插入水滑石層間當中。由實驗結果得知，以CH3(CH2)10COOH做為插層劑其催化劑效果最好。因此本論文研究以Mg-Al12C、Zn-Al12C水滑石當觸媒催化丙酸丁酯之反應，並且研究水滑石和動力反應行為之關係，其中包含了Mg-Al12C、Zn-Al12C、水滑石粒徑大小、反應階數和活化能。
由實驗數據求出Mg-Al12C和Zn-Al12C水滑石之反應速率式
本實驗亦有利用滲透蒸發膜來探討其滲透蒸發膜對於酯化反應的影響，實驗結果得知高分子膜對於丙酸、丁醇和水的flux大於丙酸丁酯的flux，表示丙酸丁酯大都沒有滲透過去，使的水滑石產生凝聚現象。即使如此，在整個滲透蒸發的過程當中，產物水是被移除的，因此整體催化反應速率還是被提升。

A series of organic intercalated layered anionic clays, named LDHs, were synthesized using coprecipitation reaction. The LDH was intercalated with long chain fatty acids (CH3(CH2)nCOOH, n=10, 14, 16) between these layers to synthesis the modified LDHs. These modified LDHs were characterized by FT-IR, X-ray, EA, and ICP and showed that these fatty acids incorporation within the inter-gallery space. From the experiments, the CH3(CH2)10COOH as intercalated agent has promote the esterification reaction well than others. Hence, we used Mg-Al12C/LDHs, Zn-Al12C/LDHs as catalyst to promote the reaction, and to investigate the relations between LDHs and the kinetic behaviors, including Mg-Al12C/LDHs, Zn-Al12C/LDHs, particle size, reaction order, and activation energy. The rate expression for Mg-Al12C/LDHs and Zn-Al12C/LDHs
In addition, we also used a polymer membrane to study the effect on the esterification coupling with pervaporation. The results showed the that propionic acid, n-butanol, and H2O has a larger flux than butyl propionate, implying LDHs may form aggregations due to the butyl propionate was not removed completely. Even if this, the reaction rate was still enhanced because the product, H2O, in this process was extracted.

中文摘要 Ⅰ
英文摘要 Ⅱ
誌謝 Ⅲ
總目錄 Ⅳ
表目錄 Ⅵ
圖目錄 Ⅷ
第一章 緒論 1
1.1前言 1
1.2催化反應 2
1.3無機層狀材料觸媒 5
1.4實驗簡介 8
1.5研究動機 9
第二章 文獻回顧 11
2.1水滑石的結構與性能 11
2.2水滑石的製備方法 13
2.3脂肪酸插層水滑石 15
2.4酯化反應相關文獻 16
2.5滲透蒸發膜的簡介 19
第三章 實驗部分 20
3.1實驗材料 21
3.2實驗儀器 22
3.3實驗步驟 23
3.3.1Mg-Al碳酸水滑石製備 23
3.3.2Mg-Al有機水滑石之製備 24
3.3.3Zn-Al有機水滑石之製備 25
3.3.4丙酸丁酯的合成反應 27
3.4實驗流程 28
3.4.1碳酸水滑石製備之流程圖 28
3.4.2有機水滑石製備之流程圖 29
3.4.3丙酸丁酯合成反應之流程圖 30
3.5儀器分析 31
3.5.1X-ray繞射分析(WXRD) 31
3.5.2紅外線光譜分析(FT-IR) 31
3.5.3核磁共振光譜分析(NMR) 31
3.5.4HPLC 31
3.5.5界電粒徑分析儀 32
第四章 結果討論 33
4.1有機水滑石鑑定 33
4.1.1有機水滑石之XRD鑑定 33
4.1.2有機水滑石之IR分析 35
4.1.3NMR的結果 36
4.1.4EA與ICP分析結果 37
4.1.5界電粒徑分析儀分析結果 37
4.2Mg-Al和Zn-Al水滑石的催化效果比較 38
4.2.1Mg-Al系 38
4.2.2Zn-Al系 39
4.3Mg-Al和Zn-Al十二脂肪酸水滑石的動力探討 40
4.4反應機構的推導 42
4.5加滲透蒸發膜反應的催化比較 44
第五章 結論 47
參考文獻 49
自述 117

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