博碩士論文 102223044 詳細資訊




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姓名 吳征戰(Cheng-Chan Wu)  查詢紙本館藏   畢業系所 化學學系
論文名稱 探討不同官能基在金屬有機骨架材料上的配位基對UiO-66在硝酸水相合成的影響
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摘要(中) 金屬有機骨架材料(Metal Organic Frameworks, MOFs)主要由金屬原子(或者團簇)與有機分子配位形成聚合物,這類聚合物具有孔洞性質,目前此類材料主要應用於儲存氣體、分離混合氣體、催化反應劑和藥物載體;而合成大部分金屬骨架材料合成方法為水熱法(Hydrothermal)或熱溶劑法(Solvothermal),其最主要差別即反應中添加水或者有機溶劑,尤其熱溶劑法所使用的溶劑多為有毒物質,例如:二甲基甲醯胺(Dimethylformamide;DMF),所以本篇論文將介紹使用水作為溶劑合成UiO-66;其為金屬有機骨架材料一種,其組成的架構為鋯(Zirconium)或鉿(Hafnium)團簇與十二有機配位體形成的架構,而有機配位分子是對苯二甲酸(Terephthalic acid)。這類本篇所使用的方法為使用對苯二甲酸衍生化的對苯二甲酸二甲酯(Dimethyl terephthalate)在硝酸底下與四氯化鋯(Zirconium chloride)高溫微波反應(140 °C;10 分鐘)後即可合成出材料。但若以對苯二甲酸作為起始物,且使用相同條件卻是得到非結晶性(Amorphous)的材料,作者對於此差異現象極為感興趣,故以本篇論文做些假設並對此做一系列的實驗作為探討。
摘要(英) Metal organic frameworks (MOFs), which are three-dimensional porous materials consisting of metal ions and organic linkers. Because of their high surface-area porosity, MOFs have been studied for use in gas storage/separation/purification, catalysis and drug carrier. Most synthesis mythologies are hydrothermal or solvothermal, which are different from adding water or organic solvent in reaction. Especially, solvothermal is using organic solvents which most of them are toxic and non-eco-friendly such as dimethylformamide. So in this study, we are going to introduce how to synthesis UiO-66 in water-acid phase. UiO-66 is one of MOFs which reticular structure is consist of zirconium or hafnium clusters and they coordinate with twelve organic linker molecules. The coordinate linkers are terephthalic acid or similar coordinate linkers, such as fumaric acid, could get iso-reticular structure. In this work, we used dimethyl terephthalic acid, derivatization of terephthalic acid, react with zirconium chloride under high temperature and microwave radiation condition (140 °C; 10 minutes). However, amorphous crystalline material was obtained by terephthalic acid as linkers in the same condition. So we interested in the distinct phenomenon and resorted to a hypothesis and further study with a series experiments.
關鍵字(中) ★ 金屬有機骨架材料
★ 水相合成
★ 官能基化配體
關鍵字(英) ★ Metal-Organic Framework
★ Water-base synthesis
★ UiO-66
論文目次 中文摘要 I
Abstract II
目錄 III
圖目錄 IV
表目錄 VI
第一章 緒論 1
1-1 金屬有機骨架材料(Metal-Organic Framework) 1
1-2 鋯金屬有機骨架材料(Zirconium-Organic Framework) 2
1-3 UiO-66焦點(UiO-66 Review) 4
1-4 實驗動機(Experiment Motivation) 6
第二章 實驗部分 9
2-1 實驗藥品 9
2-2 實驗儀器介紹 10
2-2-1 微波輔助合成儀(Microwave-Assisted Instrument) 10
2-2-2 X射線粉末繞射儀(Powder X-ray Diffraction) 12
2-2-3 熱重分析儀(Thermo-gravimetric analyzer; TGA) 14
2-2-4 等溫氮氣吸脫附儀(Nitrogen ad/desorption isotherms) 15
2-2-5 傅立葉轉換紅外線吸收光譜儀(FT-IR) 18
2-2-6 固態核磁共振儀(Solid Nuclear Magnetic Resonance;SNMR) 19
2-3 實驗步驟 21
2-3-1 熱溶劑法合成UiO-66 21
2-3-2 硝酸溶液下微波輔助合成UiO-66 21
2-3-3 硝酸溶液下微波輔助合成UiO-66-X 22
第三章 結果與討論 24
3-1 微波輔助合成UiO-66 24
3-2 詳細結構鑑定硝酸微波輔助合成的UiO-66 27
3-3 硝酸微波合成中加入添加劑(Acetic acid) 31
3-3 探討合成機制 34
3-4 不同官能基在配位鍵結強度的計算 43
3-5 結論 47
參考文獻及附錄 48
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指導教授 謝發坤(Fa-Kuen Shieh) 審核日期 2016-1-22
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