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研究生: 許雅婷
Ya-Ting Hsu
論文名稱: 具胺基之功能化中孔洞二氧化矽的合成與鑑定
Synthesis and Characterization of Amino-Functionalized Mesoporous Silica Materials
指導教授: 楊家銘
Chia-Min Yang
口試委員:
學位類別: 碩士
Master
系所名稱: 理學院 - 化學系
Department of Chemistry
論文出版年: 2007
畢業學年度: 95
語文別: 中文
論文頁數: 110
中文關鍵詞: 中孔洞二氧化矽
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  • 本論文主要在研究利用末端氧化成羧酸基的三塊狀共聚高分子P123和F127當作模板加上二氧化矽前趨物TEOS預水解的方式,以直接共聚合成法製備出不同結構的胺基功能化中孔洞二氧化矽材料。我們發現高分子末端的羧酸可促進二氧化矽前趨物的水解與縮合反應,有效克服胺基有機矽烷和TEOS水解縮合速率不同的問題,並加速模板分子與二氧化矽自組裝成三維有序結構,且增加二氧化矽縮合的程度。我們成功製備出含胺基功能化的SBA-15、KIT-5、SBA-16二氧化矽材料,並利用粉末X光繞射儀、氮氣吸脫附分析儀、熱重分析儀、固態核磁共振光譜儀、電子顯微鏡等對這些材料做結構與成分分析。其中,我們特別以具有穴狀孔洞的胺基功能化中孔洞KIT-5二氧化矽為載體來製備金奈米顆粒。從穿透式電子顯微鏡照片顯示KIT-5中的金奈米顆粒分布很均勻且大小一致,此亦反映出胺基官能基在KIT-5的孔洞表面上的分布狀況。


    We report facile syntheses of amino-functionalized large-pore mesoporous silica materials by co-condensation, using the carboxylate -terminated triblock Pluronic copolymers as structural directing agents and pre-hydrolyzed silica source of TEOS. The carboxylate end-groups were found to facilitate the hydrolysis and condensation of silica precursors and overcome the problem of the disturbed kinetics by the presence of the amino-functional silanes. The usage of the carboxylate -terminated triblock copolymers was also found to accelerate the formation of three-dimensional ordered structures of copolymer/silica hybrids in solution and enhance the degree of silica condensation of the materials. By using the carboxylate -terminated triblock copolymers, we have successfully prepared the amino-functionalized mesoporous SBA-15, KIT-5 and SBA-16 silica materials. Their elemental and structural characterizations by powder X-ray diffraction, nitrogen physisorption analysis, thermal analysis, solid-state nuclear magnetic resonance spectroscopy and electron microscopies have been performed. We also applied the amino-functionalized KIT-5 silicas to prepare the supported gold nanoparticles. The images of transmission electron microscopy revealed that the gold nanoparticles were uniform in size and were well dispersed in KIT-5 silicas. The distribution of gold nanoparticles reflected the distribution of the amino functional groups in the host KIT-5 silica materials.

    中文摘要 Ⅰ 英文摘要 Ⅱ 目錄 Ⅲ 圖目錄 Ⅵ 表目錄 ⅩⅠ 第一章 緒論 1 1-1 中孔洞二氧化矽簡介 1 1-2 界面活性劑簡介 1 1-2-1 界面活性劑的結構與種類 3 1-2-2 界面活性劑的膠體化學 5 1-2-3 雙性塊狀共聚高分子 8 1-3 二氧化矽的溶膠凝膠化學 10 1-4 中孔洞二氧化矽形成機制 15 1-5 功能化中孔洞二氧化矽的合成與應用 20 1-6 研究動機與目的 24 第二章 實驗部分 26 2-1 實驗藥品 26 2-2 界面活性劑末端氧化與具胺基功能化之 中孔洞二氧化矽的合成 27 2-2-1 將界面活性劑末端氧化反應 27 2-2-2 具胺基功能化之SBA-15的合成 27 2-2-3 具胺基功能化之KIT-6的合成 28 2-2-4 具胺基功能化之KIT-5的合成 29 2-2-5 具胺基功能化之SBA-16的合成 30 2-2-6 含胺基官能基中孔洞二氧化矽中高分子模板的移除 32 2-2-7 於具胺基功能化之KIT-5二氧化矽中製備金奈米顆粒 32 2-3 實驗鑑定儀器 33 2-3-1 X光粉末繞射儀 33 2-3-2 氮氣等溫吸脫附分析儀 36 2-3-3 熱重量分析儀 42 2-3-4 固態核磁共振光譜儀 42 2-3-5 掃描式電子顯微鏡 44 2-3-6 穿透式電子顯微鏡 46 第三章 結果與討論48 3-1 以末端氧化界面活性劑合成中孔洞二氧化矽 48 3-2 含胺基之功能化中孔洞二氧化矽的SBA-15 56 3-3 含胺基之功能化中孔洞二氧化矽的KIT-6 68 3-4 含胺基之功能化中孔洞二氧化矽的KIT-5 69 3-5 含胺基之功能化中孔洞二氧化矽的SBA-16 89 第四章 結論 103 第五章 參考文獻 105

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