功能性複合中孔洞材料的製備與應用

Preparation and Applications of Functional Nanocomposite Mesoporous Materials

林興安(Xing-An Lin)

指導教授 ： 楊家銘

國立清華大學/理學院/化學系/碩士(2007年)

https://doi.org/10.6843/NTHU.2007.00357

摘要

本篇論文主要是在製備新穎的多功能化中孔洞二氧化矽。我們應用硫酸處理法將中孔洞SBA-15的二氧化矽中孔洞開啟，進行中孔表面疏水化改質後，再以低溫鍛燒的方式將微孔開啟，形成中孔表面與微孔洞表面分別具有親水與疏水兩種不同性質的功能化SBA-15。論文第一部分中，我們將微孔表面修飾上雙鍵官能基，並使之進一步與鈀金屬鹽類形成錯合物，在經過高溫還原後，便在微孔中形成鈀金屬奈米粒子，我們並發現此奈米複合鈀催化劑可在不具有其它配位基的條件下催化Heck反應的進行。第二部分中，我們在不堵塞SBA-15的中孔洞的情形下，於微孔中嵌入氧化鈦、氧化鋅及氧化鐵三種不同金屬氧化物，再將金奈米粒子沉積在金屬氧化物上，而形成新穎的奈米金催化劑。我們發現無論是在含水氣或不含水氣的情況下進行一氧化碳氧化反應，這些樣品都具有極佳的催化活性。最後在第三部分中，我們在不堵塞中孔洞的情形下於微孔中嵌入氧化鐵，利用樣品中孔洞表面原本的疏水性質加上氧化鐵暴露於中孔洞表面所表現的表面性質等雙重作用，進行cytochrome c的吸附。我們發現此樣品表面的雙重作用能夠在接近中性pH （pH 6.5）的條件下增強對cytochrome c的吸附能力並達到最大吸附量。

關鍵字

中孔洞二氧化矽 ； 微孔洞 ； 金奈米粒子 ； 一氧化碳氧化

並列摘要

In this thesis, we report the preparations of novel multifunctional mesoporous silica materials. We apply the treatment of sulfuric acid to vacate the mesopores of mesoporous SBA-15 silica, followed by the surface functionalization of the mesopores to become hydrophobic. After low-temperature calcination to vacate the micropores, the resulting bifunctional SBA-15 silica has hydrophilic micropores as well as hydrophobic mesopores. In the first part of the thesis, we further graft the micropores with vinyl functional groups, which can then react with palladium salts and trap them in the micropores. After further reduction reaction, metallic palladium nanoparticles in the micropores of SBA-15 are formed. The palladium-containing nanocomposite catalyst show catalytic activity for the Heck reaction without any ligand present in the reaction mixture. In the second part, we selectively incorporate metal oxides, including titanium oxide, zinc oxide and iron oxide, into the micropores of SBA-15 without blocking the mesoporous channels, followed by the deposition of gold nanoparticles on the top of the metal oxides. The resulting novel gold nanocomposite catalysts are active for CO oxidation with or without the presence of moisture. Finally, the SBA-15-based nanocomposite with iron oxide in the micropores and hydrophobic mesopores is applied for cytochrome c adsorption. We find that the novel adsorbent with double surface interactions can achieve the highest adsorption amount near neutral pH condition (pH 6.5).

並列關鍵字

mesoporous silica materials ； SBA-15 ； CO oxidation ； cytochrome c

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