製備酸性官能基之中孔洞矽材與奈米釕金屬中孔洞材料催化油酸酯化及硼烷氨水解脫氫之應用

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題名:	製備酸性官能基之中孔洞矽材與奈米釕金屬中孔洞材料催化油酸酯化及硼烷氨水解脫氫之應用
作者:	劉品邑;Liu, Pin-Yi
貢獻者:	化學學系
關鍵詞:	中孔洞材料;酯化;奈米金屬粒子;硼烷氨;脫氫;mesoporous material;esterification;nanoparticles;ammmonia borane;dehydrogenation
日期:	2023-07-19
上傳時間:	2024-09-19 14:44:37 (UTC+8)
出版者:	國立中央大學
摘要:	本篇論文研究分為兩部分。第一部分研究中，使用一鍋合成法，合成出具有磺酸官能基修飾的中孔洞矽材 K6SX 系列之酸性催化劑。透過粉末 X 光繞射儀、N2 吸脫附曲線、掃描式電子顯微鏡等儀器對催化劑進行鑑定，此系列催化劑因具有高比表面積、大孔洞體積和附有酸性位點等優點，將其用於催化油酸為油酸甲酯。經過一系列的實驗優化，最後以K6S10作為此實驗的最佳催化劑，產物油酸甲酯 (MO) 在油酸/甲醇=1:20，反應時間 4 小時，其轉換率達 98%，產率為 91%。此研究中，磺酸官能基修飾的中孔洞矽材表現出高催化活性及應用性。第二部分研究中，主要是利用釕奈米金屬還原在材料 (Fe3O4@SiO2@KIT-6)中，因材料具有磁性可藉由外加磁場的方式將催化劑與反應溶劑分離，使用化學還原法可有效地將 Ru NPs 快速地還原在材料中。本部分實驗將合成出來的催化劑 Ru(X)/Y% Fe3O4@SiO2@KIT-6 經由儀器鑑定後並應用在硼烷氨水解脫氫上，研究中也探討不同濃度(M/AB)、反應溫度及促進劑 NaOH 用量等優化條件，以加速硼烷氨水解脫氫反應進行。經過實驗優化，Ru(2)/10% Fe3O4@SiO2@KIT-6 於鹼性條件下表現出良好的催化活性，其轉換頻率 (TOF) 達 290.7 min-1。;This thesis consists of two parts. In the first part, sulfonic acid (-SO3H) functionalized mesoporous silica KIT-6 was synthesized and used as heterogeneous catalyst for the esterification of oleic acid. One pot co- condensation approach was used to synthesize the -SO3H functionalized 3D mesoporous silica KIT-6 using tetraethoxysilane (TEOS) and mercaptopropyltrimethoxysilane (MPTMS) as the silicon precursors. Prepared materials were characterized by SAXRD, N2 adsorption- desorption isotherm, SEM etc. –SO3H functionalized KIT-6 showed excellent catalytic activity for the esterification of oleic acid with methanol due to its high surface area, pore volume, and plenty of acidic sites in it. The effects of different parameters, such as, amount of –SO3H loading, initiator ratio, catalyst dosage and reaction temperature on the catalytic activity were also explored. KIT-6 functionalized with 10 mol% sulfonic acid groups (K6S10) was judged as the best catalyst in the optimized experimental conditions with a high conversion rate of 98% at OA/MeOH = 1:20 and a reaction time of 4 hours. In the second part, the main work is to synthesize ruthenium nanoparticles within the pores of mesoporous silica martial (Fe3O4@SiO2@KIT-6) support, and use them as the catalysts for the hydrolytic dehydrogenation of ammonia borane. The metal nanoparticles were immobilized within the support by the double agent chemical reduction method using NaBH4 and NH3BH3 as the reducing agents. The synthesized Ru (X)/Y%Fe3O4@SiO2@KIT-6 materials were characterized by PXRD, N2 adsorption-desorption isotherm, SEM etc. Catalyst Ru(2)/10% Fe3O4@SiO2@KIT-6 exhibited high catalytic activity and turnover frequency up to 290.7 min-1, activation energy of 33.82 kJ/mol.
顯示於類別:	[化學研究所] 博碩士論文

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