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http://140.128.103.80:8080/handle/310901/448
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| Title: | Al-MCM-48負載三甲氧基矽丙基胺觸媒：製備、鑑定及催化反應 |
| Other Titles: | Al-MCM-48 Supported 3-Aminopropyltrimethoxy-silane Catalysts: Preparation, Characterization, and Catalytic Reaction. |
| Authors: | 劉康文
Liu, Kang-Wen |
| Contributors: | 柯安男
Ko, An-Nan
東海大學化學系 |
| Keywords: | 催化反應;鑑定;製備;觸媒;三甲氧基矽丙基胺
Catalytic Reaction;Characterization;Preparation;Catalysts;3-Aminopropyltrimethoxy-silane;Al-MCM-48 |
| Date: | 2010 |
| Issue Date: | 2011-01-03T05:38:53Z (UTC)
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| Abstract: | Al-MCM-48(X) (X = SiO2/Al2O3 莫耳比 = 25、50 & 100)為載體經由後合成法(postsynthesis)負載三甲氧基矽丙基胺(ATMS)製成觸媒。使用X射線繞射儀、霍氏紅外線光譜儀、熱重示差熱分析儀、氮氣吸附儀、固態核磁共振儀、掃描式電子顯微鏡與穿透式電子顯微鏡等，來鑑定觸媒的結構、型態、熱穩定性、表面積、孔洞大小與分佈。結果顯示觸媒的SiO2/Al2O3莫耳比減少時，中孔結構尚屬穩定，但表面積與孔洞體積下降，而孔洞直徑與酸量增加。負載 ATMS導致表面積減少但鹼量明顯增加。 使用固定床流動反應器，研究氣態的異丙醇與異亞丙基丙酮在上述觸媒的催化下，經由氫轉移反應合成甲基異丁基酮。探討 ATMS、 SiO2/Al2O3莫耳比、反應溫度與接觸時間對反應的影響，發現 Al-MCM-48(25) 負載 ATMS 以及 ATMS/Al-MCM48（X）之X值下降時，催化活性皆較佳，顯示觸媒酸與鹼量的增加有利於催化反應。綜合實驗結果獲知製備甲基異丁基酮的最佳條件為觸媒 ATMS/Al-MCM48（25），反應溫度425℃以及接觸時間(W/F(MO)) 33.2 g?h/mol，此時異亞丙基丙酮的轉化率 35.4% 與甲基異丁基酮選擇率高達99.6%。
Al-MCM-48(X)(X = SiO2/Al2O3 mol ratio = 25、50 & 100) mesoporous molecular sieves supported 3-aminopropyltri- methoxysliane (ATMS) were prepared via postsynthesis method. These samples were characterized with various techniques of XRD, FT-IR, TGA/DTA, N2 sorption, solid state NMR, SEM, and TEM to determine their structures, morphologies, thermal stability, surface areas, pore sizes, and pore distribution. It was found that decreasing SiO2/Al2O3 mol ratio retained the stability of mesoporous structures but both the surface area and the pore volume decreased with concomitant increase of pore diameters and acid amounts. Supporting ATMS on Al-MCM-48 caused a decrease of surface area while the base amount enhanced apparently. Methyl isobutyl ketone (MIBK) was synthesized via hydrogen transfer reaction between 2-propanol (2P) and mesityl oxide (MO) in a fixed-bed, integral-flow reactor. The effect of ATMS, SiO2/Al2O3 mol ratio, reaction temperature, and contact time on catalytic results were investigated. Results showed that Al-MCM-48(25) supporting ATMS and a decrease of X of Al-MCM-48(X) exhibited better catalytic activities, which were attributed to the increase of catalyst acid and base amounts. Base on the above experimental results, the optimum conditions were ATMS/Al-MCM-48(25), 425℃, and W/F(MO) 33.2 g?hr/mol which led to the MO conversion 35.8% and MIBK selectivity 99.6 %. |
| Appears in Collections: | [化學系所] 碩博士論文
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| 098THU00065008-001.pdf | | 1653Kb | Adobe PDF | 7167 | View/Open | | 098THU00065008-002.pdf | | 19Kb | Adobe PDF | 781 | View/Open | | 098THU00065008-003.pdf | | 37Kb | Adobe PDF | 1170 | View/Open |
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