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  • 學位論文

含酸或鹼基介孔二氧化矽材料的製備與其催化轉酯化反應之探討

Synthesis of Acid- or Base-Functionalized Mesoporous Silica as Catalysts for the Transesterification of Triacetin

指導教授 : 鄭淑芬
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摘要


本論文中,主要是利用兩性高分子合成具丁酸鈉官能基的介孔材料,並檢視其催化甲醇和三乙酸甘油酯轉酯化產生乙酸甲酯的反應活性。EO20PO70EO20(P123) 作為模板試劑,TEOS及不同官能基的矽烷為矽源,在酸性條件下加入氯氧化鋯,以直接合成出具不同官能基的扁平狀SBA-15介孔二氧化矽材料,官能基包含酸性的丙磺酸、苯磺酸、丁酸,以及鹼性的丁酸鈉。 為了了解不同官能基的SBA-15介孔二氧化矽材料對轉酯化反應之催化效果,以三醋酸甘油酯為模型反應,同樣以百分之十的酸或鹼不同官能基之扁平狀介孔二氧矽做催化,比較出弱鹼官能基較強酸有較強催化效率,其中丁酸鈉的催化效果最佳。而介孔材料的丁酸鈉含量越高,對三乙酸甘油酯的轉化率與對乙酸甲酯的產率有升高趨勢,百分之三十的丁酸鈉扁平狀介孔二氧化矽材料,五小時內就有百分之九十以上之三乙酸乙酯轉化率和百分之八十以上之乙酸甲酯產率。 本論文亦改變合成條件合成不同外觀的二氧化矽材料,如纖維狀的丁酸鈉二氧化矽材料,和沒有加入模板試劑的丁酸鈉二氧化矽材料,用以比較反應物擴散通道長短和有序性的影響。另外,表現最佳的催化劑之再活化和重複使用也被探討,從結果來看SBA-15 -30COONa-p可經由去質子化回復原來的活性,進行再利用。

關鍵字

介孔材料

並列摘要


Transesterification of triacetin with methanol was chosen as a model reaction to produce biodiesel. Mesoporous SBA-15 containing four different functional groups, including phenylsulfonic acid, propylsulfonic acid, carboxylic acid, and carboxylate, were used as acid and base catalysts, respectively. The catalytic performance of the materials in transesterification reaction was compared in terms of various functional groups, different loadings and different morphologies. Base functional groups were found more efficient than acid groups in catalyzing the transesterification. High conversion of triacetin and yield of methyl acetate were observed on platelet SBA-15 functionalized with large amount of carboxylate groups. The short-channels of SBA-15 facilitated the mass transfer in transesterification reaction.

並列關鍵字

mesoporous

參考文獻


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