https://scholars.lib.ntu.edu.tw/handle/123456789/65388
標題: | 具有酸鹼官能基之中孔洞氧化矽奈米催化劑之合成及其於纖維素轉換至羥甲基糠醛之應用 Acid-Alkaline Bi-functionalized Mesoporous Silica Nanocatalysts for Direct Cellulose-to-HMF Conversion |
作者: | 彭文暉 Peng, Wun-Huei |
關鍵字: | 中孔洞奈米材料;酸鹼催化劑;離子液體;纖維素;羥甲基糠醛;mesoporous silica nanoparticles;acid-alkaline catalyst;ionic liquids;cellulose;5-hydroxymethylfurfural | 公開日期: | 2011 | 摘要: | 本研究探討了具有大孔洞與不同酸、鹼官能基之中孔洞奈米催化劑 (LPMSN, LPMSN-NH2, LPMSN-SO3H and LPMSN-Both) 之合成及其於纖維素一步轉換至羥甲基糠醛 (5-Hydroxymethylfurfural, 5-HMF) 之應用。羥甲基糠醛是非常有價值的化合物可應用於合成高分子和燃料添加物。由於能源危機的議題,發展新的替代再生能源(如生質能)已變成一個很重要的課題。將木質纖維素轉換至羥甲基糠醛,主要牽涉了三個反應步驟。(1)利用酸催化劑使多醣類降解至葡萄糖;(2)利用鹼催化劑使葡萄糖進行異構化反應轉換至果糖;(3)利用酸催化劑使果糖進行脫水反應轉換至羥甲基糠醛。果糖轉換至羥甲基糠醛的結果顯示,酸催化劑 (LPMSN-SO3H) 可以有效促使果糖的脫水反應,進而產出70.53%的羥甲基糠醛。葡萄糖轉換至羥甲基糠醛的結果顯示,具有胺官能基的鹼、酸鹼催化劑 (LPMSN-NH2 and LPMSN-Both) 可以有效促使葡萄糖的異構化反應,進而生成了13.27和13.77%的羥甲基糠醛。纖維雙糖轉換至羥甲基糠醛的結果顯示,酸催化劑 (LPMSN-SO3H) 可以有效促使纖維雙糖的水解反應,進而產生18.93%的羥甲基糠醛。纖維素轉換至羥甲基糠醛的結果顯示,酸、酸鹼催化劑 (LPMSN-SO3H and LPMSN-Both) 整體上皆約有57%的總產率,其中酸催化劑 (LPMSN-SO3H) 又可催化纖維素產生19.23%的羥甲基糠醛。我們確信合成出中孔洞氧化矽奈米催化劑可以有效的應用在纖維素一步轉換至羥甲基糠醛。 This study reports a one-pot strategy to produce 5-hydroxymethylfurfural (5-HMF, a very useful chemical for many polymers and fuel additives) with the presence of acid (SO3H), alkaline (NH2) and acid-alkaline (SO3H and NH2) bi-functionalized mesoporous silica nanoparticles with large pores (namely, LPMSN-SO3H, LPMSN-NH2 and LPMSN-NH2-SO3H, respectively) as heterogeneous solid catalysts. Due to the crisis of energy, developing an alternative energy such as biomass energy has become an important issue. To convert lignocellulosic biomass (e.g. cellulose, cellobiose and glucose etc.) into 5-HMF, there are three major steps: (1) depolymerization of polysaccharide (cellulose) into glucose with the presence of an acid catalyst; (2) isomerization of glucose into fructose with the presence of an alkaline catalyst; (3) dehydration of fructose into 5-HMF with the presence of an acid catalyst. The results for fructose-to-HMF conversion showed that the LPMSN-SO3H catalysts could promote the dehydration of fructose to 5-HMF with a high yield of 70.53%. For glucose-to-HMF conversion, the result indicated that both the LPMSN-NH2 and LPMSN-NH2-SO3H catalysts could efficiently enhance isomerization of glucose to 5-HMF with a high yield of 13.27 and 13.77%, respectively. For cellobiose-to-HMF conversion, the results pointed out that the LPMSN-SO3H catalysts could promote the hydrolysis of cellobiose and yield the maximum amount of 5-HMF (i.e., approximately 18.93%). For the cellulose-to-HMF conversion, the results indicated that both of the LPMSN-SO3H and LPMSN-NH2-SO3H catalysts exhibit the highest yield of overall products (cellobiose, glucose and 5-HMF) approximately 57%, where the LPMSN-SO3H catalysts could produce the highest yield of 5-HMF (i.e., 19.23%). We believe that the synthesized mesoporous solid catalysts are useful for one-pot production of 5-HMF from cellulose. |
URI: | http://ntur.lib.ntu.edu.tw//handle/246246/252474 |
顯示於: | 化學工程學系 |
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ntu-100-R98524077-1.pdf | 23.54 kB | Adobe PDF | 檢視/開啟 |
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