透過您的圖書館登入
IP:107.20.123.227
  • 學位論文

官能基化SBA-15奈米粒子在纖維素水解中之應用

Applications of functionalized SBA-15 nanoparticles in hydrolysis of cellulose

指導教授 : 鄭淑芬

摘要


目前將纖維素水解成葡萄糖比較常見的催化劑有勻相無機酸與纖維素水解酶。由於無機酸使用上會有腐蝕器材、殘酸等問題,而纖維素水解酶則有成本昂貴、反應時間長、效率低等問題。近年來固態酸觸媒開始被應用在纖維素水解反應,因為其具有易與產物分離、對器材較無傷害等優點,可以克服上述方法的缺點。 由於纖維素具有非常強的疏水性,必須使用離子液體來破壞其中的分子內與分子間氫鍵來幫助水解,但離子液體並不易與產物分離也對海洋生物具有毒性。因此為了回收離子液體,本篇研究將烷基咪唑鹽類以不同方式固定在SBA-15 奈米粒子(簡稱 SBA-15n)上。在此所使用的材料會經過X光粉末繞射、氮氣吸脫附、熱重分析、掃描式電子顯微鏡、固態核磁共振等方法鑑定。產物則由高效液相層析來鑑定。 本文章將探討纖維素水解中有無添加離子液體觸媒之影響,與其嫁接不同碳鏈長度之烷基咪唑鹽類(簡稱: SBA-15n-IL3 and SBA-15n-IL6)在磺酸化SBA-15n (簡稱: PrSA-SBA-15n)下水解纖維素的差異。 在此使用PrSA-SBA-15n作為酸觸媒,發現在有添加離子液體官能基化的SBA-15n作為實驗組的產物中有效地減少多醣生成,並顯著地提高葡萄糖產率。除此之外,還發現短碳鏈的SBA-15n-IL3較長碳鏈的SBA-15n-IL6在纖維素水解的實驗中有較高的葡萄糖產率。本論文中纖維素水解效果最佳化條件是取PrSA-SBA-15n與SBA-15n-IL3以1:1重量比混合在180 °C下反應4.5小時可得到33.0%葡萄糖產率。

關鍵字

離子液體 纖維素 水解

並列摘要


Although mineral acids and cellulases are the most common catalysts for the hydrolysis of cellulose into glucose, they possess serious problems such as reactor corrosion, waste treatment and poor recyclability for the mineral acids, and high cost, low efficiency and long reaction time for cellulases. In order to overcome the above-mentioned drawbacks, solid acid catalysts, which have the advantages of easy product separation, recyclability, and less damage to the reactor, have attracted great attention in recent years. Ionic liquids have been considered green media for dissolving cellulose by breaking the inter- and intra-molecular H-bonds of cellulose chains. In order to recycle ionic liquids, two alkylimidazolium salts were immobilized onto SBA-15 nanoparticles (abbreviated SBA-15n). The functionalized SBA-15 nanoparticles were examined with powder-XRD, N2 sorption, TGA, EA, SEM and solid-state NMR. The yield of the hydrolysis product was analyzed by HPLC. In this study, the influence of immobilized ionic liquids and the tether length of imidazolium chloride (abbreviated as SBA-15n-IL3 and SBA-15n-IL6) in cellulose hydrolysis catalyzed by PrSA-SBA-15n was studied. In this study, cellulose was hydrolyzed using PrSA-SBA-15n as the catalysts, and the presence of ionic liquid functionalized SBA-15n could reduce the production of oligosaccharides and enhance the yield of glucose. In addition, SBA-15n-IL3 has higher glucose yield than SBA-15n-IL6 in the hydrolysis of cellulose. The optimal 33.0% glucose yield was obtained after 4.5 h hydrolysis of cellulose at 180 °C in the presence of PrSA-SBA-15n and SBA-15n-IL3 in 1:1 weight ratio.

並列關鍵字

SBA-15 ionic liquid cellulose hydrolysis

參考文獻


(9) D. T. Liu, K. F. Xia, W. H. Cai, R. D. Yang, L. Q. Wang, B. Wang, Carbohydrate Polymers, 2012, 87, 1058–1064.
(7) A. I. Yeh, Y. C. Huang, S. H. Chen, Carbohydrate Polymers, 2010, 79, 192–199.
(13) A.E. Visser, R.P. Swatloski, W.M. Reichert, R. Mayton, S. Sheff, A. Wierzbicki, J.H. Davis, R.D. Rogers, Environ.Sci.Technol., 2002, 36, 2523-2529.
(2) Y. Nishiyama, J. Sugiyama, H. Chanzy, P. Langan, J. Am. Chem. Soc., 2003, 125, 14300–14306.
(3) S. Miller, R. Hester, Chem. Eng. Commun., 2007, 194, 85–102.

延伸閱讀