2010-11-032024-05-17https://scholars.lib.ntu.edu.tw/handle/123456789/679617摘要:本研究三年計畫著重於設計合成具有化學催化和生物催化的多功能中孔徑固體催化劑,並應用於在離子液體中木質纖維物質的高效率及高選擇性轉換(包括纖維素轉成葡萄糖、葡萄糖轉成5-羥甲基糠醛等)。在第一年裡,我們將致力於探討在離子液體下纖維素的分解及轉換的基礎研究(包括水解反應的各項條件),以期對此反應系統有統整了解並有益於第二、三年的研究。在第二年裡,我們將合成一種中孔洞氧化矽奈米粒子其外部含有磺酸基,而內部含有咪唑基,我們將利用此催化劑來達成纖維素直接轉換成5-羥甲基糠醛的高選擇性反應,此外,我們也會測定此異相催化劑的回收特性。在第三年裡,我們將會把具有分解纖維素能力的酵素固定於大孔洞的多功能氧化矽奈粒子中,我們將會探討物理吸附和化學鍵結兩種方法的固定情形對產率及回收率的影響。 本研究計畫提出了一個結合無機材料、有機合成、生物分子科學的新設計概念合成製備新穎多功能固態催化劑,實際應用於纖維素轉換中並探討反應機制,讓材料科學家、化學家、生物學者以者以及反應工程學者都能夠充分了解中孔徑材料在奈米材料和能源應用上的優勢和潛力。本跨領域計畫同時將給參與研究計畫的學生們很好的研究訓練。本研究計畫的執行成果將會發表於國際學術期刊、專利申請、國際會議等,對基礎科學研究及實際工業應用上均有其貢獻。 <br> Abstract: This three-year research proposal is focused on the design and synthesis of multi-functionalized mesoporous solid catalysts with chemical or enzymatic functionalities, and we will apply the synthesized catalysts to the conversion of lignocellulosic biomass (e.g. cellulose-to-glucose, glucose-to-5 hydroxymethylfurfural (5-HMF), etc.) by using ionic liquids as solvents. In the first year, we will focus on the fundamental research (e.g. reaction conditions) of the hydrolysis and conversion of cellulose in the presence of ionic liquids. The results obtained in this year will be benefit to the further cellulosic conversion in the second and third years. In the second year, we will synthesize mesoporous silica nanoparticles (MSNs) with sulfuric acid functionality on the external surface and imidazole functionality on the internal surface. We will then use this bi-functionalized nanocatalysts for the direct and highly selective cellulose-to-5 HMF conversion. In addition, we will test the recyclability of the synthesized heterogeneous catalysts. In the third year, we will immobilize cellulase (i.e. an enzyme that can convert cellulose) onto large pore MSNs. We will investigate the effects of two different immobilization methods (i.e. physical absorption and chemical binding) on the efficiency and recyclability of the cellulase-immobilized mesoporous biocatalysts. This research work represents an innovative concept that combines inorganic materials, organic synthesis, and molecular biology to synthesize new multi-functionalized solid catalysts and to apply these nanomaterials in cellulosic conversion with careful investigation into the mechanism of the reaction. We envision that this work will offer a new design principle for material scientists, chemists, and engineers to fully take advantage of the mesoporous materials as catalysts for biofuel applications. The highly interdisciplinary nature of this project will also give valuable training to the students who will be working on this work. The results obtained in this proposal will be published in international journals, patents, and conferences, which contribute to both fundamental science and practical application.中孔徑氧化矽奈米粒子離子液體木質纖纖素轉換葡萄糖5-羥甲基糠醛生質能。Mesoporous silica nanoparticlesionic liquidslignocellulosic conversionglucose5-HMFbiomass energy.設計並合成多功能中孔徑固體催化劑在離子液體中對木質纖維生質物的高效率且高選擇性地轉換成生質能源