A study on biocatalysts immobilized in nanospace

纳米空间固定化生物催化剂的研究

• 批准号: 13650839
• 负责人: ONAKA Makoto
• 金额: $ 2.3万
• 依托单位: The University of Tokyo
• 依托单位国家: 日本
• 项目类别: Grant-in-Aid for Scientific Research (C)
• 财政年份: 2001
• 资助国家: 日本
• 起止时间: 2001 至 2002
• 项目状态: 已结题
• 来源: https://kaken.nii.ac.jp/grant/KAKENHI-PROJECT-13650839/
• 关键词: Mesoporous silica; Enzyme lipase; Immobilized enzyme; Biocatalyst system; Green chemical process; Sol-gel process; Long-chain carboxylic acid; Esterification; グリーンケミストリー; 生体触媒; メソ多孔体シリカ

The objectives of the research are to prepare stable biocatalyst systems encapsulated in nanoporous, hydrophobic space and to apply them to green-chemical organic synthesis in organic media. As a nanoporous material, we chose highly-ordered mesoporous silica with a pore size of 6-9 nanometer in diameter, which was prepared using Si(OEt)_4, and triblockcopolymer. The internal surface of the mesoporous silica was then modified by silane coupling agents having amino, hydroxyl, and carboxylic functional groups. Lipase enzyme was immobilized in the chemically-modified mesoporous silicas, and applied to esterification between an equimolar amount of carboxylic acid and alcohol under ambient conditions. We compared biocatalysis between lipase encapsulated in the chemically modified mesoporous silicas and commercially available lipase supported on Celite. We found several advantages: 1) Our lipase system showed 20 times as high biocatalysis in esterification as the conventional lipase, 2) the volume of our immobilized lipase is much smaller than that of Celite-supported lipase, 3) the stability of the lipase in mesoporous silica is much superior, and 4) no leaching of lipase from the pores of chemically-modified mesoporous silica was observed.

该研究的目的是制备封装在纳米多孔疏水空间中的稳定生物催化剂系统，并将其应用于有机介质中的绿色化学有机合成。作为纳米多孔材料，我们选择了由Si(OEt)_4和三嵌段共聚物制备的孔径为6-9纳米的高度有序介孔二氧化硅。然后用具有氨基、羟基和羧基官能团的硅烷偶联剂对中孔二氧化硅的内表面进行改性。将脂肪酶固定在化学改性的介孔二氧化硅中，并在环境条件下应用于等摩尔量的羧酸和醇之间的酯化反应。我们比较了封装在化学改性介孔二氧化硅中的脂肪酶和负载在硅藻土上的市售脂肪酶之间的生物催化作用。我们发现了几个优点：1）我们的脂肪酶系统在酯化方面的生物催化能力是传统脂肪酶的20倍，2）我们的固定化脂肪酶的体积比硅藻土支撑的脂肪酶小得多，3）脂肪酶在酯化过程中的稳定性介孔二氧化硅要优越得多，并且4)没有观察到脂肪酶从化学改性介孔二氧化硅的孔中浸出。