利用原位創新合成概念之機械力學法合成酵素金屬有機骨架複合材料研究

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吳誓鴻(Shi-Hong Wu) 查詢紙本館藏

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化學學系

論文名稱

利用原位創新合成概念之機械力學法合成酵素金屬有機骨架複合材料研究

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摘要(中)

金屬有機骨架材料(Metal-organic frameworks, MOFs)為近幾年研究迅速崛起的孔洞材料，以金屬離子或金屬氧化物及有機配體組成內部具有空腔的結構，其比表面積與吸附性質極高且擁有特定的骨架窗口大小，所以擁有諸多應用，其中一項即為酵素固定化之基板。
近幾年興起一種原位創新合成(de novo)方法，本實驗室於2015年首先發表CAT@ZIF-90即以MOFs的前驅物與酵素同時於水溶液內合成，縝密包覆酵素特點除了擁有大小篩選性，更在2017年研究發表指出被包覆的酵素有空間限制反摺疊(unfolding)現象，具有傳統吸附型固定化無法達到的優勢。
然而受限於大部分MOFs屬於熱溶劑法合成，使酵素在合成過程會失去活性；能夠水相合成的MOFs也以ZIF系列為主，其窗口(aperture)約為3.5Å使大部分底物無法進入。為了將酵素包覆拓展至其他MOFs，我們提出全新包覆的概念：利用短時間及幾乎無溶劑的機械球磨法能合成金屬有機骨架材料的優點，將酵素一同添加達到包覆效果。本研究以葡萄糖甘酶(BGL)與UiO-66-NH2的組合為範本，突破了傳統酵素固定化的方法，以機械球磨方式成功將BGL包覆到UiO-66-NH2中，並測定催化產物的生成保有活性，也因為UiO-66-NH2的耐酸性及孔洞篩選性質，使得BGL@UiO-66-NH2在蛋白質水解酶protease這樣的大分子環境中，能阻擋BGL被水解而保持催化活性。
此結果提供了Enzyme@MOFs創新合成方式，不再侷限於水相合成系統。期待在未來能同時結合機械球磨法與水相合成法，以原位創新合成概念合成更多類型的酵素金屬有機骨架複合材料，並對酵素做進一步研究。

摘要(英)

Metal organic frameworks(MOFs) composed by metal ions and organic linkers are porous materials which were emerging and developed rapidly in recent years. Many applications are contributed by high porosity and specific aperture of its structure. One of the MOF applications is used as the platform for enzyme immobilizations.
Recently, a de novo approach was used for encapsulating enzymes into MOFs materials, our group successfully preformed that biocomposites have been generated under aqueous and mild condition by encapsulating catalase, enzymes for hydrogen peroxide hydrolysis, into zeolitic imidazolate framework-90 (CAT@ZIF-90). By this approach, enzyme could not only be protected in protease solution by aperture size limitation but also reduce unfolding by MOF structure confinement which difficultly achieved by adsorption immobilization.
In addition to ZIFs with 3.5Å aperture which limited penetrability of large substrates, most of MOF materials are synthesized by solvothermal ways under harsh conditions such as organic solvent and high temperature etc. in which the biological activity of enzyme is hardly maintained. To this end, we thought out of the box and proposed another concept that takes the method of mechanochemical approach with advantages of rapidly time and almost non-solvent to immobilize enzymes inside of MOFs. We demonstrated a mechanochemical method for the facile preparation of biocomposites by embedding -glucosidase, enzymes for disaccharide hydrolysis, in a Zr-MOF analog, UiO-66-NH2 and also determined the apparent biological activity. UiO-66-NH2 has a large aperture and high acid resistance, thus demonstrating potential for size-shielding against protease as well as maintaining biological function. Thus, this study provides an alternative route for encapsulating enzymes into MOFs, especially for biocomposites that are difficult to obtain under mild aqueous conditions.

關鍵字(中)

★ 金屬有機骨架材料
★ 酵素固定化
★ 機械力化學
★ 葡萄糖苷酶

關鍵字(英)

★ metal-organic framework
★ enzyme immobilization
★ mechanochemistry
★ beta-glucosidase

論文目次

目錄
中文摘要 I
Abstract III
目錄 V
圖目錄 VIII
表目錄 XI
第一章緒論 1
1-1 金屬有機骨架材料之概述 1
1-1-1金屬有機骨架材料(Metal-organic Frameworks) 1
1-1-2 鋯金屬有機骨架材料(Zirconium based Metal-organic Framework) 3
1-1-3 UiO-66及其衍生物簡介 4
1-2 酵素固定化(Enzyme immobilization) 7
1-3 研究動機與目的 10
第二章實驗部分 12
2-1 實驗藥品 12
2-2 實驗儀器與原理 13
2-2-1實驗合成與鑑定儀器項目 13
2-2-2 微量型快速球磨機 14
2-2-3 X-ray繞射儀 (Powder X-ray Diffraction, PXRD) 15
2-2-4 掃描式電子顯微鏡 (Scanning Electron microscope, SEM) 17
2-2-5 紫外/可見光光譜儀 (UV/visible Spectrophotometer) 18
2-2-6 十二烷基硫酸鈉聚丙烯醯胺膠體電泳 (SDS-PAGE) 18
2-2-7 等溫氮氣吸/脫附儀 20
2-2-8 熱重力分析儀 23
2-2-9 共軛焦螢光顯微鏡 23
2-2-10 葡萄糖苷酶 (-glucosidase, BGL)與催化活性測定原理 24
2-2-11 蛋白酶 (protease) 26
2-3 實驗步驟 27
2-3-1 機械球磨法合成UiO-66-NH2 27
2-3-2 機械球磨法合成BGL@UiO-66-NH2(一步法) 27
2-3-3 機械球磨法合成BGL@UiO-66-NH2(兩步法) 28
2-3-4 測定BGL@UiO-66-NH2的BGL含量-Bradford assay 28
2-3-5 測定BGL@UiO-66-NH2的催化產物生成量 30
2-3-6 BGL@UiO-66-NH2的蛋白質凝膠電泳分析 32
2-3-7 FITC標記BGL之步驟 33
第三章結果與討論 35
3-1 不同球磨頻率與時間對UiO-66-NH2之合成晶形探討 35
3-2 球磨合成BGL@UiO-66-NH2之粉末繞射鑑定與催化活性探討 36
3-2-1 催化活性之判斷依據-速率常數kobs 36
3-2-2 One-pot合成BGL@UiO-66-NH2之表徵與活性 38
3-2-3 Two steps合成BGL@UiO-66-NH2之表徵與活性 40
3-3 BGL@UiO-66-NH2之熱重分析探討 44
3-4 BGL@UiO-66-NH2之等溫氮氣吸/脫附探討 45
3-5 BGL@UiO-66-NH2之共軛焦顯微鏡探討 47
3-6 BGL@UiO-66-NH2在蛋白酶環境之催化活性探討 49
第四章結論與未來展望 51
第五章參考資料 52

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指導教授

謝發坤

審核日期

2019-1-18

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