合成中空類沸石咪唑骨架材料及空間侷限性對於酵素活性影響之研究

Please use this identifier to cite or link to this item: http://ir.lib.ncu.edu.tw/handle/987654321/83259

Title:	合成中空類沸石咪唑骨架材料及空間侷限性對於酵素活性影響之研究
Authors:	孫庭謙;Sun, Ting-Qian
Contributors:	化學學系
Keywords:	金屬有機骨架材料;類沸石咪唑骨架材料;中空類沸石咪唑骨架材料;酵素;酵素活性
Date:	2020-08-04
Issue Date:	2020-09-02 15:15:35 (UTC+8)
Publisher:	國立中央大學
Abstract:	大多數固定化酵素由於材料和載體可能影響其結構變化、底物的擴散性、阻礙底物活性位點結合等等，其活性常低於未固定化之酵素。因此，具有可調性孔洞又能保護酵素避免受外界失活物質傷害的金屬有機骨架材料 (Metal-organic Frameworks, MOFs) 則替酵素固定化帶來新的發展可能。而本實驗室於2017年發表在JACS 的文章中，提出以原位創新合成方法 (de novo) 進行類沸石咪唑骨架 (Zeolitic imidazolate frameworks) 材料封裝酵素時，材料的空間限制會對酵素產生侷限性 (Spatial confinement) 之理論。同時利用尿素具有讓蛋白質結構展開而失去活性的特性，發現此材料酵素生物複合體因為侷限效應，在高濃度尿素下依然保有生物活性。為了更進一步探討材料的空間限制對於酵素活性表現的影響，如何開發具有保護功能又不會使得酵素自由度受限的材料，便成為一個重要的課題，而中空材料其內部空腔有機會解決空間限制對酵素活性的影響，因此本篇研究選擇中空金屬有機骨架材料作為研究模板。本研究利用不同的合成方法，合成中空(Hollow) 的類沸石咪唑骨架材料 Hollow ZIF-8以及 HZIF-90@ZnTA 並將酵素封裝於其中，探討酵素因空間侷限性減少所造成的活性變化，並比較兩者實驗結果。此外本研究參考最近文獻發表實驗過程，也成功在10分鐘之內利用單寧酸蝕刻，快速的製作出新型中空類沸石咪唑骨架材料 CAT@HZIF-90@ZnTA ，此研究成果結果或許能對於後續研究中空材料以及空間侷限性和酵素活性之間的關係提供一個嶄新的研究平台。;Immobilized enzymes usually showed lower enzymatic activity than free ones after applying for additional materials or supports, which might influence substrates diffusion, active sites accessibility, subunit dissociation, conformational change, especially volume-confined immobilization. It is necessary to find the potential material which overcomes the above-mentioned shortcomings and provides shell protection for embedded biomolecules to against external denaturing agents. Therefore, metal-organic frameworks (MOFs) with tunable porosity, and variable internal surface property for a targeted application, might be a suitable candidate for advanced enzyme immobilization. Recently, we reported a paper regrading an additional strength of the de novo approach by demonstrating that embedded enzymes in metal-organic frameworks (MOFs) via de novo approach remain biological functions under a wider range of reaction conditions such as urea. The enhanced stability of the of enzyme molecules arises from the confinement effects provided by MOF structure. However, the enzymatic activity is not as well as the activity of free enzymes, which might be caused by the influence of spatial confinement on the enzymatic functionality. In order to further investigate the influence of spatial confinement on the enzymatic functionality, herein, we synthesized the new hollow structure of Zeolitic imidazolate frameworks (Hollow ZIF-8 and HZIF-90@ZnTA) by using a modified approach based on a recent report , which embedded enzymes inside of void structures that mimic cytoplasmic conditions with less restricted environment. Accordingly, this part work may contribute to investigate the hollow structure material and the influence of spatial confinement on the enzymatic functionality.
Appears in Collections:	[Graduate Institute of Chemistry] Electronic Thesis & Dissertation

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