以水相系統合成類沸石咪唑骨架材料(ZIF-90)及其在生物酵素催化上的應用

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王劭群(Shao-Chun Wang) 查詢紙本館藏

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化學學系

論文名稱

以水相系統合成類沸石咪唑骨架材料(ZIF-90)及其在生物酵素催化上的應用
(Water-Based Synthesis of Zeolitic Imidazolate Framework-90 (ZIF-90) with a Controllable Particle Size and its Application in Biocatalysis)

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摘要(中)

類沸石咪唑骨架材料是屬於金屬有機骨架材料的範疇，其主要是利用咪唑或是咪唑衍生
物(Im)當作有機配位體與鋅、鈷等過渡金屬(M)鍵結所形成的聚合物，結構中Im-M-Im的
鍵結角度約為145度，與天然沸石中Si-O-Si的鍵結角度大約相同，故被稱之為類沸石咪
唑骨架材料，目前主要有儲存氣體、分離混和氣體、非均相催化和藥物載體的應用。本
論文所介紹的類沸石咪唑骨架材料-90(Zeolitic Imidazolate Framework-90；ZIF-90)
已有報導指出此材料易於官能基化的特點，並具有極為優異的水熱穩定性。然而，目前
合成ZIF-90之方法大多需使用有機溶劑(如DMF)，但若大量製造ZIF-90時，所產生的廢
液將對於環境造成負擔。為了符合綠色化學之製程，此研究中，我們提供了一種於水相
系統中製備ZIF-90之方法，能夠製造出粒徑大小一致且尺寸具有均一性的ZIF-90。

摘要(英)

In zeolitic imidazolate frameworks (ZIFs), a subclass of metal–organic
frameworks (MOFs), metal ions such as Zn2+ and Co2+ are linked through the
nitrogen atoms of the deprotonated imidazolate to form neutral frameworks
and provide a tunable crystalline structure and porosity and a high internal
surface area. Additionally, the M–Im–M angle is similar to that of the
Si–O–Si angle (145o) preferred in zeolites. This fact has led to the
synthesis of a large number of ZIFs with zeolite-type tetrahedral
topologies. Therefore, ZIFs have recently attracted considerable attention
for applications in gas storage, separation of small molecules,
heterogeneous catalysis, sensors and drug delivery.
Zeolitic Imidazolate Framework-90 (ZIF-90), the main character of the
thesis, was reported to have high thermal and solvent stability. However,
most of the strategies reported so far on the synthesis of ZIF-90 have
involved the use of solvents, such as dimethyl formamide (DMF), methanol, or
other organic solvents which are also expensive, in addition to their
environmental concerns, such as toxicity, high-pollution, and waste
treatment issues. Herein, we report for the first time, a rapid and
eco-friendly strategy for the synthesis of ZIF-90 under aqueous conditions,
and thus, ZIF-90 having uniform particle sizes can be produced.

關鍵字(中)

★ 微孔洞材料
★ 類沸石咪唑骨架材料
★ 固定化酵素
★ 金屬有機骨架材料
★ 環保

關鍵字(英)

★ Microporous material
★ Zeolitic imidazolate framework
★ Immobolized enzyme
★ Metal-organic framework
★ Environmental friendly

論文目次

中文摘要 A
Abstract C
第一章緒論 1
1-1 金屬有機骨架材料 1
1-2 類沸石咪唑骨架材料 3
1-3 類沸石咪唑骨架材料-90 5
1-4 研究動機與目的 6
第二章實驗部分 8
2-1 實驗藥品 8
2-2 實驗儀器與方法 8
2-2-1 X射線粉末繞射儀 (Powder X-ray Diffractometer，XRD) 8
2-2-2 場發掃描式電子顯微鏡 (Field-emission Scanning Electron Microscope，SEM) 10
2-2-3 等溫氮氣吸/脫附儀 (Accelerated Surface Area and Porosimetry system，ASAP) 11
2-2-4 熱重分析儀 (Thermogravimetric Analyzer，TGA) 13
2-2-5 傅立葉轉換紅外線光譜儀 (Fourier Transform Infrared Spectrometer，FT-IR) 14
2-2-6 固態核磁共振儀 (Solid State Nuclear Magnetic Resonance，SSNMR) 15
2-3類沸石咪唑骨架材料的合成 16
2-3-1 純水相系統合成類沸石咪唑骨架材料-90 16
2-3-2醇水混和系統合成類沸石咪唑骨架奈米材料-90 17
第三章結果與討論 19
3-1純水相系統合成類沸石咪唑骨架材料-90 19
3-1-1 類沸石咪唑骨架材料-90(ZIF-90)的鑑定 19
3-1-2 不同濃度的乙烯基吡咯烷酮水溶液對ZIF-90合成結果之討論 22
3-1-3 不同的莫耳當量比(Zn/ICA)對ZIF-90合成結果之討論 23
3-2 醇水混和系統合成類沸石咪唑骨架奈米材料-90 24
第四章結論 28
第五章緒論 29
5-1 固定化酵素(Immobilized Enzyme) 29
5-2 過氧化氫酶(Catalase) 32
5-3 蛋白酶K(Proteinase K) 35
5-4 研究動機與目的 37
第六章實驗部分 40
6-1 實驗藥品 40
6-2 實驗儀器與方法 41
6-2-1 紫外光可見光分光光譜儀 (UV/VIS Spectophotometer) 41
6-2-2 十二烷基硫酸鈉聚丙烯醯胺膠體電泳 (SDS-PAGE) 42
6-2-3 偵測蛋白質的濃度(Bradford Assay) 46
6-2-4 偵測過氧化氫水溶液之濃度 (Ferrous Oxidation in Xylenol orange assay, FOX assay) 47
6-3 類沸石咪唑骨架-90包覆過氧化氫酶材料(CAT@ZIF-90)的合成 49
6-4 類沸石咪唑骨架-90包覆過氧化氫酶材料(CAT@ZIF-90)中蛋白質的含量 50
6-5 類沸石咪唑骨架-90包覆過氧化氫酶材料(CAT@ZIF-90)的活性測試 50
6-5添加蛋白酶(Proteinase K)的抑制測試 51
第七章結果與討論 52
7-1 類沸石咪唑骨架材料-90包覆過氧化氫酶(CAT@ZIF-90)的鑑定 52
7-2 類沸石咪唑骨架材料-90包覆過氧化氫酶材料(CAT@ZIF-90)的活性 55
7-3 添加蛋白酶(Proteinase K)的結果與討論 56
第八章結論 57
第九章參考文獻 58
第十章附錄 65

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指導教授

謝發坤(Fa-Kuen Shieh)

審核日期

2014-8-14

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