內環狀官能基之中孔洞矽材應用與類沸石咪唑骨架材料包覆酵素的催化探討

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姓名

陳錫宏(Xi-Hoing Chen) 查詢紙本館藏

畢業系所

化學學系

論文名稱

內環狀官能基之中孔洞矽材應用與類沸石咪唑骨架材料包覆酵素的催化探討

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摘要(中)

本篇論文分成兩個部分：

第一部分：本實驗室成功將先前發表的新型環狀中孔洞材料XC-CAR-10應用於鑭系金屬吸附，X代表雙胺基化合物中間的碳數。此種環狀中孔洞材料利用大環分子效應提升其對鑭系金屬的吸附能力，其中3C-CAR-10能與螫合金屬離子形成六圓環穩定結構，且對於鉺離子具有相當良好的吸附能力，其飽和吸附能力約為290 µg/mg。並藉由環狀中孔洞材料中鉺離子和磷酸化蛋白質的螯合作用，使用固定化金屬離子親和層析法 (IMAC)，使磷酸化蛋白質成功被純化出來，其純化回收率可高達百分之九十。

第二部份：本實驗室先前成功將酵素置於ZIF-90的合成環境中進行從頭合成 (de novo) 反應，得到保留酵素活性的複合孔洞材料。但材料中酵素催化反應速率與天然狀態相比仍有下降，推測載體粒子大小為原因之一。故本實驗室依照文獻改良得到快速合成微米級ZIF-8的方法，並以類似條件合成奈米級ZIF-8，同時得到最佳化條件，期望能利用此兩種尺寸的ZIF-8對酵素的催化反應速率進行後續探討。

摘要(英)

The first part of my research is based on our previous report, which demonstrated the synthesis of annular-functionalized mesoporous silica with controllable size (namely, XC-CAR-10, where X represents the number of carbons in the diamines used) with a fabulous adsorption ability to metal ion owing to macrocyclic effect. Herein, we applied the annular-functionalized mesoporous silica for the lanthanide ion adsorption and further utilized the lanthanide-adsorbed mesoporous silica for phosphorylated protein purification by use of Immobilized Metal Affinity Chromatography (IMAC). It is worth noting that adsorption of 3C-CAR-10 towards ~290 µg/mg of Er3+ was achieved, and the Er3+-3C-CAR-10 showed the remarkable purification capability and selectivity of phosphorylated peptide with about 90% elution recovery.

The second part of my research is based on our previous report, which demonstrated a de novo synthesis of enzyme@ZIF-90 (Zeolitic imidazolate framework-90) and retained the enzyme activity. However, the catalytic rate of the embedded enzymes was still much slower than the native ones. One of the probable reasons of the loss in catalytic rate was likely attributed to the mass transfer owing to the particle size of carriers. Thus, the rapid syntheses of ZIF-8 with nano- and micro- size are modified and optimized in order to determine the connection between the catalytic rate of the embedded enzyme and mass transfer with size-dependent effect.

關鍵字(中)

★ 內環狀
★ 中孔洞材料
★ 磷酸化蛋白
★ 類沸石咪唑骨架材料
★ 粒徑大小
★ 催化效率

關鍵字(英)

論文目次

中文摘要 I

Abstract II

目錄 IV

圖目錄 VII

表目錄 IX

Part I 1

第一章緒論 1

1-1 中孔洞分子篩材料 1

1-1-1 簡介 1

1-1-2 發展史 2

1-1-3 應用 5

1-2 鑭系金屬近年的發展與毒性研究簡述 8

1-3 吸附理論 9

1-3-1 簡介 9

1-3-2 等溫吸附模式 10

1-3-2-1 Freundlich 等溫吸附模式 11

1-3-2-2 Langmuir 等溫吸附模式 12

1-3-3 動力吸附模型 13

1-4 蛋白質純化方法簡介 15

1-5 固定化金屬親和層析法發展與應用 17

1-5-1 載體 18

1-5-2 螫合基 18

1-5-3 金屬離子 19

1-6 磷酸化蛋白質與其純化方法 21

1-6-1 磷酸化蛋白質 21

1-6-2 磷酸化蛋白質之純化方法 22

1-7 研究動機與目標 24

第二章材料合成與鑑定部分 25

2-1 實驗藥品與設備 25

2-1-1 實驗藥品 25

2-1-2 實驗設備 26

2-2 鑑定設備與原理 27

2-2-1 實驗儀器 27

2-2-2 X射線粉末繞射儀 (PXRD) 28

2-2-3 氮氣等溫吸/脫附儀 (ASAP) 29

2-2-4 傅立葉轉換紅外線吸收光譜儀 (FT-IR) 32

2-2-5 固態核磁共振儀 (solid state NMR) 33

2-2-6 紫外線可見光吸收光譜儀 (UV-Vis) 34

2-3 中孔洞材料合成與鑑定 35

2-3-1 SBA-15 合成步驟 35

2-3-2 合成具羧酸官能基的SBA-15 36

2-3-3 移除中孔洞材料中的模板 36

2-3-4 合成具環狀結構的XC-CAR-10 37

第三章實驗部分 39

3-1 環狀結構CAR-10系列材料吸附鑭系金屬實驗 39

3-2 不同pH對鑭系金屬吸附的影響 39

3-3 環狀結構CAR-10材料與鉺離子的飽和吸附實驗 40

3-4 環狀結構CAR-10材料的動力學吸附實驗 40

3-5 磷酸化蛋白純化實驗 41

3-5-1 未吸附鉺的SBA-15材料蛋白質純化步驟 41

3-5-2 未吸附鉺的CAR-10材料蛋白質純化步驟 42

3-5-3 未吸附鉺的環狀結構CAR-10材料蛋白質純化步驟 42

3-5-4 有吸附鉺的環狀結構CAR-10材料蛋白質純化步驟 43

3-6 蛋白質純化分析方法 44

3-6-1 十二烷基磺酸鈉－聚丙烯醯胺膠體電泳 (Sodium Dodecyl Sulfate-Polyacrylamide Gel Electrophoresis, SDS-PAGE) 44

3-6-2 蛋白質濃度定量 48

第四章實驗結果與討論 49

4-1 UV-Vis吸收光譜檢量線製作 49

4-2 環狀結構CAR-10系列材料吸附鑭系金屬的實驗結果 50

4-3 不同pH值對鑭系金屬吸附的實驗結果 53

4-4 環狀結構CAR-10材料的鉺離子飽和吸附實驗結果 54

4-5 環狀結構CAR-10材料的動力學吸附實驗結果 55

4-6 蛋白質純化結果 57

第五章結論 63

Part II 64

第六章緒論 64

6-1 金屬有機骨架材料 64

6-2 類沸石咪唑骨架材料 66

6-2-1 簡介 66

6-2-2 發展史 67

6-2-3 應用 68

6-3 類沸石咪唑骨架材料-8 70

6-4 固定化酵素 (Immobilized enzyme) 71

6-5 研究動機與目標 76

第七章實驗部分 77

7-1 實驗藥品與設備 77

7-1-1 實驗藥品 77

7-1-2 實驗設備 77

7-2 鑑定儀器與原理 78

7-2-1 實驗儀器 78

7-2-2 場發掃描式電子顯微鏡 (SEM) 78

7-3 類沸石咪唑骨架材料-8 (ZIF-8) 的合成 79

7-3-1 在純水相中快速合成微米級ZIF-8 80

7-3-2 在純水相中快速合成奈米級ZIF-8 80

第八章結果與討論 81

8-1 類沸石咪唑骨架材料-8 (ZIF-8) 作為載體的條件最佳化 81

8-1-1 不同反應時間的微米級 ZIF-8 合成結果討論 81

8-1-2 不同反應時間的奈米級 ZIF-8 合成結果討論 82

第九章結論 84

第十章參考資料 85

第十一章附錄 95

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指導教授

謝發坤(Fa-Kuen Shieh)

審核日期

2015-8-26

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