三維具羧酸及胺基官能基大孔洞中孔洞材料之合成、鑑定與蛋白質吸附應用

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白家蕙(Chia-Hui Bai) 查詢紙本館藏

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論文名稱

三維具羧酸及胺基官能基大孔洞中孔洞材料之合成、鑑定與蛋白質吸附應用

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摘要(中)

本論文主要是分別利用三嵌段共聚高分子Pluronic F127及 Pluronic P123作為模板，成功地在低酸量之條件下以直接共聚合成法進行合成，分別合成具有羧酸與胺基官能基之三維立方結構之大孔洞SBA-16。
合成方面分為兩大部分，第一部分是以F127及P123當作模板，以tetraethyl orthosilicate (TEOS) 和CES (carboxyethylsilanetriol sodium salt) 當作共同矽源，在低酸量的條件下以直接共聚合成法合成出具大孔洞的中孔洞材料LP-S16C-x，且羧酸官能基含量可高達40%。第二部分同樣是以F127及P123當作模板，利用tetraethyl orthosilicate (TEOS) and 3-aminopropyl)triethoxysilane (APTES)為共同矽源，合成出含有胺基官能基的LP-S16N材料，其胺基官能基含量僅可達到5 %。並利用X-ray 粉末繞射、固態核磁共振光譜、等溫氮氣吸脫附、熱重分析儀、穿透式電子顯微鏡及掃描式電子顯微鏡等儀器鑑定材料的結構，同時也鑑定官能基含量對孔洞性質的影響。
應用方面，將分別不同的官能基之材料應用在蛋白質分子的吸附，測試是否為可做為生化分子良好的儲存處。發現具胺基官能基的材料有助於提升牛血清白蛋白的吸附量，而具羧酸官能基的材料對於血紅素的吸附效果較好，並且套入等溫吸附模式來描述中孔洞材料吸附蛋白質的系統，並進一步探討吸附動力學。接著將材料應用到選擇性蛋白質吸附，探討在不同的pH值環境下牛血清白蛋白、血紅素、溶菌酶，所產生的選擇性吸附效果。

摘要(英)

The well-ordered cubic large-pore mesoporous silicas SBA-16 (Im3m) were successfully synthesized via co-condensation under acidic conditions using Pluronic F127 and Pluronic P123 as template.
One is carboxylic acid functionalized, synthesized by co-condensation of two different silane precursors, that is, tetraethyl orthosilicate (TEOS) and carboxyethylsilanetriol sodium salt (CES), under acidic condition using F127 and P123 as template. The maximum loading of CES contents into the pore wall without degrading the Im3m mesostucture was up to 40%. These materials were denoted as LP-S16C-x, where x is the mole ratio of carboxylic acid groups. The other is synthesized by co-condensation of tetraethyl orthosilicate (TEOS) and 3-aminopropyl)triethoxysilane (APTES) under same condiction like LP-S16C-x, and is called LP-S16N.
In this study, the synthesized materials were characterized by powder X-ray diffraction(XRD), nitrogen sorption measurement, thermogravimetric analysis (TGA), 13C CP-MAS NMR, 29Si MAS NMR, fourier transform infrared spectrometer (FTIR), transmission electron microscopy (TEM), scanning electron microscopy (SEM).
In adsorption experiment, the prepared carboxylic acid and amine functionalized cubic mesoporous silicas were used as suitable adsorbents for protein adsorption (bovin serum albumin and hemoglobin). The adsorption processes were carefully studied with differernt factors. The prepared adsorbents showed an excellent adsorption capacity due to well-ordered pore structures. The isotherm models and kinetic models properties were analyzed to describe the adsorption behavior of the prepared materials. Moreover, We studied the selectively protein adsorption of bovin serum albumin, hemoglobin, and lysozyme for a range of different pH values.

關鍵字(中)

★ 大孔洞
★ 中孔洞矽材
★ 蛋白質吸附

關鍵字(英)

★ large-pore
★ mesoporous silica
★ protein adsorption

論文目次

中文摘要 I
Abstract II
目錄 IV
圖目錄 VIII
表目錄 XII
第一章緒論 1
1-1中孔洞二氧化矽分子篩 1
1-2界面活性劑之簡介 4
1-2-1界面活性劑結構與種類介紹 4
1-2-2共聚高分子 (Block copolymer) 6
1-2-3微胞的形成與結構 7
1-2-4界面活性劑與矽氧化物的交互作用 10
1-3 表面修飾官能基之中孔洞材料 13
1-4相關文獻回顧 16
1-4-1中孔洞材料SBA-16合成與介紹 16
1-4-2表面修飾羧酸官能基之中孔洞材料 17
1-4-3表面修飾胺基官能基之中孔洞材料 21
1-4-4中孔洞材料吸附蛋白質之簡介 27
1-5研究動機與目的 29
第二章實驗部分 30
2-1實驗藥品 30
2-2實驗步驟 31
2-2-1合成具羧酸官能基之LP-S16C-x 31
2-2-2以硫酸溶液裂解孔洞中的模板 32
2-2-3合成具胺基官能基之LP-S16N 32
2-2-4以後修飾法合成具胺基官能基之LP-S16N 33
2-2-5以溶劑萃取法移除LP-S16N孔洞中的模板 33
2-2-6蛋白質檢量線之製作 33
2-2-7中孔洞材料在不同反應時間及pH值下之蛋白質吸附實驗 34
2-2-8中孔洞材料在不同pH值及初始濃度之蛋白質吸附實驗 35
2-2-9蛋白質釋放實驗 35
2-2-10不同pH值下之選擇性蛋白質吸附實驗 35
2-3 實驗設備 36
2-3-1實驗合成設備 36
2-3-2 實驗鑑定儀器 36
2-4 鑑定方法 38
2-4-1 同步輻射光束線 (NSRRC Beam Line) 38
2-4-2 X射線粉末繞射 (Powder X-Ray Diffractometer) 39
2-4-3 氮氣吸脫附等溫曲線、表面積與孔洞特性之鑑定 40
2-4-4傅立葉紅外線吸收光譜儀 (Fourier Transform Infrared Spectrometer；FTIR) 45
2-4-5 熱重分析儀 (Thermogravimetric Analyzer；TGA) 46
2-4-6低真空掃描式電子顯微鏡 (Scanning Electron Microscope；SEM) 48
2-4-7穿透式電子顯微鏡 (Transmission Electron Microscope；TEM) 49
2-4-8 固態核磁共振儀 (Solid State Nuclear Magnetic Resonance；Solid State NMR) 51
2-4-9紫外光-可見光光譜儀 (UV / Vis Spectrometer) 59
第三章結果與討論 61
3-1合成不同矽源比例之中孔洞材料 61
3-1-1 LP-SBA-16系列XRD 61
3-1-2 13C CP/MAS NMR鑑定 63
3-1-3等溫氮氣吸脫附鑑定 66
3-1-4 29Si MAS NMR鑑定 70
3-1-5 FT-IR紅外線光譜 74
3-1-6 TGA 熱重分析 76
3-1-7 SEM影像 78
3-1-8 TEM影像 81
3-1-9 表面電位 84
3-2中孔洞材料吸附蛋白質之吸附實驗 86
3-2-1在不同反應時間吸附蛋白質之效果 86
3-2-2蛋白質初始濃度對中孔洞材料吸附之影響 88
3-2-3蛋白質之釋放實驗 93
3-3 中孔洞材料吸附蛋白質後之性質鑑定 95
3-3-1 XRD繞射圖譜 95
3-3-2 等溫吸脫附圖 98
3-3-3 吸附等溫模式 103
3-3-4動力學吸附探討 115
3-3-5分子內擴散模型之探討 120
3-4選擇性蛋白質吸附實驗 122
第四章結論 124
參考文獻 125
第五章附錄 136
5-1 實驗步驟 136
5-1-1利用LP-S16C-x 吸附銅金屬製備銅金屬顆粒 136
5-1-2利用LP-S16C-x 對4-Nitrophenol進行催化還原反應 136
第六章結果與討論 137
6-1 LP-S16C-x-Cu-0.0175之XRD結果 137
6-2 TEM影像 139
6-3 LP-S16C-x-Cu-y催化還原4-Nitrophenol 140

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指導教授

高憲明(Hsien-Ming Kao)

審核日期

2016-7-29

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