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    题名: 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
    作者: 白家蕙;Bai,Chia-Hui
    贡献者: 化學學系
    关键词: 大孔洞;中孔洞矽材;蛋白質吸附;large-pore;mesoporous silica;protein adsorption
    日期: 2016-07-29
    上传时间: 2016-10-13 12:46:20 (UTC+8)
    出版者: 國立中央大學
    摘要: 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。 
    ;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.
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