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    题名: 二維及三維具羧酸官能基中孔洞材料之合成、鑑定及蛋白質之吸附應用
    作者: 賴晏珊;Lai,Yan-shan
    贡献者: 化學學系
    关键词: 中孔洞材料;蛋白質;羧酸官能基;mesoporous materials;protein;carboxylic acid
    日期: 2014-07-16
    上传时间: 2014-10-15 14:36:24 (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,將具有羧酸官能基的矽源CES (carboxyethylsilanetriol sodium salt) 和TEOS (tetraethyl orthosilicate) 作為共同矽源,成功地在低酸量之條件下以直接共聚合成法進行合成,分別合成具有羧酸官能基之三維立方結構之中孔洞材料及二維六角柱狀之中孔洞材料,且羧酸官能基含量可高達50%。並利用X-ray 粉末繞射、固態核磁共振光譜、等溫氮氣吸脫附、紅外線光譜儀、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。
    將上述所合成的中孔洞材料,其簡稱分別為FTC-x,結構為三維面心立方對稱結構 (face-centered cubic structure, Fm3m) 以及CS15-x系列樣品為二維六角柱狀結構 (hexagonal, P6mm),其中x=[CES/(CES+TEOS)] ,為材料當中羧酸官能基之含量,將兩種不同結構之材料應用在蛋白質分子的吸附,測試具有羧酸官能基之材料是否為可做為生化分子良好的儲存處。發現隨著溫度及pH值愈高在適當的官能基含量中皆有助於提高吸附量,並且Langmuir 等溫吸附模式比 Freundlich 等溫吸附模式更適合描述中孔洞材料吸附蛋白質之的系統,並進一步探討吸附動力學,吸附行為屬Pseudo-second order模式。
    ;Mesoporous silicas FDU-12 and SBA-15 functionalized with various contents of carboxylic acid groups were successfully synthesized via co-condensation of tetraethyl orthosilicate (TEOS) and carboxyethylsilanetriol sodium salt (CES) under acidic conditions using triblock copolymer Pluronic F127 and P123 as template, respectively. The –COOH functionalized FDU-12 (FTC-x) exhibited a cubic mesostructure, while –COOH functionalized SBA-15 (CS15-x) was hexagonal. The materials were characterized by powder X-ray diffraction (XRD), nitrogen sorption measurements, solid-state 13C and 29Si MAS NMR spectroscopy, thermogravimetric analysis (TGA), Fourier-transform infrared spectroscopy (FT-IR), scanning electron microscopy (SEM), and transmission electron microscopy (TEM). The prepared carboxylic acid functionalized cubic and hexagonal mesoporous silicas were used as suitable adsorbents for adsorption of antimicrobial protein (hen egg white lysozyme). The adsorption processes were systematically studied by varying concentration, pH and temperature. 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. Langmuir model and pseudo-second-order kinetics were well-fitted in the simulation of the adsorption behavior of protein on the prepared materials.
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