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    题名: 三維結構具羧酸官能基大孔洞中孔洞材料之合成、鑑定與酵素固定及染料吸附應用
    作者: 蔡承勳;Tsai,Chung-Hsun
    贡献者: 化學學系
    关键词: 中孔洞矽材;大孔洞;酵素固定;染料吸附;Mesoporous silica materials;Large-pore;Enzyme immobilization;Dye adsorption
    日期: 2015-07-29
    上传时间: 2015-09-23 10:50:35 (UTC+8)
    出版者: 國立中央大學
    摘要: 本論文分作兩部分:第一部分利用三嵌段共聚高分子Pluronic F127作為模板,將具有羧酸官能基的有機矽源 CES (Carboxyehtylsilanetriol Sodium Salt) 和 TEOS (Tetraethyl Orthosilicate) 作為共同矽源,並加入TMB (1,3,5-Trimethylbenzene) 在低量酸性環境且低溫 (15 o C) 下直接共聚合成法進行合成,得到大型孔洞且孔穴狀 (Cage) 的孔洞材料LP-FTC系列,其孔洞規則排列為面心立方對稱結構 (Face-Centered Cubic Structure, Fm3m),並修飾官能基達到30 % 仍具有擴大孔徑的效果,將此材料作為固定木瓜蛋白酶的載體,其吸附量最高可達895 mg/g,經活性實驗測試吸附進入孔洞內的蛋白質仍具有催化活性並且透過等溫模型的分析,得知此系列材料吸附木瓜蛋白酶之過程屬於單層吸附的Langmuir模式,動力學屬於Pseudo-second order之吸附過程,此外亦由分子內擴散模型之速率常數結果,驗證第二步驟之分子內擴散階段為吸附蛋白質之速率決定步驟。
    第二部分以F127及P123作為共同界面活性劑,以不同比例之兩種界面活性劑達到調控界面活性劑疏水端及親水端鏈段長之功效,並以TEOS及CES作為共同矽源,在酸性條件下合成孔洞結構對稱性為Im3m且修飾上不同羧酸比例之SBA-16型中孔洞材料,稱作S16C-x系列,並用此材料在鹼性環境下吸附亞甲基藍染料,利用COO-與正電型染料間的靜電吸引力,使其吸附量可達到561 mg/g;而透過酚藏花紅與酸性藍25號之吸附測試得知,鹼性環境下對於正電型染料均有良好的吸附效果,而負電型染料則反之,此外在重複利用性上亦有很好的表現。
    ;The well-ordered cubic large-pore mesoporous silicas LP-FDU-12 (Fm3m) and the cubic mesoporous silicas SBA-16 (Im3m) were both synthesized successfully via co-condensation of tetraethyl orthosilicate (TEOS) and carboxyethylsilanetriol sodium salt (CES), also functionalized with different ratio of catboxylic groups under acidic conditions, and using triblock copolymer Pluronic F127 and Pluronic P123 as template. The former were called LP-FTC-x series, and the latter were called S16C-x series.
    The LP-FTC-x were used as adsorbents for immobilization of papain and lysozyme and the S16C-x were used as adsorbents for removing of the dyes. These processes were systematically studied by varing time, initial concentration and pH. The LP-FTC-30 showed an excellent adsorption capacity for 895 mg papain per gram adsorbent, and the S16C-30 showed an excellent adsorption capacity for 561 mg methylene blue per gram adsorbent.
    The isotherm models, kinetic models and intraparticle diffusion models properties were used to analyze the immobilization mechanism of LP-FTC-x and the adsorption mechanism of S16C-x. The data were both fitted to the Langmuir isotherm model and Pseudo-Second-Order kinetics.
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