具乙烷官能基與羧酸官能基之中孔洞材料的合成、鑑定及應用

Direct Synthesis, Characterization and Application of Ethane-Bridged Periodic Mesoporous Organosilicas Functionalized with Carboxylic Acid Groups

黃舒瑩(Shu-Ying Huang)

指導教授 ： 高憲明

國立中央大學/理學院/化學系/碩士(2012年)

摘要

本篇論文主要分為兩個部分：第一部分為使用非離子型界面活性劑 Brij 76 作為模板，以 1,2-bis(triethoxysilyl) ethane (BTEE) 與 carboxyethylsilanetriol sodium salt (CES) 為共同矽源，在酸性條件下以直接合成方式進行反應。可得規則排列的六角柱狀結構，其孔徑大小為 3–4 nm 之間，且可將羧酸官能基植入比例增高至 85%，其結構規則還相當良好。並藉由此合成出之中孔洞材料進行銀離子吸附實驗，探討具羧酸官能基的中孔洞材料對於銀金屬吸附的效果。
第二部分為以非離子型界面活性劑 F127 作為模板，其共同矽源為 tetraethyl orthosilicate (TEOS) 及 CES，並使用 1,3,5-trimethyl -benzene (TMB) 作為膨潤劑，成功地在酸性條件下合成出具羧酸官能基的 FDU-12 中孔洞材料，其為大孔洞的立方結構，孔洞大小約為 9 nm 左右。
本論文中所合成出的中孔洞材料皆利用 X-ray 粉末繞射、固態核磁共振光譜、熱重分析儀及等溫氮氣吸脫附等儀器鑑定材料的性質，並藉由酸鹼滴定法確定樣品中確實植入羧酸官能基的量。

關鍵字

中孔洞材料

並列摘要

The thesis is divided into two parts. First, bifunctional periodic mesoporous organosilicas (PMOs) functionlized with carboxylic acid groups were synthesized by co-condensation of 1,2-bis(triethoxysilyl) ethane (BTEE) and carboxyethylsilanetriol sodium salt (CES) under acidic conditions using polyethylene (10) stearyl ether (Brij 76) as a structure-directing agent. The maximum loading of CES contents into the pore wall without degrading the p6mm mesostructure was up to 85% (based on silicon). Well-ordered mesostructures with higher surface areas (up to 875 m2/g) and narrow pore size distributions (up to 4 nm) were obtained.
Second, well-ordered cubic mesopourous silicas FDU-12 functionalized with carboxylic acid groups were successfully synthesized by co-condensation of tetraethyl orthosilicate (TEOS) and CES under acidic conditions using Pluronic F127 as a tructure-directing agent. The maximum loading of CES contents into the pore wall without degrading the mesostructure was up to 55 % (based on silicon). Well-ordered mesostructures with higher surface areas (up to 647 m2/g) and narrow pore size distributions (up to 9 nm) were obtained.
Final, the resulting carboxylic acid functionalized PMOs were characterized by nitrogen sorption measurements, powder X-ray diffraction (XRD), solid-state 13C and 29Si NMR spectroscopy, thermogravimetric analysis (TGA), Fourier-transform infrared spectroscopy (FT-IR), scanning electron microscopy (SEM), transmission electron microscopy (TEM), and acid-base titrations.

並列關鍵字

Mesoporose

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