具羧酸官能基之立方結構中孔洞二氧化矽的合成、鑑定及應用; Synthesis and Application of Carboxylic Acid-Functionalized Cubic Mesoporous Silica Materials

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题名:	具羧酸官能基之立方結構中孔洞二氧化矽的合成、鑑定及應用;Synthesis and Application of Carboxylic Acid-Functionalized Cubic Mesoporous Silica Materials
作者:	林于萱;Lin,Yu-hsuan
贡献者:	化學學系
关键词:	中孔洞材料;羧酸官能基;mesoporous silica;Carboxylic acid groups
日期:	2013-07-22
上传时间:	2013-08-22 11:40:41 (UTC+8)
出版者:	國立中央大學
摘要:	本論文主要是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矽源CES (Carboxyethylsilanetriol sodium salt) 和TEOS (Tetraethyl orthosilicate) 作為共同矽源，在低量酸性條件下以直接共聚合成法進行合成，可得到孔穴狀 (cage) 的孔洞，且其孔洞規則排列為面心立方對稱結構 (Face-centered cubic structure, Fm3m)，也可將羧酸官能基的莫耳比例提高至45%，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CK-x，x=[CES/(CES+TEOS)]應用在移除廢水中有機染料分子。將CK-x (x=0 - 40) 探討對亞甲基藍的吸附，其pH值愈高且官能基含量提高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CK-x吸附亞甲基藍之的系統。另外也探討四種染料分子Phenosafranine (酚藏花紅)、Methylene blue (亞甲基藍)、Orange II (橘色二號) 和Rhodamine B (羅丹明B)的吸附量，利用不同pH和材料中有無官能基之因素來探討不同染料之最佳吸附環境，並進一步探討吸附動力學。含羧酸官能基之中孔洞材料對於吸附陽離子染料 (酚藏花紅和亞甲基藍) 具有良好的表現，且四種染料吸附動力學皆屬Pseudo-second order模式。 Well-ordered mesoporous silicas CK-x [x=CES/(CES+TEOS)] functionalized with high loadings of carboxylic acid (-COOH) groups, up to 45 mol% of the silicon sites without degradation of ordered structures, have been successfully synthesized via co-condensation of Tetraethyl orthosilicate (TEOS) and Carboxyethylsilanetriol sodium salt (CES) templated with a triblock polymer Pluronic F127 at low HCl concentrations. All these materials have been 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 mesoporous CK-x materials have been used as suitable adsorbent for four different dyes (Phenosafranine、Methylene blue、Orange II and Rhodamine B). It was observed that CK-x exhibited an excellent adsorption capacity of cationic molecules. The isotherm models and kinetic models properties were analyzed to describe the adsorption behavior of prepared materials. Langmuir mode and pseudo-second-order kinetics were well-fitted in the simulation of the adsorption behavior of dyes on prepared materials.
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