具芳香環胺基酸與內環狀結構之中孔洞材料的合成、鑑定與應用;Synthesis, Characterization and Applications of Amino Acid-modified Mesoporous Silicas and Annular Modified Mesoporous Silicas

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题名:	具芳香環胺基酸與內環狀結構之中孔洞材料的合成、鑑定與應用;Synthesis, Characterization and Applications of Amino Acid-modified Mesoporous Silicas and Annular Modified Mesoporous Silicas
作者:	蕭家騰;Hsiao,Chia-teng
贡献者:	化學研究所
关键词:	中孔洞材料;吸附劑;顯影劑;contrast agents;adsorbent;mesoporous silicas;bioconjugation
日期:	2012-08-28
上传时间:	2012-09-11 18:38:09 (UTC+8)
出版者:	國立中央大學
摘要:	本篇論文分為兩個部分：第一部分以TEOS和CES為共同矽源，界面活性劑為P123，採用直接合成法得到具有羧酸官能基的中孔洞材料CAR-10，藉由CAR-10的羧酸官能基利用交聯劑與具有芳香環的苯丙胺酸以及色胺酸產生醯胺鍵結形成產物CAR-10-Phe 和CAR-10-Trp，期望能合成出對人體無害並同時具有羧酸官能基以及芳香環雙官能基的中孔洞材料，並進一步探討具芳香環胺基酸中孔洞材料對於目標分子巴拉刈(Paraquat, PQ) 及其結構類似物 Ethyl viologen dibromide (EVB) 的吸附能力探討。第二部分為利用了具羧酸官能基的中孔洞材料CAR-10以及CAR-30，藉由交聯劑活化-COOH官能基直接與雙胺基類的分子進行醯胺鍵結，達到在中孔洞材料上修飾上內環狀結構的想法，而藉由調控內環狀的大小，以其找到一個最符合Gd金屬離子大小的結構，使之能在單位體積內負載最大量的Gd金屬離子。最後希望能將吸附Gd過後的內環狀修飾過後的中孔洞材料，測其T1、T2判斷此材料作為顯影劑材料的依據。The thesis is divided into two parts. In part one, well-ordered mesoporous silicas SBA-15 functionalized with carboxylate groups has been synthesized named CAR-X via co-condensation of tetraethoxysilane (TEOS) and carboxtethylsilanetriol sodium salt (CES) template by Pluronic P123 under acidic conditions. CAR-10 were synthetically conjugated with L-phenylalanine (Phe) and L-tryptophan (Trp), both having side chains of aromatic group, to obtain nontoxic amino acid conjugated functionalized mesoporous silica materials. The materials were used as adsorbents for the removal of the herbicide Paraquat (PQ) and its analog, ethyl viologen dibromide (EVB) in aqueous solutions. This study demonstrates that the use of amino acid-conjugated mesoporous silicas is a viable approach to reduce the PQ levels in water solutions. Such bioconjugated materials are promising candidates for new applications in the detoxification of PQ or other herbicides in clinical trials. In part two, SBA-15 type mesoporous silicas functionalized with carboxylic acid groups CAR-X were synthetically bonded with diamine compounds to modify the annular structure on materials. We attempted to control the size of macrocyclic ring to load the maximized Gadolinium ion(Gd(Ⅲ)). The relaxation time of T1 and T2 for Gd(Ⅲ) doped materials were measured by NMR. We expect this new design mesoporous silica with annular ring is able to be applied for as the new generation of MRI contrast agents or as an adsorbent for removal of other toxic metal ions.
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