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包含脂肪酸和胺的双组分水凝胶:结构、性质以及作为金属纳米颗粒合成模板的应用。

Two-component hydrogels comprising fatty acids and amines: structure, properties, and application as a template for the synthesis of metal nanoparticles.

作者信息

Basit Hajra, Pal Asish, Sen Saikat, Bhattacharya Santanu

机构信息

Department of Organic Chemistry, Indian Institute of Science, Bangalore, Karnataka, India.

出版信息

Chemistry. 2008;14(21):6534-45. doi: 10.1002/chem.200800374.

Abstract

Stearic acid or eicosanoic acid mixed with di- or oligomeric amines in specific molar ratios form stable gels in water. The formation of such hydrogels depends on the hydrophobicity of the fatty acid, and also on the type of amine used. The gelation properties of these two-component systems were investigated using electron microscopy, FTIR spectroscopy, 1H NMR spectroscopy, differential scanning calorimetry (DSC), and both single-crystal and cast-film X-ray diffraction. Results of FTIR spectral analysis suggest salt formation during gelation. 1H NMR analysis of the gels indicates that the fatty acid chains are immobilized in the gel state and when the gel melts, these chains regain their mobility. Analysis of DSC data indicates that increase in the spacer length in the di-/oligomeric amine lowers the gel-melting temperature. Two of these gelator salts developed into crystals and structural details of such systems could be secured by single-crystal X-ray diffraction analysis. The structural information of the salts thus obtained was compared with the XRD data of the self-supporting films of those gels. Such analyses provided pertinent structural insight into the supramolecular interactions that prevail within these gelator assemblies. Analysis of the crystal structure confirmed that multilayered lamellar aggregates exist in the gel and it also showed that the three-dimensional ordering observed in the crystalline phase is retained in only one direction in the gel state. Finally, the hydrogel was used as a medium for the synthesis of silver nanoparticles. The nanoparticles were found to position themselves on the fibers and produced a long, ordered assembly of gel-nanoparticle composite.

摘要

硬脂酸或二十烷酸与特定摩尔比的二胺或低聚胺在水中形成稳定的凝胶。此类水凝胶的形成取决于脂肪酸的疏水性,也取决于所用胺的类型。使用电子显微镜、傅里叶变换红外光谱(FTIR)、核磁共振氢谱(¹H NMR)、差示扫描量热法(DSC)以及单晶和铸膜X射线衍射对这些双组分体系的凝胶化特性进行了研究。FTIR光谱分析结果表明凝胶化过程中形成了盐。对凝胶的¹H NMR分析表明,脂肪酸链在凝胶状态下固定不动,而当凝胶熔化时,这些链恢复其流动性。DSC数据分析表明,二胺/低聚胺中间隔长度的增加会降低凝胶的熔化温度。其中两种凝胶剂盐形成了晶体,通过单晶X射线衍射分析可以确定此类体系的结构细节。将由此获得的盐的结构信息与这些凝胶的自支撑膜的X射线衍射数据进行了比较。此类分析为这些凝胶剂聚集体中普遍存在的超分子相互作用提供了相关的结构见解。晶体结构分析证实凝胶中存在多层片状聚集体,并且还表明在晶相中观察到的三维有序性在凝胶状态下仅在一个方向上得以保留。最后,该水凝胶被用作合成银纳米颗粒的介质。发现纳米颗粒自身定位在纤维上,并产生了凝胶 - 纳米颗粒复合材料的长而有序的组装体。

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