以杯芳烃为模板剂合成高性能(杂原子)中孔分子筛研究

中文摘要

本项目合成出了一系列水溶性全磺化杯芳烃衍生物，并在以这些物质为模板剂探索合成结构新颖的介孔分子筛材料方面开展了大量的研究；合成出了含有锆及稀土元素钕的新型介孔分子筛材料，并对其进行了表征和催化性能的研究；采用大分子化合物与表面活性剂组合形成的二元复合模板剂，合成出了多种具有特殊形貌的介孔分子筛材料；通过在空心球型介孔材料的表面组装纳米开关的方法，制得了一种具有PH值响应的"智能开关"的新型介孔材料；实验发现：在合成介孔材料时掺入一定量的钕，不仅能够得到一种具有良好的室温氧化性能的催化剂，同时，得到的介孔材料具有空心球的特殊形貌；通过使用大分子物质（PVA,F127,PEG等）作为辅助模板剂，使用DADD/DDA等作为主模板剂，可以合成出一系列具有球形、空心球形、树叶型等形貌特异的介孔材料，这些材料的合成和深入研究，对于进一步认识和理解介孔材料的形貌的形成和机理具有十分重要的意义；具有纳米智能开关的介孔空心球的成功制备，为介孔材料在药物的储存和缓释方面的应用打下了良好的基础；研究工作在JACS发表后，立即被Nature Materials选为Highlight文章加以介绍；

英文摘要

In this project, we synthesized a series of water-soluble sulfonated calix [n] arene derivatives, which were then used as the template to exploit the synthesis of mesoporous material with new structure. Firstly, we prepared new mesoporous materials containing Zr and Nd, studied their catalytic activity. Secondly, we synthesized the mesoporous zeolite with special morphology by using macromolecule and surfactant as the dual template. Thirdly, we constructed a pH-driven supramolecular nanovalve with the prepared mesoporous materials. We found that during the synthesis of mesoporous materials, the incorporation of Nd can not only yield an oxidative catalyst with decent activity at room temperature, but also yield a special morphology of hollow sphere. By using the macromolecule (e.g. PVA, F127, PEG) as the aid-template and DADD/DDA as the main-template, we synthesized a series of mesoporous materials with the morphology of sphere, hollow sphere, and leaf-type. In-depth investigation will play an important role in understanding the formation process and mechanism of the mesoporous materials. The construction of the supermolecular nanovalve helps to push the research work on the mesoporous hollow spheres in the application of drug-storage and release. This work was published in JACS, and then selected as the Highlight in Nature Materials.