杂原子纳米沸石亚雏晶交错生长法构建高结晶度有序介孔材料

项目名称： 杂原子纳米沸石亚雏晶交错生长法构建高结晶度有序介孔材料

项目编号： No.21473037

项目类型： 面上项目

立项/批准年度： 2015

项目学科： 数理科学和化学

项目作者： 张亚红

作者单位： 复旦大学

项目金额： 90万元

中文摘要： 微介孔材料的复合既可以突破微孔材料孔道小的限制，又可以解决硅基介孔材料由于受到亲水性无定型孔壁组成限制而造成的水热稳定性和催化活性差的问题，是近年来催化工作者关注的热点之一。本项目针对杂原子沸石在催化低温液相氧化反应中面临的扩散和底物限制问题，提出制备高结晶有序介孔杂原子沸石材料。以杂原子纳米沸石亚雏晶为有序介孔孔壁组装单元，通过控制亚雏晶质量、后处理过程以及孔壁厚度实现纳米沸石亚雏晶受限空间交错生长，同时实现材料的介孔有序性和孔壁的高结晶性，发展制备拓扑结构、孔径厚度、杂原子骨架结构以及组成可调的有序介孔杂原子沸石新方法。同时也将获得具有异相lewis酸活性的新型介孔材料，以过氧化物为氧化剂研究和比较其催化氧化性能，最终形成一套对适合大分子催化氧化的有序介孔沸石催化剂的控制制备及其与催化活性、稳定性之间构效关系等关键科学问题的认识。

中文关键词： 分子筛；介孔材料；催化剂制备；催化氧化；构效关系

英文摘要： The combination of mesoporous and microporous materials can not only break through the channel limit of microporous material, and but also solve the poor hydrothermal stability and activity problem of silicon-based mesoporous materials caused by their hydrophilic amorphous wall, which is one of the recent research hotspots in the material and catalysis. To solve the serious diffusion and substrate scope limitation of heteroatomic zeolite in catalytic oxidation reaction, this project aims at the preparation of high crystalline and ordered mesoporous heteroatom zeolite materials. The project will focus on developing a confined-spaced intergrowth method, and achieving a new heteroatom zeolite material with two-level ordered structures. In detailed, heteroatom nano-zeolite sub-crystallites will be used as building blocks to assemble the ordered mesoporous materials. The crystallinity and size of nano-zeolite sub-crystallites, post-treatment process and thickness of mesoporous wall are well controlled to achieve the intergrowth of nano-zeolite sub-crystallites in confined space, and so to assure the high order of mesopores and high crystallinity of wall in the as-prepared mesoporous heteroatom zeolite materials. Moreover, this ordered mesoporous heteroatom zeolite materials will possess a controllable mesoporous size and wall thickness as well as microporous framework structure and composition. This project will also apply this heteroatom molecular sieve with two-level ordered structures to the catalytic oxidation of cyclic bulky molecules, and achieve the understanding of the relationship between the activity and stability of catalysts and their structures.

英文关键词： molecular sieve;mesoporous material;catalyst preparation;catalytic oxidation;relationship of structure and performance