具有三维有序结构的多级孔分子筛的设计合成与构效关系研究

项目名称： 具有三维有序结构的多级孔分子筛的设计合成与构效关系研究

项目编号： No.21306151

项目类型： 青年科学基金项目

立项/批准年度： 2014

项目学科： 化学工业

项目作者： 陈汇勇

作者单位： 西北大学

项目金额： 25万元

中文摘要： 具有三维有序结构的多级孔分子筛是一类适用于大分子反应的新型催化剂材料。然而，由于其结构的复杂性及形成机理的不确定性，阻碍了对其微结构解析、合成设计以及构效关系的研究，严重影响了其实用化进程。本项目拟通过建立准确的原子级模型，强化对其微观结构与大分子吸附、催化性能之间关系的理论解析，指导设计制备与结构调控；基于限制域生长法，引入多次水热生长循环与晶种二次生长，合成具有三维高度有序结构的多级孔分子筛，并根据模拟数据定向调控其晶相结构、孔结构以及酸结构；以C4烃类催化转化、大分子烯烃环氧化为特征反应，评价多级孔分子筛参与大分子反应的催化效率、剖析多级孔道的结构优势以及综合利用外表面活性位。本项目的实施不仅可以提供出一套从"功能-结构-合成"之间的关系入手，设计合成适用于大分子催化反应的新型多级孔分子筛的新方法和基础理论，还为多级孔分子筛微结构解析与定量构效关系建立提供新思路和理论依据。

中文关键词： 多级孔分子筛；限制域生长；VOCs气体捕集；甲醇制烯烃；构效关系

英文摘要： Hierarchical zeolites are attracting considerable attentions from both academic and industrial points of view due to their promising integrated superiorities of acidic property and shape selectivity from the microporous structure of zeolites and facilitated access and improved transport benefitted from the complementary hierarchical network. However, it is subjected to the complexity of microstructure and the uncertainty of formation mechanism, which seriously hinder the application of hierarchical zeolites. Here, we propose a systematic study on oriented synthesis and structure-property relationship investigation of hierarchical zeolites with three-dimensionally ordered mesoporous-imprinted (3DOm-i) structure. An atomistic model will be built to particularly analyse the microstructure, and further employed to investigate the structure effects, especially the hierarchical network, on the performance in reactions involving bulky molecules. Confined growth method along with multiple hydrothermal treatments and seeded growth, which provides a versatile means for introducing ordered mesoporosity to zeolites with controllable topology and morphology, will be used for the synthesis, and based on the simulation results, systematical control of crystalline, hierarchical network and acidic property will be proceeded. Fur

英文关键词： hierarchical zeolite；confined growth；VOCs capture；methanol to olefins；structure-property relationship