聚丙烯酰胺水凝胶中核壳分子筛的可控合成及其MTO催化性能研究

项目名称： 聚丙烯酰胺水凝胶中核壳分子筛的可控合成及其MTO催化性能研究

项目编号： No.U1204215

项目类型： 联合基金项目

立项/批准年度： 2013

项目学科： 化学工程及工业化学

项目作者： 韩丽

作者单位： 郑州大学

项目金额： 30万元

中文摘要： 石油资源的日益短缺促使人们积极开发甲醇催化制烯烃技术（MTO）替代传统的轻油裂解制烯烃技术。MTO技术的关键是寿命长、低碳烯烃选择性高、稳定性好的复合分子筛催化剂的研制。为获得对MTO反应有较高催化活性的结构可调的ZSM-5/磷酸铝核壳分子筛催化剂，本项目拟将聚丙烯酰胺水凝胶引入ZSM-5/磷酸铝复合分子筛的合成凝胶中，以实现聚丙烯酰胺水凝胶中ZSM-5/磷酸铝核壳分子筛催化剂的可控合成。通过对ZSM-5/磷酸铝核壳分子筛可控合成影响因素的研究，阐明聚丙烯酰胺水凝胶中ZSM-5/磷酸铝核壳分子筛的形成机理，总结规律，为核壳复合分子筛的构筑提供新思路。通过分析材料“组成—结构—性能”之间性能协同效应，揭示壳层组成与微观结构对具有多级结构的ZSM-5/磷酸铝核壳分子筛性能的影响规律和作用机制，为新型高效MTO催化剂材料的设计开发奠定理论和技术基础。

中文关键词： 复合分子筛；核壳结构；聚丙烯酰胺水凝胶；可控合成；反应机理

英文摘要： The methanol-to-olefin (MTO) process has been highlighted in the past few years as an attractive alternative for light olefins. The key issue for the MTO process is to develop a novel composite zeolite catalyst with enhanced hydrothermal stability, mechanical strength, light olefins yield and coke resistance in MTO reaction. In this work, we report, for the first time, the controlled synthesis of ZSM-5/aluminophosphates core-shell composite zeolites via in situ crystallization in crosslinked polyacrylamide (PAM) hydrogels. The three-dimensional polyacrylamide networks with adjustable pore sizes provide unique scaffolds for the controlled synthesize of ZSM-5/aluminophosphates core-shell composite zeolites. The understanding of formation mechanisms of ZSM-5/aluminophosphates core-shell composite zeolites provides insights into the zeolite crystallization and the design of core-shell composite zeolites. The synergistic effect between compositions, structures and catalytic performances was studied and the influence of the compositions and structures of the core-shell composite zeolites on the methanol conversion to light olefins was explained. The study may provide a guideline to designing efficient catalysts for MTO reaction.

英文关键词： composite zeolite；core/shell structure；polyacrylamide hydrogel；controlled synthesis；reaction mechanism