整装式纤维@ZSM-5核-壳结构催化剂的‘Top-Down’设计合成及其甲醇制丙烯选择性调控的构效研究

项目名称： 整装式纤维@ZSM-5核-壳结构催化剂的‘Top-Down’设计合成及其甲醇制丙烯选择性调控的构效研究

项目编号： No.21473057

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： 路勇

作者单位： 华东师范大学

项目金额： 90万元

中文摘要： 微结构化催化剂和反应器（MCRs）已被广泛证实能显著优化催化剂床层的流体力学行为和提高床层内部的传质/传热性能，在多相催化领域的研究正受到越来越多的关注。本课题提出了反应器-催化剂自上而下（Top-Down）结构化设计的MTP反应选择性调控新策略。集成新型纤维结构技术独特的强化传质/传热和优化流体流动特性与ZSM-5优异的催化甲醇制烃性能，以实现反应器（Top）内流动和传递与表界面（Down）MTP催化反应的协同耦合，创制一种丙烯选择性高、导热性好、稳定可再生和渗透性能好的纤维@ZSM-5核-壳结构MTP催化剂。研究结构催化剂诸如几何构型、分子筛壳层厚度、壳层分子筛硅铝比和晶粒尺寸与晶面取向、孔隙度与孔分布等宏微结构与物化性质对生成丙烯的选择性调控关系。建立模拟、动力学和反应产物及床层温度分布测定实验方法，研究结构催化剂的几何、水力学和传递性质，及其与表界面催化反应的传递耦合作用机制。

中文关键词： 结构催化剂；分子筛；甲醇制烯烃；反应动力学；构效关系

英文摘要： Development and use of the microstructured catalyst is a promising strategy to overcome these major drawbacks due to improved hydrodynamics in combination with enhanced heat/mass transfer, thus being a major field in heterogeneous catalysis. Herein, the principle goal is to raise and then maintain a high selectivity to propylene of the MTP process, and therefore we propose a Top-Down design MCR strategy for achieving this goal. We attempt to develop a new standing-free microfibrous-structured ZSM-5 zeolite catalyst obtainable in a macroscopic scale by direct growth of ZSM-5 zeolite crystals onto a three-dimensional (3D) porous network of sinter-locked metal microfibers. This new approach can provide an efficient and effective combination of large void volume (continuously adjustable), high heat/mass transfer, narrow resistance time distribution, micro- to macro-engineered hierarchical pore structure, binder-free in situ hydrothermal synthesis, core-shell structure, and good rigidity/robustness. Thanks to the above beneficial properties, our standing-free fiber@ZSM-5 core-shell catalysts are expected to provide visible promotion on the selectivity to C2-C4 olefins especially to propylene with obviously prolonged lifetime in stream, compared to the corresponding zeolite powders. Effects of features of fiber@ZSM-5 core-shell catalysts in terms of geometry, textural properties, zeolite crysttal orientation, ect., will be sytematically investigated on their MTP selectivity and stability. Computational fluid dynamics (CFD) code FLUENT in combination with experimental testing will be employed to simulate the temperature and reaction distributions inside such microfibrous-structured catalytic bed, demonstrating the process intensification benefitted form enhanced heat/mass and improved hydrodynamics.

英文关键词： Structured Catalysts;Zeolite;Methanol-to-Olefin;Reaction Kinetic;Structure-performance relationship