择形分子筛催化剂反应-扩散的介尺度耦合机制及其调控方法

项目名称： 择形分子筛催化剂反应-扩散的介尺度耦合机制及其调控方法

项目编号： No.91534115

项目类型： 重大研究计划

立项/批准年度： 2016

项目学科： 有机化学

项目作者： 朱志荣

作者单位： 同济大学

项目金额： 67万元

中文摘要： 本项目以焦化苯与甲醇烷基化反应制对二甲苯择形催化剂为研究对象，以揭示择形分子筛催化剂表界面介尺度结构与反应-扩散耦合机制、建立理论量化模型与调控方法为研究目标。首先建立真实反映择形催化剂性能与反应过程的原位动态测试方法，并设计制备一系列具有不同酸性和孔结构特性的分子筛催化剂；分别采用固定床积分反应器与内循环等梯度微分反应器，研究在不同反应条件下催化剂分子筛外表面、孔道内的区域活性位及其催化反应、分子筛内微孔反应扩散、分子筛粘接间中孔扩散对反应转化率与产物组成的影响及其相互关系，深入分析择形催化中反应-扩散的耦合过程，揭示表界面介尺度结构形成机制与演化规律；通过多目标变分的多尺度计算方式，对反应组分在分子筛晶粒、催化剂颗粒内部的动态分布进行微分衡算，模拟催化反应受孔内外传质扩散影响的过程，建立择形催化材料的介尺度数学量化理论模型；据此提出有效的反向调控方法，指导制备出新型的烷基化择形催化剂。

中文关键词： 分子筛催化剂；反应-扩散；择形催化；耦合效应；介尺度

英文摘要： This project tries to clarify the coupling mechanism of reaction – diffusion, the interface mesoscale structures, theoretical mathematical model and controlling method over shape-selective zeolite catalysts, in order to develop the catalyst for alkylation of coking benzene with methanol to produce para-xylene. Firstly, the in-situ & dynamic characterization methods will be established accurately to determine the properties of shape-selective catalysts and alkylation reaction respectively. In addition, a variety of shape-selective zeolite catalysts with the typical acidity & structure will be prepared. By using the fixed bed reactor and the internal circulation gradientless reactor, under the different reaction conditions, the effect of the reactive sites on the external surface and in the channel of zeolites and their catalytic reaction, the diffusion in the microporous channel of zeolites and the diffusion in the mesoporous channel among zeolites /adhesives on the reaction conversion and product composition will be investigated, and their relationship among these mesoscale factors will be studied as well. Moreover, the coupling process of reaction – diffusion in the shape-selective zeolite catalyst will be analyzed, and the formation of the interface mesoscale structures and its transformation is clarified. By means of differential calculation in the multi-dimensions and the multi-factors & objectives, the dynamic composition distribution of the reactants & products will be simulated in the zeolite channels and the pores of catalyst particles. The process between the catalytic reaction and microporous and mesoporous diffusion will be simulated. The mesoscale mathematical model for shape-selective catalysts will be established. Based on the above results, the effective controlling method will be proposed, and the new shape-selective catalyst for alkylation will be designed and prepared with the high performance.

英文关键词： zeolite catalyst;reaction - diffusion;shape-selective catalysis;coupling mechanism;Mesoscale