微通道反应器内环己酮肟贝克曼重排反应研究

项目名称： 微通道反应器内环己酮肟贝克曼重排反应研究

项目编号： No.U1463208

项目类型： 联合基金项目

立项/批准年度： 2015

项目学科： 数理科学和化学

项目作者： 骆广生

作者单位： 清华大学

项目金额： 300万元

中文摘要： 本项目以环己酮肟贝克曼重排反应为对象，围绕“贝克曼重排反应的催化机制和动力学特性”和“微尺度条件下贝克曼重排反应过程传递与反应的耦合规律”两个关键科学问题展开研究。以微通道反应器为研究平台，深入研究烟酸、有机酸和固体催化剂三种催化体系中的贝克曼重排反应本征动力学、热效应、主要副产物和选择性变化规律。采用Micro-PIV、高速显微和在线红外等现代观测技术研究重排反应过程的微尺度流动、分散、混合、传递和反应规律。针对液相重排反应，研究其微尺度反应特性，探讨反应强化机制和发展过程强化新方法，建立耦合传递和反应性能的数学模型。针对气相重排反应，在微通道反应器内研究反应转化率的变化规律，研究催化剂失活规律、反应工艺条件对副产物种类及含量的影响。结合CFD模拟方法深入探讨微通道反应器内相间传递和反应的耦合规律，发展适用于贝克曼气相重排反应的新型微通道设备和过程强化新方法。

中文关键词： 微反应器；贝克曼重排；反应动力学；选择性

英文摘要： This project focuses on the Beckmann rearrangement of cyclohexanone oxime, an important step in the synthesis of caprolactam. Two key scientific problems to be solved in the project are ‘the catalytic mechanism and reaction kinetics of Beckmann rearrangement’ and ‘the transport-reaction coupling mechanism of Beckmann rearrangement process in microreactors’. In details, the microreactor has been chosen as the major reactor. The reaction kinetics, reaction enthalpy, main side reactions and selectivity will be determined in three catalytic systems: oleum, organic acid and solid catalysts. The flow, dispersion, mixing, transport and reaction performances at microscale will be investigated with advanced measurement technologies, such as micro-PIV, high-speed microscopic and infrared thermal imaging. For the liquid phase rearrangement, the reaction performance and process intensification will be explored and a new mathematical model will be developed to discuss coupling mechanism of transport and reaction process. For the gas phase rearrangement, the conversion, catalyst deactivation, side products in microchannel reactors will be determined. Furthermore, the coupling mechanism of multi-phase transport and reaction will be discussed with both the experiment and CFD simulation method. Based on the above research, it is promising to develop some new microstructured equipment and process intensification methods for the Beckmann rearrangement.

英文关键词： Microreactor;Beckmann rearrangement;Reaction kinetics;Selectivity