对二甲苯液相催化氧化动力学(Ⅰ)反应机理和动力学模型

KINETICS OF p-XYLENE LIQUID PHASE CATALYTIC OXIDATION(Ⅰ) REACTION MECHANISM AND KINETIC MODEL

针对PX高温液相催化氧化过程的特点开发了一套气液固三相反应实验技术 ,进行了氧化过程的动力学实验研究 .根据自由基反应机理和Co Mn Br三元催化体系的作用机制对PX氧化过程进行了深入的剖析 ,分析了芳烃中甲基和醛基的各步氧化机理及其与催化剂循环之间的耦合作用 .在此基础上推导出关于反应物浓度的动力学模型 ,并根据实验数据计算出各动力学参数 .

In this paper, a novel experimental technique for gas-liquid-solid reaction was developed to study kinetics of p -xylene oxidation under the condition of high temperature and pressure. Methyl and aldehyed oxidation during the p -xylene oxidation process was studied according to radical reaction mechanism and recycling of the cobalt-manganese-bromide catalyst. The coupling effect between catalysts and radical reactions was analyzed in detail, and a kinetic model was developed based on the proposed mechanism.Model parameters were determined by data fitting.The model agreed well with the experiments.