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作 者:柳祥伟[1] 唐黎华[1] 张琪[1] 吴勇强[1] 倪燕慧[1] 朱子彬[1]
机构地区:[1]华东理工大学大型工业反应器工程教育部工程研究中心,上海200237
出 处:《高校化学工程学报》2011年第4期603-608,共6页Journal of Chemical Engineering of Chinese Universities
摘 要:在内循环无梯度反应器中测定了甲醇合成反应的宏观动力学,实验压力为8 MPa,反应温度190~250℃,实验采用国产NC309催化剂,直径为Ф5 mm×5 mm的圆柱状颗粒,原料气组成覆盖工业生产范围。选取以各组分逸度表示的CO、CO2加氢合成甲醇的Langmuir-Hinshelwood双速率反应动力学模型。根据实验所得到的数据,运用改进的遗传算法和马夸特算法相结合的方法,确定了动力学参数,残差分析和统计检验表明动力学模型是适宜的。得到的CO、CO2反应速率常数分别为:k1=4.626×102 exp(-4.3818×10 4/RT)、k2=2.614×103 exp(-6.3935×10 4/RT),其中两个反应的活化能分别为:E1=4.3818×104J·mol-1、E 2=6.3935×104J·mol-1。The global kinetics of methanol synthesis over NC309 Cu-based catalyst was investigated in an internal recycle gradientless reactor at 8 MPa and 190~250℃.The catalyst used is in the shape of cylindrical particles with the size of φ5 mm×5 mm,and the composition of feed gas is in the scope of industry production.The Langmuir-Hinshelwood double rate global kinetic models were selected in which the reaction rates of CO hydrogenation and CO2 hydrogenation were expressed as the functions of the reactant fugacity.According to the experimental data,the kinetics parameters were calculated by the improved Genetic Algorithm combining with Marquardt method,then the reaction rate constants k1 and k2 and the activation energies E1 and E2 for CO and CO2 hydrogenations were obtained respectively.The residual error distribution and the statistic test show that the global kinetic models selected are reliable and acceptable.
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