SC309催化剂甲醇合成反应本征动力学研究

Intrinsic kinetics of methanol synthesis over catalyst SC309

在等温积分反应器中测定了SC309型催化剂甲醇合成反应本征动力学数据。实验采用粒度为0.154mm～0.198mm的细颗粒催化剂,反应温度为180℃～260℃,反应压力为4MPa～8MPa,体积空速为4000h-1～10000h-1。选取L-H型方程建立了以各组分逸度表示的CO、CO2加氢合成甲醇反应本征动力学模型,使用通用全局马夸特算法进行参数估值,获得动力学模型参数。残差分析和统计检验表明,动力学模型是适宜的。实验结果表明,CO、CO2转化率在实验条件范围内随温度的升高先增加后降低,在240℃左右存在最大值,随压力的升高而增加,随空速的升高而降低。

The intrinsic kinetics of methanol synthesis over catalyst SC309 with the size of 0.154mm-0.198mm was investigated experimentally in an isothermal integral reactor at 180℃-260℃,4MPa-8MPa and space velocity of 4 000h-1-10 000h-1.The intrinsic kinetic models of the Langmuir-Hinshelwood type were derived in terms of the hydrogenation reaction rates of CO and CO2 in the form of the reactant fugacity,and the parameters of the models were obtained through Universal Global Optimization integrated with Marquardt method.It was proved by residual analysis and statistical test that the intrinsic kinetic models are reliable and acceptable.In the range of the experimental conditions,the conversions of CO and CO2 increased firstly and then decreased with temperature with a maximum at about 240℃,increased monotonically with pressure and decreased with space velocity.