LB型节能催化剂上高温变换反应本征动力学及工业化测定

WGS reaction intrinsic kinetics and industrial measurement over LB energy-saving high temperature shift catalyst

运用正交实验设计安排了LB型节能催化剂高温变换反应本征动力学实验,测得不同温度、不同流量、不同水碳比、不同反应气体摩尔分数下LB型节能催化剂上CO高温变换反应本征动力学数据。用甲酸盐机理模型和幂函数模型拟合实验数据,确定了本征动力学模型参数。进行了本征动力学模型统计检验,表明所建模型无论局部还是整体都是显著和可信的。在此基础上,进行了大型合成氨装置上LB型节能催化剂高变反应工业化测定,按多组分单一反应等温球形催化剂一维非均相反应-扩散模型,利用配置法结合解非线性方程组的Merson法求解模型,得到了工业反应器中催化剂床层温度、内扩散有效因子、CO转化率和摩尔分数随床层相对高度的分布,模拟结果与工业化测定结果吻合。

The intrinsic kinetics experiments were conducted at different temperatures, different gas flow rates, different steam/gas ratios and different gas components over LB energy-saving high temperature shift catalyst. This is necessary for industrial application, process optimization and fundamental chemistry research of LB catalyst. The kinetics data were fitted with formate mechanism and power-law models, and the parameters in the models were estimated. Statistical examination showed that the two models were highly acceptable and creditable. Based on the kinetics results, the industrial measurement of LB catalyst used in a large-scale ammonia-synthesis plant was performed. With one-dimension heterogeneous diffusion- reaction model of isothermal spherical catalyst for multicomponent single reaction, the industrial reactor was simulated by using the configuration method and Merson method. The simulated distributions of bed temperature, intraparticle diffusion efficiency factor, CO content and shift ratio with respect to catalyst bed height were obtained, and the distributions agreed with those of industrial measurements.