低汽气比LB型中温变换催化剂上水煤气变换反应的动力学研究  

Kinetic Study of High Temperature Water-Gas Shift Reaction over LB Type Catalyst

作　　者：李建伟[1] 白静宇[2] 姚飞[2] 李成岳[1] 

机构地区：[1]北京化工大学可控化学反应科学与技术基础教育部重点实验室,北京100029 [2]北京化工大学经济管理学院,北京100029

出　　处：《催化学报》2005年第1期25-31,共7页

摘　　要：采用微型等温积分反应器 ,在 3MPa ,5 98～ 72 8K以及气体组成 (摩尔分率 )为CO 0 0 6 6～ 0 139,CO2 0 0 4 1～ 0 1,H20 2 6 2～ 0 4 5 7,H2 O 0 2 17～ 0 386和N2 0 0 77～ 0 2 71的条件下 ,对国产LB型低汽气比中温变换催化剂的动力学特性进行了系统的研究 .对基于一级反应模式、二级反应模式和幂函数经验式的三种变换反应动力学模型 ,以Simplex Gauss Newton复合法估计了相应的模型参数 .数理统计检验结果表明 ,三种动力学模型在统计学意义上均是可信的 .进一步的工业应用检验表明 ,由于结构上的不同 ,当用于非等温工业反应器性能分析时 ,三种模型预报的结果具有明显差异 ,相比之下 ,幂函数型动力学方程更适宜于描述LB型变换催化剂的动力学特性 .因此 ,由等温实验数据和传统的数理统计检验获得的动力学模型具有不确定性 ,为使动力学模型的应用更为可靠 ,对所建立的动力学模型进行工业应用检验是必要的 .The intrinsic kinetic experiments of high temperature water-gas shift reaction over a domestic catalyst of LB type were carried out in an integral microreactor under the conditions of 3 MPa, 598 similar to 728 K, and feed gas composition (mole fraction) of CO 0.066 similar to 0.139, CO2 0.041 similar to 0.1, H-2 0.262 similar to 0.457, H2O 0.217 similar to 0.386, and N-2 0.077 similar to 0.271. Three kinds of typical kinetic models, one-order, two-order and power-law type, were distinguished. By means of the Simplex-Gauss-Newton complex optimal method, parameters of these kinetic models were estimated. Statistical tests show that these models are all highly acceptable and reliable, but industrial application tests indicate that there would be a considerable difference in performance prediction among different models when they are employed to model an industrial reactor for their structural differences. This once again suggests that the kinetic models which are developed by isothermal experimental data and traditional symbolic statistical method are uncertain. It seems to be a more advantageous method to develop a suitable kinetic model combining the traditional kinetic investigation with the industrial application judgement. Based on this viewpoint, the power-law type kinetic model is chosen to describe the kinetic performance of the LB type catalyst, and a good agreement with experimental and industrial operation data is obtained.

关 键 词：水煤气变换反应 中温变换催化剂 动力学 动力学模型 

分 类 号：O643[理学—物理化学]