新型钴钼系耐硫变换催化剂本征动力学  

Intrinsic kinetics of a new cobalt molybdenum sulfur-tolerant shift catalyst

作　　者：冯云飞[1,2] 江莉龙[1,3] 曹彦宁[1,3] 张惠云[1,2] 马永德[1,3] 林诚[1,2] 

机构地区：[1]福州大学化学化工学院,福建福州350108 [2]福州大学化学工程与技术研究所,福建福州350108 [3]福州大学化肥催化剂国家工程研究中心,福建福州350002

出　　处：《工业催化》2013年第2期32-37,共6页Industrial Catalysis

基　　金：福建省科技厅产学重大项目(2012H6010);福建省发改委产业技术开发项目(闽发改高科[2010]1002号)

摘　　要：采用等温管式积分反应器,在(550～750)K、(2.0～3.5)MPa和空速(15～30)L.(g.h)-1条件下,对新型钴钼系耐硫变换催化剂进行变换反应本征动力学研究。建立了包含压力项的幂函数型动力学模型,根据实验测定数据,结合具有全局寻优能力微粒群算法和求解微分方程的龙格-库塔法,通过迭代寻优对变换反应动力学模型进行参数估计,获得高度显著、可信的动力学模型:r=-(dNCO)/(dW)=39981.876exp(-(68424.0)/(RT))PCO0.4176PH2O0.9297PCO2-0.5516PH2-0.7503(1-β)。结果表明,在催化剂上进行变换反应时,反应速率对CO组分分压变化的敏感性较低,H2O组分分压对反应速率的影响较大,高汽气比下催化活性较高。Abstract： The intrinsic kinetics of new cobalt molybdenum sulfur-tolerant catalyst for shift was studied in an isothermal integral tubular reactor under the reaction condition of temperature 750） K,pressure （2.0-3.5） MPa and space velocity （15-30） L. （g. h）-1. The intrinsic （550 - kineticsmodel taking the form of power function which included the pressure was built as flfllows：r=dNco/dw=399981.876exp（-68424.0/RT）P0.4176P0.9297P-0.5516P-0.7503（1-β）Using particle swarm optimization andRunge-Kutta algorithm, the parameters in the kinetics model were fit to the experimental data. The accuracy and the correlating degree of experimental data and calculated model were verified by F-test and correlation index test. The results showed that the reaction rate was not sensitive to pressure change of CO component but was sensitive to the pressure of H20 component. High catalytic activity was obtained underhigh steam gas ratio.

关 键 词：化学动力学 变换反应 钴钼系耐硫催化剂 本征动力学 微粒群算法 龙格-库塔法 动力学模型 

分 类 号：O643.1[理学—物理化学] TQ426.94[理学—化学]