NiMo/Al_2O_3催化剂上菲加氢反应体系动力学

Kinetics of Phenanthrene Hydrogenation System over Ni Mo/Al_2O_3 Catalyst

采用Ni Mo/Al2O3催化剂,以菲和氢气为原料,在固定床连续流动微反装置上,系统地考察了反应温度、反应压力以及空速等对菲加氢反应的影响。利用热力学计算的反应平衡常数,根据Langmuir-Hinshelwood-Hougen-Watson(LHHW)吸附理论推导反应动力学方程式,采用拟牛顿法中的BFGS算法估计反应速率常数、活化能以及吸附常数,并对不同的反应网络途径进行了对比筛选。在研究的反应条件下,存在从9,10-二氢菲到1,10-八氢菲的反应路径,但不能排除存在从9,10-二氢菲到四氢菲的的反应路径,模型拟合效果良好。

Withphenanthrene andhydrogen as raw materials, the hydrogenation of phenanthrene was tested over NiMo/Al2O3 catalyst in the fixed-bed microreactors. Effects of temperature, reaction pressure and space velocity on the reaction were systematically investigated. Based on the equilibrium constants by the thermodynamic method and kinetic equation derived by the Langmuir-Hinshelwood-Hougen-Watson adsorption theory, the reaction rate constants, activation energy and adsorption constants were estimated by Broyden-Fletcher-Goldfarb-Shanno（BFGS） quasi-Newton scheme, and the different reaction networks were compared and screened. Under the reaction conditions of the study, the result showed that the reaction path from 9, 10-dihydrophenathrene to 1,10-octahydrophenanthrene was confirmed, and the path from 9, 10-dihydrophenathrene to tetrahydrophenathrene could not be excluded, and the fitting result of screened model was good.