SCI和EI收录∣中国化工学会会刊

›› 2010, Vol. 18 ›› Issue (5): 721-729.

• CATALYSIS, KINETICS AND REACTORS • Previous Articles     Next Articles

Experimental and Kinetic Study of Selective Catalytic Reduction of NO with NH3 over CuO/Al2O3/Cordierite Catalyst

LEI Zhigang, LONG Aibin, JIA Meiru, LIU Xueyi   

  1. State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029, China
  • Received:2010-02-22 Revised:2010-08-13 Online:2010-10-28 Published:2010-10-28
  • Supported by:
    Supported by the National Natural Science Foundation of China (20821004, 20736001, 21076008);the Research Fund for the Doctoral Program of Higher Education of China (2090010110002)

Experimental and Kinetic Study of Selective Catalytic Reduction of NO with NH3 over CuO/Al2O3/Cordierite Catalyst

雷志刚, 龙爱斌, 贾美如, 刘学义   

  1. State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029, China
  • 通讯作者: LEI Zhigang,E-mail:leizhg@mail.buct.edu.cn
  • 基金资助:
    Supported by the National Natural Science Foundation of China (20821004, 20736001, 21076008);the Research Fund for the Doctoral Program of Higher Education of China (2090010110002)

Abstract: The CuO/γ-Al2O3/cordierite catalyst, after being sulfated by sulfur dioxide (SO2) at 673 K, exhibits high activities for selective catalytic reduction (SCR) of nitrogen oxide (NO) with ammonia (NH3) at 573-723 K. The intrinsic kinetics of SCR of NO with NH3 over CuO/γ-Al2O3/cordierite catalyst has been measured in a fixed-bed reactor in the absence of internal and external diffusions. The experimental results show that the reaction rate can be quantified by a first-order expression with activation energy Ea' of 94.01 kJ·mol-1 and the corresponding pre-exponential factor A' of 3.39×108 cm3·g-1·s-1 when NH3 is excessive. However, when NH3 is not enough, an Eley-Rideal kinetic model based on experimental data is derived with Ea of 105.79 kJ·mol-1, the corresponding A of 2.94×109cm3·g-1·s-1, heat of adsorption ΔHads of 87.90 kJ·mol-1 and the corresponding Aads of 9.24 cm3·mol-1. The intrinsic kinetic model obtained was incorporated in a 3D mathematical model of monolithic reactor, and the agreement of the prediction with experimental data indicates that the present kinetic model is adequate for the reactor design and engineering scale-up.

Key words: kinetics, selective catalytic reduction, CuO/γ-Al2O3/cordierite catalyst, monolithic honeycomb reactor, mathematical model

摘要: The CuO/γ-Al2O3/cordierite catalyst, after being sulfated by sulfur dioxide (SO2) at 673 K, exhibits high activities for selective catalytic reduction (SCR) of nitrogen oxide (NO) with ammonia (NH3) at 573-723 K. The intrinsic kinetics of SCR of NO with NH3 over CuO/γ-Al2O3/cordierite catalyst has been measured in a fixed-bed reactor in the absence of internal and external diffusions. The experimental results show that the reaction rate can be quantified by a first-order expression with activation energy Ea' of 94.01 kJ·mol-1 and the corresponding pre-exponential factor A' of 3.39×108 cm3·g-1·s-1 when NH3 is excessive. However, when NH3 is not enough, an Eley-Rideal kinetic model based on experimental data is derived with Ea of 105.79 kJ·mol-1, the corresponding A of 2.94×109cm3·g-1·s-1, heat of adsorption ΔHads of 87.90 kJ·mol-1 and the corresponding Aads of 9.24 cm3·mol-1. The intrinsic kinetic model obtained was incorporated in a 3D mathematical model of monolithic reactor, and the agreement of the prediction with experimental data indicates that the present kinetic model is adequate for the reactor design and engineering scale-up.

关键词: kinetics, selective catalytic reduction, CuO/γ-Al2O3/cordierite catalyst, monolithic honeycomb reactor, mathematical model