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

摘要/Abstract

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 E_a' 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 E_a of 105.79 kJ·mol^-1, the corresponding A of 2.94×10⁹cm³·g^-1·s^-1, heat of adsorption ΔH_{ads 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

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 E_a' 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 E_a of 105.79 kJ·mol^-1, the corresponding A of 2.94×10⁹cm³·g^-1·s^-1, heat of adsorption ΔH_{ads 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

雷志刚, 龙爱斌, 贾美如, 刘学义. Experimental and Kinetic Study of Selective Catalytic Reduction of NO with NH₃ over CuO/Al₂O₃/Cordierite Catalyst[J]. , 2010, 18(5): 721-729.

LEI Zhigang, LONG Aibin, JIA Meiru, LIU Xueyi. Experimental and Kinetic Study of Selective Catalytic Reduction of NO with NH₃ over CuO/Al₂O₃/Cordierite Catalyst[J]. , 2010, 18(5): 721-729.

参考文献

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

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

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