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

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