Steam reforming of methane over Ni catalysts prepared from hydrotalcite-type precursors: Catalytic activity and reaction kinetics

doi:10.1016/j.cjche.2013.11.002

Abstract

Abstract: Ni/Mg-Al catalysts derived fromhydrotalcite-type precursorswere prepared by a co-precipitation technique and applied to steamreforming of methane. By comparison with Ni/γ-Al₂O₃ and Ni/α-Al₂O₃ catalysts prepared by incipientwetness impregnation, the Ni/Mg-Al catalyst presented much higher activity as a result of higher specific surface area and better Ni dispersion. The Ni/Mg-Al catalyst with a Ni/Mg/Almolar ratio of 0.5:2.5:1 exhibited the highest activity for steam methane reforming andwas selected for kinetic investigation. With external and internal diffusion limitations eliminated, kinetic experiments were carried out at atmospheric pressure and over a temperature range of 823-973 K. The results demonstrated that the overall conversion of CH₄ and the conversion of CH₄ to CO₂ were strongly influenced by reaction temperature, residence time of reactants aswell asmolar ratio of steam to methane. A classical Langmuir-Hinshelwood kinetic model proposed by Xu and Froment (1989) fitted the experimental data with excellent agreement. The estimated adsorption parameters were consistent thermodynamically.

Key words: Methane steam reforming, Hydrogen, Hydrotalcite, Catalyst, Kinetics

摘要： Ni/Mg-Al catalysts derived fromhydrotalcite-type precursorswere prepared by a co-precipitation technique and applied to steamreforming of methane. By comparison with Ni/γ-Al₂O₃ and Ni/α-Al₂O₃ catalysts prepared by incipientwetness impregnation, the Ni/Mg-Al catalyst presented much higher activity as a result of higher specific surface area and better Ni dispersion. The Ni/Mg-Al catalyst with a Ni/Mg/Almolar ratio of 0.5:2.5:1 exhibited the highest activity for steam methane reforming andwas selected for kinetic investigation. With external and internal diffusion limitations eliminated, kinetic experiments were carried out at atmospheric pressure and over a temperature range of 823-973 K. The results demonstrated that the overall conversion of CH₄ and the conversion of CH₄ to CO₂ were strongly influenced by reaction temperature, residence time of reactants aswell asmolar ratio of steam to methane. A classical Langmuir-Hinshelwood kinetic model proposed by Xu and Froment (1989) fitted the experimental data with excellent agreement. The estimated adsorption parameters were consistent thermodynamically.

关键词: Methane steam reforming, Hydrogen, Hydrotalcite, Catalyst, Kinetics

Yang Qi, Zhenmin Cheng, Zhiming Zhou. Steam reforming of methane over Ni catalysts prepared from hydrotalcite-type precursors: Catalytic activity and reaction kinetics[J]. Chin.J.Chem.Eng., 2015, 23(1): 76-85.

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