Preparation of Fe-Mn/K/Al2O3 Fischer-Tropsch Catalyst and Its Catalytic Kinetics for the Hydrogenation of Carbon Monoxide

doi:10.1016/S1004-9541(13)60503-0

Abstract

Abstract: A K promoted iron-manganese catalyst was prepared by sol-gel method, and subsequently was tested for hydrogenation of carbon monoxide to light olefins. The kinetic experiments on a well-characterized Fe-Mn/K/Al₂O₃ catalyst were performed in a fixed-bed micro-reactor in a temperature range of 280-380 ℃, pressure range of 0.1-1.2 MPa, H₂/CO feed molar ratio range of 1-2.1 and a space velocity range of 2000-7200 h^-¹. Considering the mechanism of the process and Langmuir-Hinshelwood-Hogan-Watson (LHHW) approach, unassisted CO dissociation and H-assisted CO dissociation mechanisms were defined. The best models were obtained using non-linear regression analysis and Levenberg-Marquardt algorithm. Consequently, 4 models were considered as the preferred models based on the carbide mechanism. Finally, a model was proposed as a best model that assumed the following kinetically relevant steps in the iron-Fischer-Tropsch (FT) synthesis: (1) CO dissociation occurred without hydrogen interaction and was not a rate-limiting step; (2) the first hydrogen addition to surface carbon was the rate-determining steps. The activation energy and adsorption enthalpy were calculated 40.0 and -30.2 kJ·mol^-¹, respectively.

Key words: Fischer-Tropsch synthesis, catalysis, kinetics, chemical reactors, Levenberg-Marquardt (LM) method, Langmuir-Hinshelwood-Hogan-Watson (LHHW) kinetics

摘要： A K promoted iron-manganese catalyst was prepared by sol-gel method, and subsequently was tested for hydrogenation of carbon monoxide to light olefins. The kinetic experiments on a well-characterized Fe-Mn/K/Al₂O₃ catalyst were performed in a fixed-bed micro-reactor in a temperature range of 280-380 ℃, pressure range of 0.1-1.2 MPa, H₂/CO feed molar ratio range of 1-2.1 and a space velocity range of 2000-7200 h^-¹. Considering the mechanism of the process and Langmuir-Hinshelwood-Hogan-Watson (LHHW) approach, unassisted CO dissociation and H-assisted CO dissociation mechanisms were defined. The best models were obtained using non-linear regression analysis and Levenberg-Marquardt algorithm. Consequently, 4 models were considered as the preferred models based on the carbide mechanism. Finally, a model was proposed as a best model that assumed the following kinetically relevant steps in the iron-Fischer-Tropsch (FT) synthesis: (1) CO dissociation occurred without hydrogen interaction and was not a rate-limiting step; (2) the first hydrogen addition to surface carbon was the rate-determining steps. The activation energy and adsorption enthalpy were calculated 40.0 and -30.2 kJ·mol^-¹, respectively.

关键词: Fischer-Tropsch synthesis, catalysis, kinetics, chemical reactors, Levenberg-Marquardt (LM) method, Langmuir-Hinshelwood-Hogan-Watson (LHHW) kinetics

F. Fazlollahi, M. Sarkari, H. Gharebaghi, H. Atashi, M. M. Zarei, A. A. Mirzaei, W. C. Hecker. Preparation of Fe-Mn/K/Al₂O₃ Fischer-Tropsch Catalyst and Its Catalytic Kinetics for the Hydrogenation of Carbon Monoxide[J]. Chin.J.Chem.Eng., 2013, 21(5): 507-519.

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Preparation of Fe-Mn/K/Al₂O₃ Fischer-Tropsch Catalyst and Its Catalytic Kinetics for the Hydrogenation of Carbon Monoxide

Preparation of Fe-Mn/K/Al₂O₃ Fischer-Tropsch Catalyst and Its Catalytic Kinetics for the Hydrogenation of Carbon Monoxide

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