Kinetic Study of the Carbon Filament Formation by Methane Cracking on a Nickel Catalyst

A rigorous kinetic model for the formation of filamentous carbon on a nickel catalyst by methane cracking is derived. The experimental study was performed in an electrobalance unit. The temperature ranged from 773 to 823 K and the partial pressure of methane ranged from 1.5 to 10 bar. The mode of experimentation ensured that the rate of growth of the carbon filaments was always based upon the same number of filaments. A kinetic model is selected in which the abstraction of the first hydrogen atom from molecularly adsorbed methane is the rate-determining step. Based on the results of the parameter estimation, an energy diagram for the methane cracking is constructed.

[1]  A. Hamza,et al.  The activation of alkanes on Ni(100) , 1987 .

[2]  Robert C. Reid,et al.  Carbon deposition studies using nickel and cobalt catalysts , 1982 .

[3]  H. Wise,et al.  Thermodynamic properties of surface carbon on metals. 1. Nickel , 1983 .

[4]  A. D. Johnson,et al.  Collision‐induced dissociative chemisorption of adsorbates: Chemistry with a hammer , 1987 .

[5]  E. Ponzi,et al.  Kinetics of carbon formation from CH4-H2 mixtures on nickel-alumina catalyst , 1991 .

[6]  I. Chorkendorff,et al.  Xps study of chemisorption of CH4 on Ni(100) , 1990 .

[7]  J. Blakely,et al.  Segregation isosteres for carbon at the (100) surface of nickel , 1976 .

[8]  I. Alstrup,et al.  The kinetics of carbon formation from CH4 + H2 on a silica-supported nickel catalyst , 1992 .

[9]  G. Froment,et al.  Chemical Reactor Analysis and Design , 1979 .

[10]  E. Boellaard,et al.  The formation of filamentous carbon on iron and nickel catalysts : I. Thermodynamics , 1985 .

[11]  J. Rostrup-Nielsen.  Equilibria of decomposition reactions of carbon monoxide and methane over nickel catalysts , 1972 .

[12]  C. H. Bartholomew.  Hydrogen adsorption on supported cobalt, iron, and nickel , 1991 .

[13]  Xudong Jiang,et al.  The effect of sulfur on the dissociative adsorption of methane on nickel , 1990 .

[14]  M. B. Lee,et al.  Activated dissociative chemisorption of CH4 on Ni(111): Observation of a methyl radical and implication for the pressure gap in catalysis , 1986 .

[15]  C. H. Bartholomew.  Carbon Deposition in Steam Reforming and Methanation , 1982 .

[16]  D. Goodman,et al.  Dissociative adsorption of alkanes on Ni(100): Comparison with molecular beam results , 1988 .

[17]  G. Bond,et al.  Catalysis, science and technology , 1983 .

[18]  G. Froment,et al.  Filamentous carbon formation and gasification: Thermodynamics, driving force, nucleation, and steady-state growth , 1997 .

[19]  I. Alstrup,et al.  A new model explaining carbon filament growth on nickel, iron, and NiCu alloy catalysts , 1988 .

[20]  Jens R. Rostrup-Nielsen,et al.  Catalytic Steam Reforming , 1984 .

[21]  J. Mccarty,et al.  Thermodynamics of carbon coadsorbed with sulfur on Ni(100) , 1991 .

[22]  P. Siegbahn,et al.  A theoretical study of CHx chemisorption on the Ni(100) and Ni(111) surfaces , 1990 .

[23]  M. B. Lee,et al.  Dynamics of the activated dissociative chemisorption of CH4 and implication for the pressure gap in catalysis: A molecular beam–high resolution electron energy loss study , 1987 .

[24]  David L. Trimm,et al.  The Formation and Removal of Coke from Nickel Catalyst , 1977 .

[25]  B. D. Kay,et al.  Kinetics of the activated dissociative adsorption of methane on the low index planes of nickel single crystal surfaces , 1987 .

[26]  Hong Yang,et al.  Dissociative chemisorption of CH4 on Ni(111) , 1992 .

[27]  J. Konvalinka,et al.  Temperature programmed desorption of hydrogen from nickel catalysts , 1981 .

[28]  I. Alstrup,et al.  Kinetics of carbon formation from CH4 + H2 on silica-supported nickel and Ni-Cu catalysts , 1993 .