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Carbon formation and CO methanation on silica-supported nickel and nickel-copper catalysts in CO + H{sub 2} mixtures

Journal Article · · Journal of Catalysis
;  [1]; ;  [2]
  1. Universidade do Minho, Guimaraes (Portugal)
  2. Haldor Topsoe Research Labs., Lyngby (Denmark)

The steady-state rates of simultaneous carbon formation and methanation on silica-supported nickel and nickel-copper catalysts in CO + H{sub 2} gas mixtures have been measured in the partial pressure range 10-30 kPa and the temperature range 583-873 K. The steady-state kinetic results for carbon formation can be explained by a model previously used for carbon formation in pure CO gas, but modified to take into account the influence of hydrogen. Comparisons between the results for Ni/SiO{sub 2}, Ni{sub 0.99}Cu{sub 0.01}/SiO{sub 2}, and Ni{sub 0.75}Cu{sub 0.25}/SiO{sub 2} show that the specific rate of carbon formation is increased when 1 at.% of Cu is added to a nickel catalyst, but that the rate decreases when the Cu content is increased to 10 at.%, and that no carbon formation is seen for the Ni{sub 0.75}Cu{sub 0.25}/SiO{sub 2} catalyst. The addition of a small amount of Cu, on the other hand, decreases the methanation rate while at higher Cu contents the rate goes up again and a maximum is observed at about 7 at.% Cu. Thus a simple ensemble model cannot explain the influence of copper on the rate of carbon formation or methanation. Comparison of carbon formation and methanation rates for the Ni/SiO{sub 2} and the Ni{sub 0.99}Cu{sub 0.01}/SiO{sub 2} catalysts indicates that the two reactions have different rate-controlling steps and that the carbon formation influences the methanation rate mainly through poisoning of the catalysts. 27 refs., 9 figs., 5 tabs.

OSTI ID:
263695
Journal Information:
Journal of Catalysis, Journal Name: Journal of Catalysis Journal Issue: 2 Vol. 158; ISSN 0021-9517; ISSN JCTLA5
Country of Publication:
United States
Language:
English