Abstract

The kinetics of sulfur deactivation of alumina-supported nickel and ruthenium catalysts are examined under methanation conditions in the presence of low concentration of H 2S (<10 ppm) added to the feed stream ( H 2 CO = 4 1 ) . Based on a theoretical analysis of catalyst deactivation by irreversibly adsorbed surface sulfur atoms, we calculate the deactivation rate constants for the poisoning process. The Ru Al 2O 3 catalyst exhibits a higher poisoning rate constant than Ni Al 2O 3 . The catalytic properties of Ni Al 2O 3 are greatly modified by the addition of low concentrations of Ir. The Ni Ir Al 2O 3 catalyst exhibits higher methanation activity and greater resistance to sulfur deactivation. Temperature-programmed desorption and surface reaction studies indicate the formation of new binding states for CO adspecies on the surface of the Ni Ir catalyst. Surface composition measurements by means of Auger electron spectroscopy demonstrate considerable Ir enrichment on the surface of the Ni Ir Al 2O 3 catalyst.

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