The effect of chlorine modification of silica-supported Ru on its CO hydrogenation properties

An investigation of CO hydrogenation on Cl-modified supported Ru catalysts has been carried out using both steady-state Fischer-Tropsch synthesis and steady-state isotopic transient kinetic analysis of methanation. The steady-state reaction results illustrate how the presence of chlorine acts to dec...

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Bibliographic Details
Published in:Journal of catalysis 1990-05, Vol.123 (1), p.1-11
Main Authors: Iyagba, Elijah T., Eddy Hoost, T., Nwalor, John U., Goodwin, James G.
Format: Article
Language:English
Subjects:
01 COAL, LIGNITE, AND PEAT
010408 - Coal, Lignite, & Peat- C1 Processes- (1987-)
ALKANES
CARBON COMPOUNDS
CARBON MONOXIDE
CARBON OXIDES
CATALYSIS
CATALYST SUPPORTS
CATALYSTS
CATALYTIC EFFECTS
CHALCOGENIDES
CHEMICAL REACTION KINETICS
CHEMICAL REACTIONS
Chemistry
CHLORINE
DEACTIVATION
ELEMENTS
Exact sciences and technology
FISCHER-TROPSCH SYNTHESIS
General and physical chemistry
HALOGENS
HYDROCARBONS
HYDROGENATION
KINETICS
METALS
METHANATION
METHANE
MORPHOLOGICAL CHANGES
NONMETALS
ORGANIC COMPOUNDS
OXIDES
OXYGEN COMPOUNDS
PLATINUM METALS
REACTION INTERMEDIATES
REACTION KINETICS
RUTHENIUM
SILICON COMPOUNDS
SILICON OXIDES
SURFACE PROPERTIES
SYNTHESIS
Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry
TRANSITION ELEMENTS
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Summary:An investigation of CO hydrogenation on Cl-modified supported Ru catalysts has been carried out using both steady-state Fischer-Tropsch synthesis and steady-state isotopic transient kinetic analysis of methanation. The steady-state reaction results illustrate how the presence of chlorine acts to decrease catalytic activity and to enhance the selectivity of methane formation even though it is present on the catalyst only during the initial stages of the reaction. The deactivation results for F-T as well as the isotopic transient results suggest that structural rearrangements induced by the presence of chlorine, rather than selective site blocking or electronic interactions, may be the primary mechanism of chlorine modification of the catalytic properties of supported ruthenium for CO hydrogenation. Isotopic transients indicated that the decrease in methanation activity with increasing initial Cl concentration was a function of a decrease in the number of reactive surface intermediates (or sites) and not of a change in site activity.
ISSN:0021-9517
1090-2694
DOI:10.1016/0021-9517(90)90152-A