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Alkali promotion of nickel catalysts for carbon monoxide methanation

Journal Article · · J. Catal.; (United States)
Differential reactor studies of carbon monoxide hydrogenation have been carried out on a series of 8 percent Ni/SiO/sub 2/--Al/sub 2/O/sub 3/ catalysts in which the supports have been impregnated with increasing amounts of sodium. Magnetic measurements show that the extent of reduction and the nickel crystallite size are not influenced by the sodium on the support. Hydrogen adsorption measurements reveal that the exposed surfaces are in agreement with the crystallite sizes and are not significantly poisoned by the alkali. The turnover number increases with sodium content and passes through a maximum at 0.3 percent Na with an enhancement by a factor of 6. Kinetic data best fit the surface reaction mechanism for which rate = kK(/sub CO/P/sub CO/P/sup /sup 1///sub 2///sub H//(1 + K/sub CO/P/sub CO/)/sup 2/. For K/sub CO/, the pre-exponential factor and heat of adsorption are unchanged by Na, but the parameters of k are not. The pre-exponential factor passes through a maximum and the activation energy decreases as the Na level increases. These results are best explained by an initial decrease in acidity, which keeps the nickel surface clean, followed by a poisoning via direct metal interaction or support modification by the alkali.
Research Organization:
Univ. of Houston, TX
OSTI ID:
5358774
Journal Information:
J. Catal.; (United States), Journal Name: J. Catal.; (United States) Vol. 51:1; ISSN JCTLA
Country of Publication:
United States
Language:
English