期刊
JOURNAL OF PHYSICAL CHEMISTRY B
卷 109, 期 6, 页码 2432-2438出版社
AMER CHEMICAL SOC
DOI: 10.1021/jp040239s
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The CO methanation reaction over nickel was studied at low CO concentrations and at hydrogen pressures slightly above ambient pressure. The kinetics of this reaction is well described by a first-order expression with CO dissociation at the nickel surface as the rate-determining step. At very low CO concentrations, adsorption of CO molecules and H atoms compete for the sites at the surface, whereas the coverage of CO is close to unity at higher CO pressures. The ratio of the equilibrium constants for CO and H atom adsorption, K-CO/K-H, was obtained from the rate of CO methanation at various CO concentrations. K-H was determined independently from temperature programmed adsorption/desorption of hydrogen to be K-H = 7.7 x 10(-4) (bar(-0.5)) exp[43 (kJ/mol)/RT] and hence the equilibrium constants for adsorption of CO molecules may be calculated to be K-CO = 3 x 10(-7) (bar(-1)) exp[122 (kJ/mol)/RT]. Furthermore, the rate of dissociation of CO at the catalyst surface was determined to be 5 x 10(9) (s(-1)) exp[-96.7 (kJ/mol)/RT] assuming that 5% of the surface nickel atoms are active for CO dissociation, The results are compared to equilibrium and rate constants reported in the literature.
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