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• W2046107910 abstract "NO reduction by CH4 over a 40% La2O3/γ-Al2O3 catalyst in the absence and presence of O2 in the feed was studied. The addition of either CO2 or H2O to the feed produced a reversible inhibitory effect on the rate similar to that observed with unsupported La2O3; however, the extent of rate inhibition was considerably smaller than on unsupported La2O3. At 973 K, either CO2 (9%) or H2O (2%) in the feed decreased activity by about 35% in the absence of O2 and by only 20% with excess O2 in the feed. In the absence of O2, a reaction mechanism previously proposed for La2O3 was altered to include competitive CO2 and H2O adsorption and to give the following rate expression for N2 formation: rN2=k′PNOPCH4(1+KNOPNO+KCH4PCH4+KCO2PCO2+KH2OPH2O)2. This equation fit the data well, had apparent activation energies of 14–25 kcal/mol, and gave thermodynamically consistent enthalpies and entropies of adsorption. Stable rates at 973 K with O2 and either CO2 or H2O in the feed were between 0.94 and 0.99 μmol N2/s/g catalyst. In the presence of excess O2, after CO2 and H2O adsorption were again included, a rate equation proposed earlier for La2O3 again provided a good fit to the data with H2O in the feed as well as thermodynamically consistent parameters determined under integral reaction operation. However, with both CO2 and excess O2 in the feed, this rate expression could not provide thermodynamically meaningful parameters from the fitting constants even though it fit the data well. This was attributed to a major contribution from the alumina to the overall rate, because CO2 had no significant effect on NO reduction on alumina, but it inhibited this reaction on La2O3. A reaction model was proposed for γ-Al2O3 that gave the rate expression for total CH4 disappearance due to both combustion and NO reduction over γ-Al2O3 (rCH4)T=k′comPCH4PO20.5+k′NOPNOPCH4PO20.5(1+K′NO2PNOPO20.5+KCH4PCH4+KO20.5PO20.5+KCO2PCO2+KH2OPH2O)2, which gave a satisfactory fit to the data along with thermodynamically consistent parameters. The second term in this equation, which represents the rate of N2 formation, was then combined with the rate equation for N2 formation on pure La2O3 in the presence of O2 to describe overall catalyst performance, and the data were fit well, assuming that La2O3 composed 6.8% of the total surface area, a value close to that of 6.1% obtained from XRD line-broadening calculations." @default.
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• W2046107910 date "2003-03-10" @default.
• W2046107910 modified "2023-09-27" @default.
• W2046107910 title "The effect of CO2 and H2O on the kinetics of NO reduction by CH4 over a La2O3/γ-Al2O3 catalyst" @default.
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• W2046107910 doi "https://doi.org/10.1016/s0021-9517(02)00092-1" @default.
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