Decomposition of nitric oxide over perovskite oxide catalysts:: effect of CO2, H2O and CH4

Direct nitric oxide decomposition over perovskites is fairly slow and complex, its mechanism changing dramatically with temperature. Previous kinetic study for three representative compositions (La0.87Sr0.13Mn0.2Ni0.8O3-delta, La0.66Sr0.34Ni0.3 Co0.7O3-delta and La0.8Sr0.2Cu0.15Fe0.85O3-delta) has shown that depending on the temperature range, the inhibition effect of oxygen either increases or decreases with temperature. This paper deals with the effect of CO2, H2O and CH4 on the nitric oxide decomposition over the same perovskites studied at a steady-state in a plug-flow reactor with 1 g catalyst and total flowrates of 50 or 100 ml/min of 2 or 5% NO. The effect of carbon dioxide (0.5-10%) was evaluated between 873 and 923 K, whereas that of H2O vapor (1.6 or 2.5%) from 723 to 923 K. Both CO2 and H2O inhibit the NO decomposition, but inhibition by CO2 is considerably stronger. For all three catalysts, these effects increase with temperature. Kinetic parameters for the inhibiting effects of CO2 and H2O over the three perovskites were determined. Addition of methane to the feed (NO/CH4 = 4) increases conversion of NO to N-2 about two to four times, depending on the initial NO concentration and on temperature. This, however. is still much too low for practical applications. Furthermore, the rates of methane oxidation by nitric oxide over perovskites are substantially slower than those of methane oxidation by oxygen. Thus, perovskites do not seem to be suitable for catalytic selective NO reduction with methane. (C) 2002 Elsevier Science B.V. All rights reserved.