Kinetics of methane combustion over CVD-made cobalt oxide catalysts

The present investigation provides the required kinetic parameters to evaluate and to predict the rate of the catalytic combustion of methane over cobalt oxide. For this purpose, monolithic cordierites with low specific surface area were uniformly coated with cobalt oxide thin films of controlled thickness using the chemical vapor deposition (CVD) process. The obtained catalysts were tested in the catalytic combustion of methane in oxygen-deficient and -rich conditions. Catalysts with loadings above 0.46 wt.% are active starting at a temperature of 250 degrees C and completely convert methane to CO2 below 550 degrees C where the conversion rate reaches 35 mu mol (CH4)/g(cat) s. The involvement of the bulk-oxide-ions in the catalytic reaction was supported by the constant value of the normalized reaction rate to the weight of deposited cobalt oxide. The experimental data fit well to the Mars-Van Krevelen redox model and can be approximated with a power rate law in oxygen-rich mixtures. The resulting activation energies and frequency factors allow the identification of the rate-limiting step and accurately reproduce the effect of the temperature and partial pressure of the reactants on the specific reaction rate. (c) 2006 Elsevier B.V. All rights reserved.