Industrial & Engineering Chemistry Research, Vol.50, No.18, 10493-10499, 2011
Rate Expression for Water-Gas Shift over a Gold/Ferrochrome Catalyst
The kinetics of low-temperature water-gas shift over gold/ferrochrome catalysts were studied at atmospheric pressure and temperatures between 160 and 180 degrees C. During two extended kinetic experiments lasting 903 and 1313 h, the activity of the catalyst decreased by 52% and 78%, respectively. The corresponding changes in the Brunauer-Emmett-Teller surface areas were 16% and 12%, respectively, suggesting that changes in the support surface area are not the primary cause for deactivation. The use of a bracketing technique, wherein the system was regularly returned to a standard set of reaction conditions, allowed the rate expression to be written as the product of an activity factor, which accounted for catalyst deactivation, and a power-law rate expression, which accounted for the dependence of the reaction rate upon temperature and composition. The power-law kinetic expression, including a term to account for the approach to equilibrium, was found to describe the kinetics of the reaction reasonably well. The resulting reaction orders were 0.39 for CO, 0.99 for H2O, -0.28 for CO2, and -0.25 for H-2, and the apparent activation energy was equal to 88.2 kJ/mol.