R. Hakkarainen et al., COMPARISON OF THE DYNAMICS OF THE HIGH-TEMPERATURE WATER-GAS SHIFT REACTION ON OXIDE CATALYSTS, Catalysis today, 20(3), 1994, pp. 395-408
The dynamics of the high-temperature water-gas shift reaction on iron
oxide and Co-Mo-oxide catalysts was studied with transient response ex
periments performed at 563-673 K at atmospheric pressure in a gradient
less spinning basket reactor. At the reaction start-up the step respon
se of CO2 on the iron oxide catalyst was always faster than the respon
se of H2, whereas the response of H2 on the Co-Mo catalyst was faster
than the response of CO2. Water pretreatment retarded the response of
H2 on the iron oxide catalyst, whereas a similar pretreatment accelera
ted the response of H2 on the Co-Mo catalyst. Based on the results of
the transient response experiments reaction mechanisms were proposed f
or the water-gas shift reaction on both catalysts. The rate determinin
g steps on the iron oxide catalyst were assumed to be the CO2 desorpti
on and surface hydroxyl decomposition steps. The rate determining step
s on the Co-Mo catalyst were assumed to be the surface reaction and CO
2 desorption steps. The transient responses were modelled with non-ste
ady-state rate equations based on the mechanisms, and the kinetic cons
tants were determined by regression analysis. The kinetic models were
able to describe the transient behaviours of the oxide catalysts.