e-journal
The catalytic performance of Cu-containing zeolites in N2O decomposition and the influence of O2, NO and H2O on recombination of oxygen
Abstract.
The catalytic decomposition of N2O was studied over Cu-containing zeolites with different Cu loadings
and framework topologies (MFI, MOR, FER, BEA, and FAU). The influence of NO, O2, and H2O on the rate
of N2O decomposition was investigated in detail. A kinetic model was developed based on the relevant
elementary reaction steps in the mechanism of N2O decomposition. The recombination of oxygen atoms
into molecular oxygen is recognized as the rate-limiting step in N2O decomposition. The rate of oxygen
desorption depends strongly on the Cu loading. At low Cu loadings, migration of oxygen atoms is required
for recombinative desorption. NO accelerates oxygen recombination, because it provides an alternative
route for oxygen migration via gas-phase NO2. The effect of water differs for Cu-containing zeolites with
high and low Cu loadings. At high Cu loading, the rate is suppressed by competitive adsorption of water
on the active sites, resulting in an increase in apparent activation energy. The rate of N2O decomposition
is increased substantially for catalysts with a low Cu loading. This is tentatively attributed to water induced mobility of Cu ions, which facilitates oxygen migration. The effect of water addition is fully
reversible.
Keywords:
N2O decomposition
NO
Water
Cu-zeolites
Mechanism
Kinetics
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