Journal
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
Volume 49, Issue 1, Pages 39-52Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ie9003464
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Funding
- Swedish Research Council [621-2003-4149, 621-2006-3706]
- Knut and Alice Wallenberg Foundation [Dnr KAW 2005.0055]
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The selective catalytic reduction of NOx with ammonia over all Fe-zeolite catalyst was investigated experimentally and a transient kinetic model was developed. The model includes reactions that describe ammonia storage and oxidation, NO oxidation, selective catalytic reduction (SCR) of NO and NO2, formation of N2O, ammonia inhibition and ammonium nitrate formation. The model call account for a broad range of experimental conditions in the presence of H2O, CO2 and O-2 at temperatures from 150 to 650 degrees C. The catalyst stores ammonia at temperatures up to 400 degrees C and shows ammonia oxidation activity from 350 degrees C. The catalyst is also active for the oxidation of NO to NO2 and the oxidation reaches equilibrium at 500 degrees C. The SCR of NO is already active at 150 degrees C and the introduction of equal amounts of NO and NO2 greatly enhances the conversion of NOx at temperatures up to 300 degrees C. The formation of N2O is negligible if small fractions of NO2 are fed to the reactor, but a significant amount of N2O is formed at high NO2 to NO ratios. An ammonia inhibition oil the SCR of NO is observed at 200 degrees C. This kinetic model contains 12 reactions and is able to describe the experimental results Well. The model was validated using short transient experiments and experimental conditions not used in the parameter estimation and predicted these new conditions adequately.
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