| Article ID | Journal | Published Year | Pages | File Type |
|---|---|---|---|---|
| 46454 | Applied Catalysis B: Environmental | 2012 | 13 Pages |
We present a systematic kinetic investigation of the full NO/NO2/N2O–NH3 SCR reacting system performed over a commercial Fe-promoted zeolite catalyst in the form of powder in a representative temperature range (150–550 °C) at high space velocities. The well-known reactions of the NO/NO2–NH3 SCR system, namely NH3 adsorption, NH3 and NO oxidation, standard-, fast- and NO2-SCR reactions, ammonium nitrate formation, and N2O formation are considered. In addition, dedicated runs with N2O added to the feed stream showed that two more reactions, namely N2O reduction by NO (N2O + NO → N2 + NO2) and N2O reduction by NH3 (2NH3 + 3 N2O → 4 N2 + 3H2O) become significant at T > 330 °C and need to be considered for kinetic modelling.The kinetic runs were fitted by multiresponse nonlinear regression to obtain estimates of the intrinsic rate parameters. Such parameters, as well as the relevant geometrical and morphological catalyst properties, were then successfully used to simulate on a purely predictive basis additional transient SCR runs performed over core honeycomb samples of the same Fe-zeolite catalyst, revealing modest effects of mass transfer limitations.In comparison with other published SCR kinetic models, the model herein developed accounts also for the N2O reactivity with NO and NH3, which is shown to be an important feature in order to accurately reproduce high-T operation of SCR converters based on Fe-zeolite catalysts.
Graphical abstractFigure optionsDownload full-size imageDownload as PowerPoint slideHighlights► Systematic investigation of NO/NO2/N2O–NH3 SCR reactions over commercial Fe-zeolite. ► N2O reactivity related to its NO-assisted decomposition and to its SCR with NH3. ► Global kinetic model developed to fully describe the NO/NO2/N2O–NH3 SCR reactions. ► First SCR model accounting also for N2O decomposition/reactivity. ► Dynamic 1D + 1D model of SCR monolithic converters accounting for mass transfer effects.
