Low temperature selective catalytic reduction of NO with NH3 over Mn–Fe spinel: Performance, mechanism and kinetic study
(Fe3−xMnx)1−δO4 was synthesized using a co-precipitation method and then developed as a catalyst for the low temperature selective catalytic reduction (SCR) of NO with NH3. The SCR activity of (Fe3−xMnx)1−δO4 was clearly enhanced with the increase of Mn content. The results of in situ DRIFTS study demonstrated that both the Eley–Rideal mechanism (i.e. reaction of activated ammonia with gaseous NO) and the Langmuir–Hinshelwood mechanism (i.e. reaction of adsorbed ammonia species with adsorbed NOx species) might happen during the SCR reaction over (Fe3−xMnx)1−δO4. According to the kinetic analysis, the respective contribution of the Langmuir–Hinshelwood mechanism and the Eley–Rideal mechanism on the SCR reaction was studied. Only the adsorption of NO + O2 on (Fe2.8Mn0.2)1−δO4 was promoted, so the Langmuir–Hinshelwood mechanism predominated over NO conversion on (Fe2.8Mn0.2)1−δO4 especially at lower temperatures. Both the adsorption of NO + O2 and the adsorption of NH3 on (Fe2.5Mn0.5)1−δO4 were obviously promoted, so NO conversion on (Fe2.5Mn0.5)1−δO4 mainly followed the Eley–Rideal mechanism especially at higher temperatures. Both the nitrate route and the over-oxidization of adsorbed ammonia species contributed to the formation of N2O on (Fe2.8Mn0.2)1−δO4 above 140 °C. However, the formation of N2O on (Fe2.5Mn0.5)1−δO4 mainly resulted from the over-oxidization of adsorbed ammonia species. Although the activity of (Fe2.5Mn0.5)1−δO4 was suppressed in the presence of H2O and SO2, the deactivated catalyst can be regenerated after the water washing.
Graphical abstract.Figure optionsDownload full-size imageDownload as PowerPoint slideHighlights► Mn–Fe spinel shows an excellent low temperature SCR activity. ► The SCR activity is promoted with the increase of Mn content. ► The SCR reaction over (Fe2.5Mn0.5)1−δO4 mainly follows the E–R mechanism. ► Catalyst deactivated by SO2 can be regenerated through water washing.
Journal: Applied Catalysis B: Environmental - Volume 110, 2 November 2011, Pages 71–80