Abstract

The reaction mechanisms of selective catalytic reduction (SCR) of N 2 O with CH 4 and N 2 O decomposition over Fe ion-exchanged zeolite catalysts (Fe-BEA, Fe-MFI) were studied. In O 2 -TPD studies, we observed new desorption peaks from Fe-BEA catalyst after N 2 O treatment. However, the new adsorbed oxygen species hardly reacted with CH 4 . This indicates that coexistence of N 2 O and CH 4 is necessary for the high SCR activity. In infrared (FTIR) spectroscopy, most of Fe-OH species (the OH group on Fe ion species) took part in the N 2 O+CH 4 reaction, and the methoxy and formate species were formed. The methoxy species were oxidized with N 2 O more rapidly than O 2 , while the formate species were oxidized with both N 2 O and O 2 at almost the same rate. The isotopic tracer study using 18 O(a) showed that O 2 formation during N 2 O decomposition proceeds via Eley-Rideal (ER) mechanism. A possible mechanism is discussed in terms of active oxygen species formed from N 2 O, which may play an important role in the activation/oxidation of CH 4 at initial steps.

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