G. Delahay et al., Selective catalytic reduction of NO with NH3 in presence of oxygen over copper exchanged NaY zeolites, J CHIM PHYS, 96(3), 1999, pp. 443-454
A series of Cu-NaY, prepared by ion-exchange and impregnation, was characte
rized by temperature programmed reduction (TPR) and oxidation (TPO) and als
o tested for the selective catalytic reduction (SCR) of NO by NH3 in an oxy
gen rich atmosphere, and in the NH3 oxidation. From the TPR profiles, the a
mount of isolated Cu2+ species, [Cu-O-Cu](2+) dimer species and CuO aggrega
tes were evaluated, The TPO of Cu+-NaY issued from the reduction of Cu2+-Na
Y by NH3, shows that NO alone cannot perform the reoxidation of Cu+ to Cu2 below 873 K, but this reaction is enhanced in the presence of NO/O-2 with
respect to O-2 alone. The SCR of NO with NH3 in 3% O-2 leads to three peaks
in the NO conversion curve, when conducted in the temperature programmed r
eaction mode. The first peak is a transient effect due to the impossible re
generation of Cu+ to Cu2+. As soon as the reoxydation of Cu+ to Cu2+ become
feasible by NO/O-2, the reaction starts (second peak) and would be related
to the presence of copper in supercages. The formation of N2O in this temp
erature range occurs in the presence of copper oxide aggregates. The final
conversion, at high temperature leads to 100% conversion of NO and is due t
o a better oxidation of Cu+ by NO/O-2 and O-2 alone. In this latter tempera
ture range, the formation of N2O comes mainly from the reaction between NO
and NH3 in the sodalite cavities but also from the oxidation of NH3.