A series of Ce-modified
Cu–FeO
x
catalysts were synthesized
with a sol–gel hydrothermal method.
These catalysts contained different molar ratios of Ce, Cu, and Fe,
and were applied to the process of NO catalytic removal by CO (CO-deNO).
The physical and chemical parameters of the samples were characterized
by XRD, XPS, ESR, H2-TPR, NO-TPO, and NO-TPD techniques.
Moreover, the CO-deNO mechanisms for the representative catalysts
were investigated by in situ DRIFTS. The SO2 and H2O resistances, and their corresponding mechanisms, were also
systematically investigated. The catalytic activity testing shows
that the optimized molar ratio of Cu, Ce, and Fe is 1:0.5:1.5. At
this ratio, the CO-deNO efficiency is highest, but the N2O selectivity is also relatively high. Increasing the Fe percentage
could reduce the N2O concentration. The characterization
indicates that, at the optimized ratio, the interaction between Fe
and Cu is at its strongest, which could increase the formation probability
of surface synergistic oxygen vacancies. The Ce existing in the catalysts
plays a key role in the adsorption of NO and CO. Moreover, the increasing
percentage of Fe could enhance the adsorption and dissociation of
NO, and promote the evolution of CO, which can compensate for the
effects of the weaker interaction. The NO and CO evolution pathway
runs as follows: NO → M–NO2 → NO2
– → M–N2O/NO3
– → N2O/N2;
CO → COO– → CO3
2– → CO2. The H2O and SO2 resistance
tests suggest that the appropriate incremental increase in Fe percentage
will increase the SO2 or H2O resistance, with
the underlying mechanism being that Fe inhibits the formation of sulfates
and produces more water adsorption sites, and the increasing Fe percentage
would optimize the pore structure.