A comparative study was performed to investigate the
NH3-selective catalytic reduction (SCR) reaction activity
of Cu-SSZ-13
zeolites having Si/Al ratios (SARs) of 5, 18, and 30. Remarkably,
the Cu-SSZ-13 zeolite catalysts exhibited completely opposite behaviors
as a function of SAR under standard SCR (SSCR) and fast SCR (FSCR)
reaction atmospheres. Under SSCR conditions, the NO
x
conversion increased as expected with the decreasing SAR.
Under FSCR conditions, however, the NO
x
conversion decreased as the SAR decreased, contrary to expectations.
In this study, based on characterization of the catalysts by X-ray
diffraction, transmission electron microscopy, electron paramagnetic
resonance, H2-temperature-programmed reduction, temperature-programmed
desorption, and diffuse reflectance infrared Fourier transform spectroscopy,
together with theoretical calculations, the authors found that the
amount of Brønsted acid sites goes up while the SAR goes down,
leading to an increase in the accumulation of NH4NO3 under FSCR reaction conditions. Moreover, the accumulated
NH4NO3 is of greater stability for those low
SAR Cu-SSZ-13 catalysts. These two reasons cause the FSCR performance
of Cu-SSZ-13 to decrease with a decrease in SAR. As a result, the
NO2 effect on SCR activity changes from promotion to inhibition
as the SAR decreases.