A Cu/SSZ-13
catalyst containing predominately Z2Cu sites
is prepared. Using FTIR spectroscopy, two nonsteady-state measurements,
(1) continuous NO titration of an NH3 saturated catalyst
and (2) intermittent NO on/off cycles during quasi-steady state (i.e.,
NO perturbation), are conducted to shed light on active sites, reaction
intermediates, and possible reaction mechanisms. During continuous
NO titration, a strong NH3 inhibition effect is found,
where Cu active sites containing NH3 ligands are less active
than Cu sites depleted of NH3 ligands. In the NO perturbation
experiments, it is demonstrated that NO+NH3 interactions
lead to formation of Brønsted acid sites, which further interact
with NH3 to form NH4
+. Perturbation
measurements, using ND3 to replace NH3 in order
to distinguish ammonia and nitrate vibrations, further show that NH4NO3 and other surface nitrates are not involved
in the SCR process under typical low-temperature quasi-steady-state
conditions.
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