CeO2-based catalysts commonly suffer from weak NH3 adsorption,
which leads to inferior activity at medium/low
temperatures for the selective catalytic reduction (SCR) of NO with
NH3. Doping and loading onto a suitable support are two
effective means to promote the NH3 adsorption of CeO2-based materials. However, using traditional trial-and-error
experimental methods via dopants to enhance NH3 adsorption
is generally time-consuming and inefficient. Here, by means of DFT
calculations, we successfully screened two elements (Mo and Cu) for
doping into CeO2. With electronic analysis, the underlying
mechanism of NH3 adsorption properties was well-illustrated.
However, silicalite-1 with a stable ultrahigh specific surface area
was synthesized to support CeO2 for the first time, enabling
CeO2 to have a high accessible reactive surface area. All
the experimental NH3-TPD, in situ DRIFTS, and NO
x
conversion catalytic activity results support our
DFT calculations and the proposed mechanism. Our combined theoretical–experimental
study proposes rational screening strategies for NH3–SCR
from DFT calculations to experimental studies, thus providing insight
into the development of CeO2-based SCR catalysts.