Ceria nanocrystallites with different morphologies and crystal planes were hydrothermally prepared, and the effects of ceria supports on the physicochemical and catalytic properties of Pd/CeO 2 for the CO and propane oxidation were examined. The results showed that the structure and chemical state of Pd on ceria were affected by ceria crystal planes. The Pd species on CeO 2 -R (rods) and CeO 2 -C (cubes) mainly formed Pd x Ce 1−x O 2−σ solid solution with −Pd 2+ −O 2− −Ce 4+ − linkage. In addition, the PdO x nanoparticles were dominated on the surface of Pd/CeO 2 -O (octahedrons). For the CO oxidation, the Pd/CeO 2 -R catalyst showed the highest catalytic activity among three catalysts, its reaction rate reached 2.07 × 10 −4 mol g Pd −1 s −1 at 50 °C, in which CeO 2 -R mainly exposed the ( 110) and (100) facets with low oxygen vacancy formation energy, strong reducibility, and high surface oxygen mobility. TOF of Pd/CeO 2 -R (3.78 × 10 −2 s −1 ) was much higher than that of Pd/CeO 2 -C (6.40 × 10 −3 s −1 ) and Pd/CeO 2 -O (1.24 × 10 −3 s −1 ) at 50 °C, and its activation energy (E a ) was 40.4 kJ/mol. For propane oxidation, the highest reaction rate (8.08 × 10 −5 mol g Pd −1 s −1 at 300 °C) was obtained over the Pd/CeO 2 -O catalyst, in which CeO 2 -O mainly exposed the (111) facet. There are strong surface Ce−O bonds on the ceria (111) facet, which favors the existence of PdO particles and propane activation. The turnover frequency (TOF) of the Pd/CeO 2 -O catalyst was highest (3.52 × 10 −2 s −1 ) at 300 °C and its E a value was 49.1 kJ/mol. These results demonstrate the inverse facet sensitivity of ceria for the CO and propane oxidation over Pd/ ceria.
Sm-Mn mixed oxide catalysts prepared
by the coprecipitation method
were developed, and their catalytic activities were tested for the
selective catalytic reduction (SCR) of NO with ammonia at low temperature.
The results showed that the amount of Sm markedly influenced the activity
of the MnO
x
catalyst for SCR, that the
activity of the Sm-Mn mixed oxide catalyst exhibited a volcano-type
tendency with an increase in the Sm content, and that the appropriate
mole ratio of Sm to Mn in the catalyst was 0.1. In addition, the presence
of Sm in the MnO
x
catalyst can obviously
enhance both water and sulfur dioxide resistances. The effect of Sm
on the physiochemical properties of the Sm-MnO
x
catalyst were investigated by XRD, low-temperature N2 adsorption, XPS, and FE-SEM techniques. The results showed that
the presence of Sm in the Sm-MnO
x
catalyst
can restrain the crystallization of MnO
x
and increase its surface area and the relative content of both Mn4+ and surface oxygen (OS) on the surface of the
Sm-MnO
x
catalyst. NH3-TPD,
NO-TPD, and in situ DRIFT techniques were used to investigate the
absorption of NH3 and NO on the Sm-MnO
x
catalyst and their surface reactions. The results revealed
that the presence of Sm in the Sm0.1-MnO
x
catalyst can increase the absorption amount of NH3 and NO on the catalyst and does not vary the SCR reaction mechanism
over the MnO
x
catalyst: that is, the coexistence
of Eley–Rideal and Langmuir–Hinshelwood mechanisms (bidentate
nitrate is the active intermediate), in which the Eley–Rideal
mechanism is predominant.
Cu/ZSM-5 and Ce doped Cu/ZSM-5 catalysts were prepared by the incipient-wetness-impregnation method, and the effect of Ce doping on the structure and the catalytic performance of the Cu/ZSM-5 catalyst was investigated in detail for the selective catalytic reduction (SCR) of NO with NH 3 . The results showed that the addition of Ce can markedly broaden the operation temperature window of the Cu/ZSM-5 catalyst for NH 3 -SCR and enhance its H 2 O and SO 2 resistance. The presence of Ce promoted an enrichment of copper species (isolated Cu 2+ ions and CuO nanoparticles) on the catalyst surface and the increase in the Lewis acid sites on the surface of the Cu/ZSM-5 catalyst, and strengthened the redox property of the Cu/ZSM-5 catalyst. As a result, Ce-doped Cu/ZSM-5 catalyst possessed the high adsorption ability of NH 3 and nitrite/nitrate, which is propitious to the increase in the reactivity of the Ce-doped Cu/ZSM-5 catalyst. In situ DRIFTS results indicated that the NH 3 -SCR reaction on the Cu/ZSM-5 catalyst and Ce 1 -Cu 4 /ZSM-5 catalysts definitely followed LangmuirHinshelwood mechanisms, and bridged nitrates and bidentate nitrates were the active intermediate.However, Eley-Rideal mechanism can't be confirmed over the Cu/ZSM-5 and Ce 1 -Cu 4 /ZSM-5catalysts.
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