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.
Ruthenium (Ru) nanoparticles (∼3 nm) with mass loading ranging from 1.5 to 3.2 wt % are supported on a reducible substrate, cerium dioxide (CeO, the resultant sample is called Ru/CeO), for application in the catalytic combustion of propane. Because of the unique electronic configuration of CeO, a strong metal-support interaction is generated between the Ru nanoparticles and CeO to stabilize Ru nanoparticles for oxidation reactions well. In addition, the CeO host with high oxygen storage capacity can provide an abundance of active oxygen for redox reactions and thus greatly increases the rates of oxidation reactions or even modifies the redox steps. As a result of such advantages, a remarkably high performance in the total oxidation of propane at low temperature is achieved on Ru/CeO. This work exemplifies a promising strategy for developing robust supported catalysts for short-chain volatile organic compound removal.
Tailoring
the interfaces between active metal centers and supporting
materials is an efficient strategy to obtain a superior catalyst for
a certain reaction. Herein, an active interface between Ru and CeO2 was identified and constructed by adjusting the morphology
of CeO2 support, such as rods (R), cubes (C), and octahedra
(O), to optimize both the activity and the stability of Ru/CeO2 catalyst for propane combustion. We found that the morphology
of CeO2 support does not significantly affect the chemical
states of Ru species but controls the interaction between the Ru and
CeO2, leading to the tuning of oxygen vacancy in the CeO2 surface around the Ru–CeO2 interface. The
Ru/CeO2 catalyst possesses more oxygen vacancy when CeO2-R with predominantly exposed CeO2{110} surface
facets is used, providing a higher ability to adsorb and activate
oxygen and propane. As a result, the Ru/CeO2-R catalyst
exhibits higher catalytic activity and stability for propane combustion
compared with the Ru/CeO2-C and Ru/CeO2-O catalysts.
This work highlights a new strategy for the design of efficient metal/CeO2 catalysts by engineering morphology and associated surface
facet of CeO2 support for the elimination of light alkane
pollutants and other volatile organic compounds.
Supported gold (Au) nanocatalysts hold great promise for heterogeneous catalysis; however, their practical application is greatly hampered by poor thermodynamic stability. Herein, a general synthetic strategy is reported where discrete metal nanoparticles are made resistant to sintering, preserving their catalytic activities in high-temperature oxidation processes. Taking advantage of the unique coating chemistry of dopamine, sacrificial carbon layers are constructed on the material surface, stabilizing the supported catalyst. Upon annealing at high temperature under an inert atmosphere, the interactions between support and metal nanoparticle are dramatically enhanced, while the sacrificial carbon layers can be subsequently removed through oxidative calcination in air. Owing to the improved metal-support contact and strengthened electronic interactions, the resulting Au nanocatalysts are resistant to sintering and exhibit excellent durability for catalytic combustion of propylene at elevated temperatures. Moreover, the facile synthetic strategy can be extended to the stabilization of other supported catalysts on a broad range of supports, providing a general approach to enhancing the thermal stability and sintering resistance of supported nanocatalysts.
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