6 research outputs found
A Highly Effective Catalyst of Sm-MnO<sub><i>x</i></sub> for the NH<sub>3</sub>‑SCR of NO<sub><i>x</i></sub> at Low Temperature: Promotional Role of Sm and Its Catalytic Performance
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<sub><i>x</i></sub> 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<sub><i>x</i></sub> catalyst can obviously
enhance both water and sulfur dioxide resistances. The effect of Sm
on the physiochemical properties of the Sm-MnO<sub><i>x</i></sub> catalyst were investigated by XRD, low-temperature N<sub>2</sub> adsorption, XPS, and FE-SEM techniques. The results showed that
the presence of Sm in the Sm-MnO<sub><i>x</i></sub> catalyst
can restrain the crystallization of MnO<sub><i>x</i></sub> and increase its surface area and the relative content of both Mn<sup>4+</sup> and surface oxygen (O<sub>S</sub>) on the surface of the
Sm-MnO<sub><i>x</i></sub> catalyst. NH<sub>3</sub>-TPD,
NO-TPD, and in situ DRIFT techniques were used to investigate the
absorption of NH<sub>3</sub> and NO on the Sm-MnO<sub><i>x</i></sub> catalyst and their surface reactions. The results revealed
that the presence of Sm in the Sm<sub>0.1</sub>-MnO<sub><i>x</i></sub> catalyst can increase the absorption amount of NH<sub>3</sub> and NO on the catalyst and does not vary the SCR reaction mechanism
over the MnO<sub><i>x</i></sub> 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
Total Oxidation of Propane over a Ru/CeO<sub>2</sub> Catalyst at Low Temperature
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<sub>2</sub>, the resultant sample is called Ru/CeO<sub>2</sub>), for application in the catalytic combustion of propane.
Because of the unique electronic configuration of CeO<sub>2</sub>,
a strong metal–support interaction is generated between the
Ru nanoparticles and CeO<sub>2</sub> to stabilize Ru nanoparticles
for oxidation reactions well. In addition, the CeO<sub>2</sub> 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<sub>2</sub>. This
work exemplifies a promising strategy for developing robust supported
catalysts for short-chain volatile organic compound removal
Incorporating Rich Mesoporosity into a Ceria-Based Catalyst via Mechanochemistry
Ceria-based materials
possessing mesoporous structures afford higher
activity than the corresponding bulk materials in CO oxidation and
other catalytic applications, because of the wide pore channel and
high surface area. The development of a direct, template-free, and
scalable technology for directing porosity inside ceria-based materials
is highly welcome. Herein, a family of mesoporous transition-metal-doped
ceria catalysts with specific surface areas up to 122 m<sup>2</sup> g<sup>–1</sup> is constructed by mechanochemical grinding.
No templates, additives, or solvents are needed in this process, while
the mechanochemistry-mediated restructuring and the decomposing of
the organic group led to plentiful mesopores. Interestingly, the copper
species are evenly dispersed in the ceria matrix at the atomic scale,
as observed in high resolution scanning transmission electron microscopy
in high angle annular dark field. The copper-doped ceria materials
show good activity in the CO oxidation
Highly Efficient Oxidation of Propane at Low Temperature over a Pt-Based Catalyst by Optimization Support
Pt-based catalysts have attracted widespread attention
in environmental
protection applications, especially in the catalytic destruction of
light alkane pollutants. However, developing a satisfying platinum
catalyst with high activity, excellent water-resistance, and practical
suitability for hydrocarbon combustion at low temperature is challenging.
In this study, the Pt catalyst supported on the selected Nb2O5 oxide exhibited an efficient catalytic activity in
propane oxidation and exceeded that of most catalysts reported in
the literature. More importantly, the Pt/Nb2O5 catalyst maintained excellent activity and durability even after
high-temperature aging at 700 °C and under harsh working conditions,
such as a certain degree of moisture, high space velocity, and composite
pollutants. The excellent performance of the Pt/Nb2O5 catalyst was attributed to the abundant metallic Pt species
stabilized on the surface of Nb2O5, which prompted
the C–H bond dissociation ability as the rate-determining step.
Furthermore, propane was initially activated via oxidehydrogenation
and followed the acrylate species path as a more efficient propane
oxidation path on the Pt/Nb2O5 surface. Overall,
Pt/Nb2O5 can be considered a promising catalyst
for the catalytic oxidation of alkanes from industrial sources and
could provide inspiration for designing superb catalysts for the oxidation
of light alkanes
Low-Temperature Methane Combustion over Pd/H-ZSM-5: Active Pd Sites with Specific Electronic Properties Modulated by Acidic Sites of H‑ZSM‑5
Pd/H-ZSM-5
catalysts could completely catalyze CH<sub>4</sub> to
CO<sub>2</sub> at as low as 320 °C, while there is no detectable
catalytic activity for pure H-ZSM-5 at 320 °C and only a conversion
of 40% could be obtained at 500 °C over pure H-ZSM-5. Both the
theoretical and experimental results prove that surface acidic sites
could facilitate the formation of active metal species as the anchoring
sites, which could further modify the electronic and coordination
structure of metal species. PdO<sub><i>x</i></sub> interacting
with the surface Brönsted acid sites of H-ZSM-5 could exhibit
Lewis acidity and lower oxidation states, as proven by the XPS, XPS
valence band, CO-DRIFTS, pyridine FT-IR, and NH<sub>3</sub>-TPD data.
Density functional theory calculations suggest PdO<sub><i>x</i></sub> groups to be the active sites for methane combustion, in the
form of [AlO<sub>2</sub>]ÂPdÂ(OH)-ZSM-5. The stronger Lewis acidity
of coordinatively unsaturated Pd and the stronger basicity of oxygen
from anchored PdO<sub><i>x</i></sub> species are two key
characteristics of the active sites ([AlO<sub>2</sub>]ÂPdÂ(OH)-ZSM-5)
for methane combustion. As a result, the PdO<sub><i>x</i></sub> species anchored by Brønsted acid sites of H-ZSM-5 exhibit
high performance for catalytic combustion of CH<sub>4</sub> over Pd/H-ZSM-5
catalysts
Revealing the Size Effect of Ceria Nanocube-Supported Platinum Nanoparticles in Complete Propane Oxidation
The
elimination of propane is one of the key tasks in
reducing
volatile organic compounds (VOCs) and automotive exhaust emissions.
The platinum nanoparticle (NP) is a promising catalyst for propane
oxidation, while the study of its structural characteristics and functionality
remains in its infancy. In this work, we synthesized the nanocubes
CeO2 with a well-defined (100) facet supporting Pt NPs
with various sizes, from 1.3 to 7 nm, and systematically investigated
the effect of the Pt size on complete propane oxidation efficiency.
In particular, CeO2(100) supported Pt NPs smaller than
4 nm promote the formation of positively charged Pt sites, which hinder
the adsorption and activation of propane and reduce the intrinsic
activity for propane oxidation. Consequently, within this size range,
the catalytic performance is primarily influenced by the electronic
state of the Pt species, with metallic Pt being identified as the
active site for the reaction. Conversely, as the particle size exceeds
4 nm, metallic Pt particles become dominant and the geometric structure
starts to influence the activity as well. Such entanglement of electronic
and geometric factors gives rise to a volcano relationship between
reaction rates and Pt particle sizes ranging from 1.3 to 7 nm, while
an increased correlation can be observed between the turnover frequencies
and the particle sizes in this range. This knowledge can guide the
synthesis of highly active catalysts, enabling the efficient oxidation
of VOCs with reduced precious metal loadings