22 research outputs found
Enhanced Activity of Ti-Modified V<sub>2</sub>O<sub>5</sub>/CeO<sub>2</sub> Catalyst for the Selective Catalytic Reduction of NO<sub><i>x</i></sub> with NH<sub>3</sub>
A novel V<sub>2</sub>O<sub>5</sub>/CeTiO<sub><i>x</i></sub> catalyst showed excellent catalytic
performance in the selective
catalytic reduction (SCR) of NO<sub><i>x</i></sub> with
NH<sub>3</sub>. The addition of Ti into V<sub>2</sub>O<sub>5</sub>/CeO<sub>2</sub> enhanced catalytic activity, N<sub>2</sub> selectivity,
and resistance against SO<sub>2</sub> and H<sub>2</sub>O. These catalysts
were also characterized by N<sub>2</sub> adsorption, XRD, XPS, and
H<sub>2</sub>-TPR. The lower crystallinity, more reduced species,
better dispersion of surface vanadium species, and more acid sites
due to the modification of V<sub>2</sub>O<sub>5</sub>/CeO<sub>2</sub> with TiO<sub>2</sub> all improved the NH<sub>3</sub>–SCR
activity significantly. Based on <i>in situ</i> DRIFTS,
it was concluded that the NH<sub>3</sub>–SCR reaction over
V<sub>2</sub>O<sub>5</sub>/CeTiO<sub><i>x</i></sub> and
V<sub>2</sub>O<sub>5</sub>/CeO<sub>2</sub> mainly followed the Eley–Rideal
mechanism
Respective Role of Fe and Mn Oxide Contents for Arsenic Sorption in Iron and Manganese Binary Oxide: An X‑ray Absorption Spectroscopy Investigation
In
our previous studies, a synthesized Fe–Mn binary oxide was
found to be very effective for both AsÂ(V) and AsÂ(III) removal in aqueous
phase, because AsÂ(III) could be easily oxidized to AsÂ(V). AsÂ(III)
oxidation and AsÂ(V) sorption by the Fe–Mn binary oxide may
also play an important role in the natural cycling of As, because
of its common occurrence in the environment. In the present study,
the respective role of Fe and Mn contents present in the Fe–Mn
binary oxide on AsÂ(III) removal was investigated via a direct <i>in situ</i> determination of arsenic speciation using X-ray
absorption spectroscopy. X-ray absorption near edge structure results
indicate that Mn atoms exist in a mixed valence state of +3 and +4
and further confirm that MnO<sub><i>x</i></sub> (1.5 < <i>x</i> < 2) content is mainly responsible for oxidizing AsÂ(III)
to AsÂ(V) through a two-step pathway [reduction of MnÂ(IV) to MnÂ(III)
and subsequent MnÂ(III) to MnÂ(II)] and FeOOH content is dominant for
adsorbing the formed AsÂ(V). No significant AsÂ(III) oxidation by pure
FeOOH had been observed during its sorption, when the system was exposed
to air. The extended X-ray absorption fine structure results reveal
that the As surface complex on both the AsÂ(V)- and AsÂ(III)-treated
sample surfaces is an inner-sphere bidentate binuclear corner-sharing
complex with an As–M (M = Fe or Mn) interatomic distance of
3.22–3.24 Å. In addition, the MnO<sub><i>x</i></sub> and FeOOH contents exist only as a mixture, and no solid solution
is formed. Because of its high effectiveness, low cost, and environmental
friendliness, the Fe–Mn binary oxide would play a beneficial
role as both an efficient oxidant of AsÂ(III) and a sorbent for AsÂ(V)
in drinking water treatment and environmental remediation
Supplementary_Material - Inflammatory Responses are Sex Specific in Chronic Hypoxic–Ischemic Encephalopathy
<p>Supplementary_Material for Inflammatory Responses are Sex Specific in Chronic Hypoxic–Ischemic Encephalopathy by Abdullah Al Mamun, Haifu Yu, Sharmeen Romana, and Fudong Liu in Cell Transplantation</p
The Effects of Mn<sup>2+</sup> Precursors on the Structure and Ozone Decomposition Activity of Cryptomelane-Type Manganese Oxide (OMS-2) Catalysts
The effects of Mn<sup>2+</sup> precursors on the structure and
ozone decomposition activity of cryptomelane-type manganese oxide
(OMS-2) catalysts were investigated under high-humidity conditions.
The OMS-2 catalysts were synthesized using a hydrothermal approach.
Characterization of OMS-2 was carried out using X-ray diffraction
(XRD), scanning electron microscopy (SEM), N<sub>2</sub> physical
adsorption, Raman spectroscopy, X-ray absorption fine structure (XAFS),
H<sub>2</sub> temperature-programmed reduction (H<sub>2</sub>-TPR),
and inductively coupled plasma (ICP) spectroscopy. The OMS-2-Ac synthesized
using MnAc<sub>2</sub> as a Mn<sup>2+</sup> precursor showed the best
catalytic activity for ozone decomposition (∼80%) under RH
= 90% and space velocity of 600000 h<sup>–1</sup> and is a
promising catalyst for purifying waste gases containing ozone under
high-humidity conditions. Acetate groups could prevent the aggregation
of manganese oxide particles, which may introduce more crystalline
defects. On the basis of the characterization results, it is supposed
that the greater surface area and higher amount of Mn<sup>3+</sup> are the main factors that contribute to the excellent performance
of OMS-2-Ac. This study can improve our understanding of ozone decomposition
on OMS-2 catalysts and serve as a guide in using OMS-2 for ozone removal
NH<sub>3</sub>‑SCR Performance of Fresh and Hydrothermally Aged Fe-ZSM‑5 in Standard and Fast Selective Catalytic Reduction Reactions
Hydrothermal stability
is one of the challenges for the practical
application of Fe-ZSM-5 catalysts in the selective catalytic reduction
(SCR) of NO with NH<sub>3</sub> (NH<sub>3</sub>-SCR) for diesel engines.
The presence of NO<sub>2</sub> in the exhaust gases can enhance the
deNOx activity because of the fast SCR reaction. In this work, a Fe-ZSM-5
catalyst was prepared by a solid-state ion-exchange method and was
hydrothermally deactivated at 800 °C in the presence of 10% H<sub>2</sub>O. The activity of fresh and hydrothermal aged Fe-ZSM-5 catalysts
was investigated in standard SCR (NO<sub>2</sub>/NO<i>x</i> = 0) and in fast SCR with NO<sub>2</sub>/NO<i>x</i> =
0.3 and 0.5. In standard SCR, hydrothermal aging of Fe-ZSM-5 resulted
in a significant decrease of low-temperature activity and a slight
increase in high-temperature activity. In fast SCR, NO<i>x</i> conversion over aged Fe-ZSM-5 was significantly increased but was
still lower than that over fresh catalyst. Additionally, production
of N<sub>2</sub>O in fast SCR was much more apparent over aged Fe-ZSM-5
than over fresh catalyst. We propose that, in fast SCR, the rate of
key reactions related to NO is slower over aged Fe-ZSM-5 than over
fresh catalyst, thus increasing the probabilities of side reactions
involving the formation of N<sub>2</sub>O
Engineering a PtCu Alloy to Improve N<sub>2</sub> Selectivity of NH<sub>3</sub>–SCO over the Pt/SSZ-13 Catalyst
Improving
the N2 selectivity is always a great
challenge
for the selective catalytic oxidation of ammonia (NH3–SCO)
over noble-metal-based (especially Pt) catalysts. In this work, Cu
as an efficient promoter was introduced into the Pt/SSZ-13 catalyst
to significantly improve the N2 selectivity of the NH3–SCO reaction. A PtCu alloy was formed in the PtCu/SSZ-13
catalyst, as confirmed by X-ray diffraction, transmission electron
microscopy, energy dispersive spectrometry mapping, and X-ray absorption
spectroscopy results. As indicated by the X-ray photoelectron spectroscopy
analysis, the Pt species in the alloyed PtCu nanoparticle was mainly
present in the electron-rich state on PtCu/SSZ-13, while the electron-deficient
Cu and isolated Cu2+ species were both present on the surface
of PtCu/SSZ-13. Due to such a unique alloyed structure with an altered
oxidation state, the N2 selectivity of NH3–SCO
on the PtCu/SSZ-13 catalyst was remarkably improved, while the NH3–SCO activity was kept comparable to that on Pt/SSZ-13.
The reaction path was changed from the NH mechanism on Pt/SSZ-13 to
both NH and internal selective catalytic reduction mechanisms on the
PtCu/SSZ-13 catalyst, which was considered the main reason for the
enhanced N2 selectivity. This work provides a new route
to synthesize efficient alloy catalysts for optimizing the N2 selectivity of NH3–SCO for NH3 slip
control in diesel exhaust purification
Nature of Ag Species on Ag/γ-Al<sub>2</sub>O<sub>3</sub>: A Combined Experimental and Theoretical Study
The nature of silver species on Ag/Al<sub>2</sub>O<sub>3</sub> catalysts
with different silver loadings was studied by photoelectron spectroscopy
(XPS) and X-ray absorption near-edge spectroscopy (XANES) and extended
X-ray absorption fine structure spectroscopy (EXAFS) combined with
theoretical calculation (DFT). On the basis of selective catalytic
reduction of NO<sub><i>x</i></sub> by ethanol experiments,
it was found that the optimum silver content varies from 1 wt % to
2 wt %. The supported silver species are predominated by +1 oxidation
state ions attached to surface oxygen atoms (Ag–O) under low
silver loading of 2 wt %, which play a crucial role during the HC-SCR
process. An Ag–Ag shell emerged clearly in analysis of EXAFS
data when silver loading was increased to 2 wt %, which was beneficial
for low-temperature activity. The theoretical models for Ag<sub>n</sub><sup>δ+</sup> species (1 ≤ <i>n</i> ≤
4, both ions and oxidized silver clusters) on alumina were consistent
with the coordination structure analysis by EXAFS. The predominant
silver ions are most likely stabilized at isolated tetrahedral Al
sites (Ag–O–Al<sub>IVb</sub>) on the γ-Al<sub>2</sub>O<sub>3</sub> (110) surface. However, the most reactive silver
ion seems to be anchored on a tricoordinate Al<sub>III</sub> site
(Ag–O–Al<sub>III</sub>). Density of states analysis
revealed that the Ag–O–Al<sub>III</sub> entity might
be a very active silver species in terms of the hybridization of Ag,
O, and Al orbitals to promote its catalytic activity
Significant Promotion Effect of Mo Additive on a Novel Ce–Zr Mixed Oxide Catalyst for the Selective Catalytic Reduction of NO<sub><i>x</i></sub> with NH<sub>3</sub>
A novel Mo-promoted Ce–Zr
mixed oxide catalyst prepared by a homogeneous precipitation method
was used for the selective catalytic reduction (SCR) of NO<sub><i>x</i></sub> with NH<sub>3</sub>. The optimal catalyst showed
high NH<sub>3</sub>-SCR activity, SO<sub>2</sub>/H<sub>2</sub>O durability,
and thermal stability under test conditions. The addition of Mo inhibited
growth of the CeO<sub>2</sub> particle size, improved the redox ability,
and increased the amount of surface acidity, especially the Lewis
acidity, all of which were favorable for the excellent NH<sub>3</sub>-SCR performance. It is believed that the catalyst is promising for
the removal of NO<sub><i>x</i></sub> from diesel engine
exhaust
Excellent Performance of One-Pot Synthesized Cu-SSZ-13 Catalyst for the Selective Catalytic Reduction of NO<sub><i>x</i></sub> with NH<sub>3</sub>
Cu-SSZ-13
samples prepared by a novel one-pot synthesis method
achieved excellent NH<sub>3</sub>–SCR performance and high
N<sub>2</sub> selectivity from 150 to 550 °C after ion exchange
treatments. The selected Cu<sub>3.8</sub>-SSZ-13 catalyst was highly
resistant to large space velocity (800 000 h<sup>–1</sup>) and also maintained high NO<sub><i>x</i></sub> conversion
in the presence of CO<sub>2</sub>, H<sub>2</sub>O, and C<sub>3</sub>H<sub>6</sub> in the simulated diesel exhaust. Isolated Cu<sup>2+</sup> ions located in three different sites were responsible for its excellent
NH<sub>3</sub>–SCR activity. Primary results suggest that the
one-pot synthesized Cu-SSZ-13 catalyst is a promising candidate as
an NH<sub>3</sub>–SCR catalyst for the NO<sub><i>x</i></sub> abatement from diesel vehicles