The Conundrum of “Pair Sites” in Langmuir–Hinshelwood Reaction Kinetics in Heterogeneous Catalysis
ACS Catalysis,
Journal Year:
2024,
Volume and Issue:
14(13), P. 10260 - 10270
Published: June 21, 2024
Understanding
reaction
kinetics
is
crucial
for
designing
and
applying
heterogeneous
catalytic
processes
in
chemical
energy
conversion.
Here,
we
revisit
the
Langmuir–Hinshelwood
(L-H)
kinetic
model
bimolecular
surface
reactions,
originally
formulated
metal
catalysts,
assuming
immobile
adsorbates
on
neighboring
pair
sites,
with
rate
varying
linearly
density
of
sites
(sites
per
unit
area);
r
∝
[*]o1.
Supported
oxide
however,
offer
systematic
control
over
[*]o
through
variation
active
two-dimensional
loading
submonolayer
region.
Various
reactions
catalyzed
by
supported
oxides
are
analyzed,
such
as
VOx
including
methanol
oxidation,
oxidative
dehydrogenation
propane
ethane,
SO2
oxidation
to
SO3,
propene
acrolein,
n-butane
maleic
anhydride,
selective
reduction
nitric
ammonia.
The
analysis
reveals
diverse
dependencies
these
[*]on,
where
n
equals
1
a
unimolecular
rate-determining
step
2
those
rate-limiting
or
exchange
more
than
electrons.
We
propose
refraining
from
priori
assumptions
about
nature
adsorbate
behavior,
advocating
instead
data-driven
elucidation
based
coverage,
etc.
Additionally,
recent
studies
mechanisms
have
shed
light
nonadjacent
catalyzing
contrast
traditional
requirement
adjacent/pair
sites.
These
findings
underscore
need
nuanced
approach
modeling
catalysis,
especially
encouraging
reliance
experimental
data
idealized
that
often
difficult
justify.
Language: Английский
Influence of Anion in Tuning of the Crystal Structure, Optical and Redox Properties of Ce3+/4+-Based Materials
Anees A. Ansari,
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Ruichan Lv,
No information about this author
Shafiya Mohammad
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et al.
Ceramics International,
Journal Year:
2025,
Volume and Issue:
unknown
Published: April 1, 2025
Language: Английский
Practical and scalable hydrogenation of nitro compounds using palladium-based nanocatalyst under ambient conditions
Catalysis Today,
Journal Year:
2024,
Volume and Issue:
442, P. 114940 - 114940
Published: July 11, 2024
Language: Английский
Sequential hydrogenation enhanced by bidirectional hydrogen spillover over cascade catalyst
Shuai Wang,
No information about this author
Daowei Gao,
No information about this author
Rongyao Wang
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et al.
AIChE Journal,
Journal Year:
2025,
Volume and Issue:
unknown
Published: Feb. 7, 2025
Abstract
Formulating
a
synergetic
strategy
to
govern
the
catalytic
function
of
dual
metal
sites
is
paramount
achieving
precise
control
cascade
reactions.
Herein,
we
construct
dual‐site
catalyst
with
Pt
and
Ru
species
localized
in
micropores
mesopores
zeolite,
respectively.
This
architecture
enables
spatial
separation
nanoscale
proximity.
Compared
mono/bi‐metallic
catalysts,
this
4.4–9.5
times
enhancement
activity
during
sequential
hydrogenation
nitroaromatics
cyclohexylamine.
Particularly,
bidirectional
hydrogen
spillover
assists
between
confirmed,
where
active
migrates
from
less
adjacent
first/second
step
reaction.
Characterization
studies
density
functional
theory
calculations
suggest
that
enhances
coverage
at
for
each
step,
thereby
reducing
energy
barrier
rate‐controlling
step.
intriguing
phenomenon
reveals
mechanism
accelerated
presents
an
opportunity
devising
immensely
efficient
catalysts.
Language: Английский
Modulation of active site in CePO4/PtCo via multiple synergistic effects for enhanced nitroaromatic hydrogenation
Shuai Wang,
No information about this author
Zhenshuai Wu,
No information about this author
Changxu Wang
No information about this author
et al.
Journal of Colloid and Interface Science,
Journal Year:
2025,
Volume and Issue:
695, P. 137776 - 137776
Published: May 2, 2025
Language: Английский
Harnessing Phase-Dependent Acidity and Redox Activity of Ru-Decorated CePO4 Catalysts for Biofuel Production from Lignin Model Compounds and Lignin Bio-oil
ACS Sustainable Chemistry & Engineering,
Journal Year:
2025,
Volume and Issue:
unknown
Published: May 15, 2025
Language: Английский
Coordinating cracking and hydrogenation of polyethylene waste via acid-metal site isolation for selective hydrocarbon production
Chemical Engineering Science,
Journal Year:
2025,
Volume and Issue:
unknown, P. 121882 - 121882
Published: May 1, 2025
Language: Английский
One-Pot Synthesis of Magnetic Core-Shell Fe3O4@C Nanospheres with Pt Nanoparticle Immobilization for Catalytic Hydrogenation of Nitroarenes
Jun Qiao,
No information about this author
Yang Gao,
No information about this author
Kai Zheng
No information about this author
et al.
Applied Sciences,
Journal Year:
2025,
Volume and Issue:
15(10), P. 5773 - 5773
Published: May 21, 2025
Magnetic
materials
with
intriguing
structural
and
functional
modifications
demonstrate
broad
application
potential
in
various
fields,
including
drug
delivery,
absorption,
extraction,
separation,
catalysis.
In
particular,
the
catalytic
hydrogenation
of
functionalized
organic
nitro
compounds
represents
a
significant
research
focus
contemporary
catalysis
studies.
A
facile
synthesis
Fe3O4@C–Pt
core-shell
nanocatalysts
was
developed
this
work
through
sequential
process
involving
(1)
one-pot
hydrothermal
followed
by
N2-annealing
to
obtain
Fe3O4@C
core
(2)
subsequent
solvothermal
deposition
platinum
nanoparticles.
Comprehensive
characterization
performed
using
FT-IR,
XRD,
Raman
spectroscopy,
TEM,
XPS,
BET
surface
area
analysis,
TGA,
VSM
techniques.
The
resulting
magnetic
exhibited
uniformly
dispersed
Pt
nanoparticles
demonstrated
exceptional
performance
nitroarene
reactions.
Remarkably,
system
showed
excellent
group
tolerance
across
all
20
substituted
nitroarenes,
consistently
yielding
corresponding
aromatic
amine
products
>93%
conversion
efficiency.
Furthermore,
responsiveness
enabled
convenient
catalyst
recovery
simple
maintained
activity
over
10
consecutive
reuse
cycles
without
degradation.
Language: Английский
Pt Nanoclusters Supported on Ti3C2Tx Nanosheets for the Selective Hydrogenation of Halogenated Nitroarenes under Mild Conditions
Xiangbin Li,
No information about this author
Wei Gao,
No information about this author
Lu Li
No information about this author
et al.
ACS Applied Nano Materials,
Journal Year:
2024,
Volume and Issue:
7(12), P. 14540 - 14548
Published: June 7, 2024
We
successfully
constructed
an
ultrathin
Ti3C2Tx
supported
Pt
nanocluster
catalyst
for
highly
selective
and
efficient
hydrogenation
of
p-chloronitrobenzene
(p-CNB)
to
p-chloroaniline
(p-CAN)
under
mild
conditions
(30
°C,
0.1
MPa
H2).
The
Pt/Ti3C2Tx
displayed
a
very
high
conversion
(>99%)
selectivity
(>99%).
In
addition,
higher
reaction
rate
(41
mol
h–1
g–1)
was
obtained
in
comparison
with
the
previously
reported
catalysts.
excellent
catalytic
activity
attributed
strong
metal–support
interactions
between
nanoclusters
support,
which
electrons
were
transferred
from
sites,
affording
electron
density
active
sites.
Moreover,
electrostatic
repulsion
C–Cl
moiety
sites
inhibited
dechlorination
process.
also
exhibited
performance
substrate
scope
(reducible
heterocyclics
such
as
pyridine
phthalimide),
stability
(10th
cycles,
>99%
98%),
gram-scale
(99%
yield,
1.89
g).
This
work
will
promote
research
constructing
noble
metal-based
catalysts
halogenated
nitroarenes.
Language: Английский