ACS Catalysis,
Journal Year:
2024,
Volume and Issue:
unknown, P. 956 - 966
Published: Dec. 31, 2024
Dynamic
structural
changes
in
the
reactive
environment
often
lead
to
catalyst
deactivation
thermal-catalysis
field.
Taking
advantage
of
dynamic
bulk
phases,
interfaces,
and
surface
structures
design
highly
active
catalysts
is
a
unique
but
important
strategy.
Herein,
we
report
supersaturated
ceria
solid
solution
enabling
styrene
yield
91.8%
over
extended
redox
cycles
at
430
°C
oxidative
dehydrogenation
(ODH)
ethylbenzene.
In-situ
characterizations
reveal
that
oxygen
anions
(O2–)
transition-metal
cations
(Fe
Mn)
reversibly
shuttle
through
(bulk
↔
surface)
K–Ce0.47Fe0.2Mn0.33O2−δ
during
ODH
process.
The
acts
as
cations/oxygen
reservoir,
creating
atomic
interfaces
K–Fe–O/K–Mn–O
an
gateway
for
efficient
ethylbenzene
ODH.
findings
concerning
formation
cations,
lattice
migration,
coupling
between
donation
catalytic
reactions
offer
new
strategies
designing
high-performance
catalysts.
ChemCatChem,
Journal Year:
2024,
Volume and Issue:
unknown
Published: June 5, 2024
Abstract
The
direct
conversion
of
cheap
and
widely
available
C
1
−C
3
alkanes
in
natural
gas/shale
gas
into
building
blocks
for
the
chemical
industry
is
highly
attractive
from
an
environmental
perspective
as
a
replacement
current
oil‐based
processes.
Due
to
high
inertness
these
alkanes,
but
reactivity
desired
reaction
products,
which
are
easily
involved
non‐selective
sequential
reactions,
ongoing
research
activities
focused
on
controlling
product
selectivity
through
catalyst
design
and/or
reactor
operation.
In
this
context,
we
have
critically
analyzed
studies
dealing
with
effect
steam
or
liquid
water
activity
and,
particular,
CH
4
,
2
H
6
8
2+
‐hydrocarbons,
formaldehyde,
methanol,
ethylene,
acetic
acid,
propene.
addition,
our
personal
views
possible
future
developments
also
given.
Physical review. E,
Journal Year:
2024,
Volume and Issue:
110(3)
Published: Sept. 26, 2024
Kinetics
of
heterogeneous
catalytic
reactions
are
often
complicated
by
various
factors,
and
from
the
perspective
statistical
physics
development
corresponding
models
is
frequently
challenging
especially
in
case
practically
important
alloy
catalysts.
To
extend
basics
this
area,
I
use
a
generic
kinetic
model
N_{2}
formation
NO
reaction
with
such
species
as
CO
or
H_{2}.
The
focus
on
surface
bimetallic
low
integral
fraction
one
metals
so
that
formed
only
at
surface.
main
goal
to
illustrate
specifics
kinetics
clarify
accuracy
approximations
which
inevitable
for
analysis
systems.
key
results
follows.
(i)
In
baseline
one-metal
Langmuir-type
equations,
predicts
existence
optimal
adsorbate
binding
energy
maximal
rate.
(ii)
With
suitable
substitution
symbols,
equations
employed
uniform
[item
(i)]
can
be
used
mean-field
description
random
alloy.
particular,
maximum
dependence
rate
converted
respect
composition.
(iii)
random-alloy
have
been
described
exactly.
lower
somewhat
smeared
compared
predicted
approximation
an
monometallic
catalyst.
(iv)
scrutinized
also
two-dimensional
(2D)
segregation
metal
atoms
limits
slow
rapid
diffusion
between
spots.
shown
qualitatively
different
these
case.
(v)
thermodynamic
criteria
2D
derived
well.
ACS Catalysis,
Journal Year:
2024,
Volume and Issue:
unknown, P. 956 - 966
Published: Dec. 31, 2024
Dynamic
structural
changes
in
the
reactive
environment
often
lead
to
catalyst
deactivation
thermal-catalysis
field.
Taking
advantage
of
dynamic
bulk
phases,
interfaces,
and
surface
structures
design
highly
active
catalysts
is
a
unique
but
important
strategy.
Herein,
we
report
supersaturated
ceria
solid
solution
enabling
styrene
yield
91.8%
over
extended
redox
cycles
at
430
°C
oxidative
dehydrogenation
(ODH)
ethylbenzene.
In-situ
characterizations
reveal
that
oxygen
anions
(O2–)
transition-metal
cations
(Fe
Mn)
reversibly
shuttle
through
(bulk
↔
surface)
K–Ce0.47Fe0.2Mn0.33O2−δ
during
ODH
process.
The
acts
as
cations/oxygen
reservoir,
creating
atomic
interfaces
K–Fe–O/K–Mn–O
an
gateway
for
efficient
ethylbenzene
ODH.
findings
concerning
formation
cations,
lattice
migration,
coupling
between
donation
catalytic
reactions
offer
new
strategies
designing
high-performance
catalysts.
