ACS Applied Materials & Interfaces,
Год журнала:
2024,
Номер
unknown
Опубликована: Ноя. 25, 2024
The
catalytic
conversion
of
CO2
to
CO
through
hydrogenation
has
emerged
as
a
promising
strategy
for
utilization,
given
that
serves
valuable
C1
platform
compound
synthesizing
liquid
fuels
and
chemicals.
However,
the
predominant
formation
CH4
via
deep
over
Ru-based
catalysts
poses
challenges
in
achieving
selective
production.
High
reaction
temperatures
often
lead
catalyst
deactivation
changes
selectivity
due
dynamic
metal
evolution
or
agglomeration,
even
with
classic
strong
metal–support
interaction.
Herein,
we
have
developed
FeOx/Ru/Rutile
multilayer
epitaxial
structure
by
depositing
FeOx
layer
onto
epitaxially
grown
RuO2
nanolayers
on
surface
rutile
nanoparticles.
This
transformed
into
which
Ru
nanoparticles
were
decorated
layers
ultrastable
metal-support
interaction
(SMSI).
Subsequently,
decoration
effectively
shifted
dominant
product
from
95%
during
hydrogenation.
Remarkably,
this
exhibits
exceptional
stability
can
be
operated
stably
at
550
°C
long
time
without
apparent
deactivation.
Compared
observed
supported
nanoparticles,
between
maintains
their
electronic
states
different
temperatures.
Furthermore,
Ru–FeOx
inhibits
H2
activation
capability,
adsorption,
subsequent
CO.
transformation
employed
here,
utilizes
initial
structures,
applied
construct
SMSI
enhance
catalysts'
performance.
Advanced Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Март 23, 2025
Abstract
Supported
reducible
oxides,
such
as
indium
oxide
on
monoclinic
zirconia
(In
2
O
3
/m‐ZrO
),
are
promising
catalysts
for
green
methanol
synthesis
via
CO
hydrogenation.
Growing
evidence
suggests
that
dynamic
restructuring
under
reaction
conditions
plays
a
crucial
but
poorly
understood
role
in
catalytic
performance.
To
address
this,
the
direct
visualization
of
state‐of‐the‐art
In
catalyst
hydrogenation
(
T
=
553
K,
P
1.9
bar,
:H
1:4)
is
pioneered
using
situ
scanning
transmission
electron
microscopy
(STEM),
comparing
its
behavior
to
supports
with
similar
(tetragonal,
t‐ZrO
or
anatase
TiO
)
lower
(LSm‐ZrO
surface
areas.
Complementary
infrared
spectroscopy
and
tests
confirm
formation
equivalent
conditions.
A
machine‐learning‐based
difference
imaging
approach
differentiates
ranks
patterns,
revealing
partially
reduced
InO
x
species
m‐ZrO
undergo
cyclic
aggregation‐redispersion
atomic
migration,
maintaining
high
active
phase
dispersion.
High‐resolution
ex
STEM
analysis
further
shows
epitaxial
mono‐
bilayers
(100)
facets,
highlighting
strong
oxide‐support
interactions.
contrast,
sintering
prevails
,
a‐TiO
low‐surface
correlating
productivity.
This
work
underscores
pivotal
interfacial
interactions
reaction‐induced
establishes
framework
tracking
nanoscale
dynamics.
Abstract
Thermocatalytic
conversions
of
carbon
dioxide
(CO
2
)
to
value‐added
products
offer
promising
approaches
achieving
net
negative
emissions.
The
catalysts
for
CO
conversions,
particularly
hydrogenation
reactions,
usually
involve
more
than
one
catalytic
sites
working
together.
In
this
review,
we
first
introduce
the
advanced
characterization
techniques
used
identify
in
catalysts,
hydrogen
(H
activation
and
adsorption/activation.
We
then
discuss
how
dual
or
multiple‐site
configurations
influence
activity
selectivity
reactions
such
as
reverse
water‐gas
shift
(RWGS),
methanation,
methanol
(MeOH).
finally
explain
Catalytic
Sites
Contiguity
(CSC)
concept
that
our
research
group
developed
from
work
reforming
methane
use
it
understand
relationship
between
spatial
arrangement
efficiency
reactant
conversion
recent
publications
on
MeOH
synthesis
hydrogenation.
hope
insights
into
impact
CSC
performance
lead
a
potential
top‐down
design
method
optimizing
catalysts.
Industrial & Engineering Chemistry Research,
Год журнала:
2024,
Номер
unknown
Опубликована: Ноя. 16, 2024
This
Review
summarizes
recent
advancements
in
regulating
microenvironments
for
enhancing
CO2
conversion,
particularly
focusing
on
copper-based
catalysts,
which
are
crucial
transforming
to
valuable
chemicals
and
fuels.
We
discuss
strategies
microenvironment
regulation,
including
single-atom
catalyst
design,
particle
size/facets/morphology
control,
confinement
effects,
interfacial
engineering.
These
approaches
influence
the
efficiency
selectivity
of
conversion
by
optimizing
active
site
density,
controlling
reactant/intermediate
concentrations,
promoting
charge-transfer
processes.
highlight
importance
mass
transfer,
electrolyte
properties,
modifying
electrode
structures
improving
conversion.
Despite
significant
progress,
challenges
remain
electrocatalytically
achieving
high
current
densities
multicarbon
products,
developing
effective
quantify
contribution
catalytic
performance.
Future
research
will
focus
advanced
characterization
techniques,
exploring
novel
materials
synthesis
methods,
utilizing
machine
learning
theoretical
modeling
design
optimization.
Nanomaterials,
Год журнала:
2023,
Номер
13(19), С. 2672 - 2672
Опубликована: Сен. 29, 2023
The
interaction
between
metal
particles
and
the
oxide
support,
so-called
metal-support
interaction,
plays
a
critical
role
in
performance
of
heterogenous
catalysts.
Probing
dynamic
evolution
these
interactions
under
reactive
gas
atmospheres
is
crucial
to
comprehending
structure-performance
relationship
eventually
designing
new
catalysts
with
enhanced
properties.
Cobalt
supported
on
TiO2
(Co/TiO2)
an
industrially
relevant
catalyst
applied
Fischer-Tropsch
synthesis.
Although
it
widely
acknowledged
that
Co/TiO2
restructured
during
reaction
process,
little
known
about
impact
specific
phase
environment
at
material's
surface.
combination
soft
hard
X-ray
photoemission
spectroscopies
are
used
investigate
situ
Co
pure
NaBH4-modified
H2,
O2,
CO2:H2
atmospheres.
methods,
which
allows
for
simultaneous
probing
chemical
composition
surface
subsurface
layers,
one
study's
unique
features.
It
shown
cobalt
encapsulated
below
stoichiometric
layer.
This
arrangement
preserved
CO2
hydrogenation
conditions
(i.e.,
CO2:H2),
but
changes
rapidly
upon
exposure
O2.
pretreatment
support
NaBH4
affects
mobility
prevents
spillover
onto
particles.
