Reverse
water-gas
shift
(RWGS)
reaction
is
a
promising
strategy
for
the
effective
valorization
of
CO2.
Because
its
endothermic
nature,
high-performance
catalyst
with
high
durability
at
temperatures
has
been
required.
Herein,
we
reveal
dynamic
structural
changes
platinum-loaded
molybdenum
suboxide
catalysts
(Pt/MoOx)
in
RWGS
by
multiple
operando
and
situ
measurements,
exhibits
activity
CO
selectivity,
as
well
stability
500
°C
due
to
emergence
contiguous
Mo
species
(Mo--Mo)
strong
metal-support
interaction
(SMSI)
effect
MoOx.
In
X-ray
absorption
fine
structure
(XAFS)
measurements
demonstrated
that
driven
reversible
redox
situ-formed
MoOx
suboxide,
where
Mo--Mo
act
activation
sites
Comprehensive
analysis
revealed
shell
surrounding
Pt
nanoparticles
(NPs)
suppresses
adsorption,
thereby
resulting
selectivity.
Furthermore,
exhibited
continuous
increase
earlier
stage
operation
°C,
which
was
attributed
partial
carburization
during
associated
electron
density
species.
These
findings
advance
understanding
mechanism
suggest
innovative
strategies
development
oxide
enhanced
stability.
ACS Nano,
Journal Year:
2023,
Volume and Issue:
17(21), P. 20804 - 20824
Published: Nov. 3, 2023
The
splitting
of
water
through
electrocatalysis
offers
a
sustainable
method
for
the
production
hydrogen.
In
alkaline
electrolytes,
lack
protons
forces
dissociation
to
occur
before
hydrogen
evolution
reaction
(HER).
While
pure
Pt
is
gold
standard
electrocatalyst
in
acidic
since
5d
orbital
nearly
fully
occupied,
when
it
overlaps
with
molecular
water,
generates
Pauli
repulsion.
As
result,
formation
Pt–H*
bond
an
environment
difficult,
which
slows
HER
and
negates
benefits
using
catalyst.
To
overcome
this
limitation,
can
be
alloyed
transition
metals,
such
as
Fe,
Co,
Ni.
This
approach
has
potential
not
only
enhance
performance
but
also
increase
dispersion
decrease
its
usage,
thus
overall
improving
catalyst's
cost-effectiveness.
excellent
adsorption
ability
metals
contributes
generation
proton-rich
local
near
Pt-based
alloy
that
promotes
HER.
Significant
progress
been
achieved
comprehending
mechanism
manipulation
structure
composition
electrocatalysts
based
on
alloy.
objective
review
analyze
condense
latest
developments
It
focuses
modified
alloys
clarifies
design
principles
catalytic
catalysts
from
both
experimental
theoretical
perspective.
highlights
some
difficulties
encountered
during
opportunities
increasing
performance.
Finally,
guidance
development
more
efficient
provided.
ACS Nano,
Journal Year:
2023,
Volume and Issue:
17(12), P. 11869 - 11881
Published: June 8, 2023
Photocatalytic
reduction
of
CO2
to
value-added
solar
fuels
is
great
significance
alleviate
the
severe
environmental
and
energy
crisis.
Herein,
we
report
construction
a
synergistic
silver
nanoparticle
catalyst
with
adjacent
atomic
cobalt-silver
dual-metal
sites
on
P-doped
carbon
nitride
(Co1Ag(1+n)-PCN)
for
photocatalytic
reduction.
The
optimized
photocatalyst
achieves
high
CO
formation
rate
46.82
μmol
gcat-1
70.1%
selectivity
in
solid-liquid
mode
without
sacrificial
agents,
which
2.68
2.18-fold
compared
that
exclusive
single-atom
(Ag1-CN)
site
(Co1Ag1-PCN)
photocatalysts,
respectively.
closely
integrated
situ
experiments
density
functional
theory
calculations
unravel
electronic
metal-support
interactions
(EMSIs)
Ag
nanoparticles
Ag-N2C2
Co-N6-P
promote
adsorption
CO2*
COOH*
intermediates
form
CH4,
as
well
boost
enrichment
transfer
photoexcited
electrons.
Moreover,
atomically
dispersed
Co-Ag
SA
serve
fast-electron-transfer
channel
while
act
electron
acceptor
enrich
separate
more
photogenerated
This
work
provides
general
platform
delicately
design
high-performance
catalysts
highly
efficient
conversion.
Science,
Journal Year:
2024,
Volume and Issue:
386(6724), P. 915 - 920
Published: Nov. 21, 2024
The
metal-support
interaction
is
one
of
the
most
important
pillars
in
heterogeneous
catalysis,
but
developing
a
fundamental
theory
has
been
challenging
because
intricate
interfaces.
Based
on
experimental
data,
interpretable
machine
learning,
theoretical
derivation,
and
first-principles
simulations,
we
established
general
metal-oxide
interactions
grounded
metal-metal
metal-oxygen
interactions.
applies
to
metal
nanoparticles
atoms
oxide
supports
films
supports.
We
found
that
for
late-transition
catalysts,
metal-metal
dominated
support
effects
suboxide
encapsulation
over
nanoparticles.
A
principle
strong
occurrence
formulated
substantiated
by
extensive
experiments
including
10
metals
16
oxides.
valuable
insights
revealed
(strong)
advance
interfacial
design
supported
catalysts.
ACS Catalysis,
Journal Year:
2024,
Volume and Issue:
14(4), P. 2409 - 2417
Published: Feb. 1, 2024
Strong
metal–support
interaction
(SMSI)
is
commonly
observed
for
platinum-group
metals
on
reducible
oxide
supports
upon
a
high-temperature
reduction
(≥500
°C).
Herein,
we
show
that
the
SMSI
state
can
be
constructed
over
Ru/anatase-TiO2
catalyst
using
CO2
hydrogenation
reaction
gas
at
low
temperature
of
∼210
°C,
which
could
overturn
selectivity
from
100%
CH4
to
>99%
CO.
It
revealed
exposed
metallic
Ru
nanoparticles
promote
formation
via
formate
intermediates
temperatures
<200
°C.
Elevating
under
H2-containing
atmosphere
causes
evolution
active
TiOx
suboxide
form
an
encapsulated
structure
Ru@TiOx,
changes
surface
intermediate
carboxy
species
during
hydrogenation,
thus
leading
exclusive
CO
with
long-term
catalytic
stability.
The
O2-containing
treatment
Ru@TiOx
achieve
cyclic
switch
product
between
and
CH4.
This
work
provides
effective
strategy
modulate
very
temperature.
Journal of the American Chemical Society,
Journal Year:
2024,
Volume and Issue:
146(26), P. 17659 - 17668
Published: June 21, 2024
Reactive
metal-support
interaction
(RMSI)
is
an
emerging
way
to
regulate
the
catalytic
performance
for
supported
metal
catalysts.
However,
induction
of
RMSI
by
thermal
reduction
often
accompanied
encapsulation
effect
on
metals,
which
limits
mechanism
research
and
applications
RMSI.
In
this
work,
a
gradient
orbital
coupling
construction
strategy
was
successfully
developed
induce
in
Pt-carbide
system
without
reductant,
leading
formation
L1
ACS Materials Letters,
Journal Year:
2023,
Volume and Issue:
5(10), P. 2629 - 2647
Published: Aug. 30, 2023
Interesting
phenomena
such
as
encapsulation,
charge
transfer,
and
bond
formation,
etc.
induced
by
classical
strong
metal–support
interaction
(SMSI)
during
high-temperature
reduction
have
received
wide
attention
for
their
potential
to
determine
the
catalytic
behavior
of
supported
metal
catalysts.
However,
a
systematically
scientific
understanding
about
effects
SMSI
on
CO2
hydrogenation
performance
is
still
insufficient
primarily
due
diversities
in
catalysts
reaction
conditions.
Here,
we
outline
"double-edged
sword
effects"
activity,
stability,
even
selectivity
C1
high-value
compounds
(CO,
methane,
methanol).
Specifically,
moderate
could
efficiently
optimize
structural
electronic
properties
tune
conversion
key
intermediates
involved
hydrogenation,
thereby
enhancing
performance.
Nevertheless,
excessive
fatal
methanation
methanol
synthesis
catalysts,
because
encapsulation
active
centers
suppresses
further
reactive
intermediates.
Additionally,
alter
regulating
dissociation
H2
breakage
C–O
bonds.
Subsequently,
dependencies
are
emphasized
with
aim
providing
guidance
developing
an
appropriate
rational
design.
To
conclude,
highlighted
perspectives
deeper
also
presented.
