Chemistry - Methods,
Год журнала:
2024,
Номер
4(11)
Опубликована: Окт. 18, 2024
Abstract
The
growing
interest
in
physically
deposited
model
catalysts
for
uncovering
complex
structure‐activity
relationships
is
spurred
by
the
possibility
of
depositing
nanoparticles
precise
atomic
structure
and
composition
using
cluster‐beam
sources.
However,
limitations
accompanying
these
synthesis
techniques,
such
as
low
deposition
rates
flat
sample
geometry,
present
a
challenge
situ
structural
characterization
bulk‐sensitive
methods,
X‐ray
absorption
spectroscopy
(XAS),
especially
at
elevated
pressures
(1–100
bar).
To
overcome
this
challenge,
we
constructed
an
XAS
cell
operating
grazing
incidence
(GI)
geometry.
GIXAS
was
used
to
investigate
cluster‐beam‐generated
Pd
Au
0.3
Ag
0.7
under
CO
2
‐to‐methanol
hydrogenation
conditions
(230
°C,
20
bar,
:H
=1
:
3).
These
nanoparticles,
with
metal
loading
0.96–10
μg
cm
−2
,
demonstrated
stability
resistance
sintering
upon
activation
H
120
°C
catalytic
conditions,
revealed
XAS.
promising
results
from
our
work
will
help
bridge
gap
investigation
materials
produced
gas‐phase
cluster
industrially
relevant
temperatures,
which
vital
mechanistic
understanding
processes.
Chemical Society Reviews,
Год журнала:
2024,
Номер
53(17), С. 8563 - 8631
Опубликована: Янв. 1, 2024
Ionic
liquids
(ILs)
and
deep
eutectic
solvents
(DESs)
have
tremendous
potential
for
reactive
capture
of
CO
2
,
due
to
their
highly
properties,
including
a
wide
electrochemical
stability
window,
low
volatility,
high
solubility.
Nature Communications,
Год журнала:
2024,
Номер
15(1)
Опубликована: Июль 20, 2024
Abstract
Copper
and
nitrogen
co-doped
carbon
catalysts
exhibit
a
remarkable
behavior
during
the
electrocatalytic
CO
2
reduction
(CO
RR),
namely,
formation
of
metal
nanoparticles
from
Cu
single
atoms,
their
subsequent
reversible
redispersion.
Here
we
show
that
switchable
nature
these
species
holds
key
for
on-demand
control
over
distribution
RR
products,
lack
which
has
thus
far
hindered
wide-spread
practical
adoption
RR.
By
intermitting
pulses
working
cathodic
potential
with
anodic
potential,
were
able
to
achieve
controlled
fragmentation
particles
partial
regeneration
atom
sites.
tuning
pulse
durations,
by
tracking
catalyst’s
evolution
using
operando
quick
X-ray
absorption
spectroscopy,
speciation
catalyst
can
be
steered
toward
sites,
ultrasmall
clusters
or
large
nanoparticles,
each
exhibiting
unique
functionalities.
Growing
global
population,
escalating
energy
consumption,
and
climate
change
threaten
future
security.
Fossil
fuel
combustion,
primarily
coal,
oil,
natural
gas,
exacerbates
the
greenhouse
effect
driving
warming
through
CO
Nature Communications,
Год журнала:
2025,
Номер
16(1)
Опубликована: Март 16, 2025
In-situ
and
operando
techniques
in
heterogeneous
electrocatalysis
are
a
powerful
tool
used
to
elucidate
reaction
mechanisms.
Ultimately,
they
key
determining
concrete
links
between
catalyst's
physical/electronic
structure
its
activity
en
route
designing
next-generation
systems.
To
this
end,
the
exact
execution
interpretation
of
these
lines
experiments
is
critical
as
determines
strength
conclusions
that
can
be
drawn
what
uncertainties
remain.
Instead
focusing
on
how
were
understand
systems,
case
with
most
reviews
topic,
work
instead
initiates
nuanced
discussion
1)
best
carry
out
each
technique
2)
initiate
analysis
which
level
insights
from
set
in-situ
or
experiments/controls
carried
out.
We
focus
several
commonly
techniques,
including
vibrational
(IR,
Raman)
spectroscopy,
X-ray
absorption
spectroscopy
electrochemical
mass
spectrometry.
In
addition
this,
we
include
sections
reactor
design
link
theoretical
modelling
applicable
across
all
techniques.
While
electrocatalysis,
make
when
appropriate
areas
photo-
thermo-catalytic
highlight
common
pitfalls
field,
avoid
them,
sets
complementary
may
strengthen
analysis.
end
an
overview
gaps
remain
innovations
must
made
overcome
them.
situ
useful
towards
mechanistic
investigations
electrocatalytic
systems
but
interpreted
properly.
Here,
authors
provide
guidelines
for
practices
use
methods.
ACS Catalysis,
Год журнала:
2024,
Номер
14(10), С. 8105 - 8115
Опубликована: Май 8, 2024
Photocatalytic
CO2
reduction
(PCO2R)
represents
a
critical
pathway
in
renewable
energy
generation.
Silver
nanoparticles
(Ag
NPs)
of
varying
sizes
were
deposited
on
TiO2
surfaces,
exhibiting
size-dependent
catalytic
activities
and
selectivities
due
to
distinct
charge
transfer
dynamics.
The
integration
the
particle
size
Ag/TiO2
Schottky
junction
density
supplied
ample
active
sites
for
reduction.
Modifying
Ag
NPs
significantly
enhanced
photocatalytic
performance
heterojunction.
Notably,
Ag0.5%/TiO2
showed
CO
generation
rate
86.8
μmol
g–1
h–1,
which
was
1.79
times
higher
than
that
anatase.
More
importantly,
Ag3.0%/TiO2
resulted
highest
selectivity
CH4
(28.1%).
influenced
ratio
thermal
electron
during
photoexcitation
intermediate
product
pathways
process.
This
research
provides
insights
experimental
foundations
regulation
designing
heterojunction
catalysts
PCO2R.
Advanced Energy Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Март 12, 2025
Abstract
Electrocatalytic
conversion
of
carbon
dioxide
(CO
2
)
into
valuable
carbon‐based
fuels
and
chemicals
represents
a
promising
approach
to
closing
the
cycle
setting
circular
economy.
Nevertheless,
for
current
electrocatalytic
CO
reduction
reaction
(ECO
RR)
systems,
realizing
100%
with
simultaneously
high
overall
rate
(i.e.,
single‐pass
conversion)
Faradaic
efficiency
(FE)
remains
significant
challenge.
Enhancing
often
results
in
decrease
FE,
conversely,
improving
FE
may
limit
rate.
Metal–CO
(M–CO
batteries
functions
face
similar
challenges,
particularly
reversible
M–CO
batteries,
which
do
not
accomplish
net
because
nearly
all
RR
products
are
reoxidized
during
subsequent
charging
process.
Such
system
neutrality
poses
substantial
challenges.
This
perspective
provides
an
in‐depth
analysis
state‐of‐the‐art
ECO
systems
alongside
main
strategies
employed
address
their
respective
The
critical
importance
achieving
both
is
underscored
practical
applications
effectively
close
cycle.
Furthermore,
strategic
roadmap
that
outlines
future
research
directions
presented,
thereby
facilitating
advancement
comprehensive
electroconversion
technologies.
Advanced Energy Materials,
Год журнала:
2024,
Номер
14(33)
Опубликована: Май 29, 2024
Abstract
The
electrochemical
reduction
of
CO
2
(eCO
RR)
that
exclusively
produces
one
product
at
industrial
current
density
is
crucial
for
the
substantial
storage
renewable
energy.
Modulating
electronic
structure
atomically
dispersed
catalysts
can
effectively
regulate
adsorption
rate‐determining‐step
intermediates
to
achieve
desired
products.
Here,
study
constructs
a
hybrid
catalyst
consisting
single
Ag
atoms
and
atomic
clusters
supported
on
nitrogen‐doped
multi‐walled
carbon
nanotubes
important
intermediate
*COOH.
X‐ray
photoelectron
absorption
near‐edge
spectroscopies
demonstrate
turning
into
weaken
electron
transfer
between
Ag–N
present
relatively
rich
state.
Thus,
rate‐determining
step
*COOH
massive
formation
significantly
accelerated,
as
proven
by
in
situ
synchrotron
infrared
spectroscopy
functional
theory
calculations.
Using
this
strategy,
Faradaic
efficiency
outperforming
99%
from
−0.3
−0.8
V
(vs
reversible
hydrogen
electrode)
with
densities
above
200
mA
cm
−2
half‐cell
energetic
86%
achieved.
This
work
highlights
promising
approach
advancing
synergistic
achieving
more
controllable
efficient
eCO
RR.
