Nano Letters,
Journal Year:
2025,
Volume and Issue:
unknown
Published: May 7, 2025
Electroreduction
of
CO2
(ECR)
to
CO
or
syngas
is
an
effective
approach
alleviating
greenhouse
gas
emissions.
Herein,
nickel
nanoparticles
coated
with
halogen/nitrogen
codoped
carbon
were
prepared
(X-Ni/NC-a).
Cl-Ni/NC-a
can
obtain
three
important
compositions
(CO:H2)
under
different
voltages,
such
as
0.97,
0.51,
and
0.32,
which
are
the
ratios
for
hydroformylation,
methanol,
ethanol
synthesis,
respectively.
For
Br-Ni/NC-a,
Faraday
efficiency
(FEco)
exceed
96%,
a
partial
current
density
(jco)
48
mA
cm-2.
Additionally,
Br-Ni/NC-a
used
in
Zn-CO2
battery
(ZCB);
power
reach
2.6
mW
cm-2,
charge-discharge
stability
110
h.
DFT
calculations
revealed
that
strong
interaction
between
regulates
electronic
structure
catalyst,
affecting
adsorption/desorption
intermediates.
This
study
provides
feasible
scheme
halogen
doping
modulate
selectivity
ECR
potential
application
catalysts
ZCB.
Journal of the American Chemical Society,
Journal Year:
2025,
Volume and Issue:
unknown
Published: Feb. 5, 2025
Multi-proton-coupled
electron
transfer,
multitudinous
intermediates,
and
unavoidable
competing
hydrogen
evolution
reaction
during
CO2
electroreduction
make
it
tricky
to
control
high
selectivity
for
specific
products.
Here,
we
present
spatial
confinement
of
Fe
single
atoms
(FeN2S2)
by
adjacent
FeS
clusters
(Fe4S4)
orientate
the
transition
adsorption
configuration
from
C,O-side
O-end,
which
triggers
a
shift
activated
first-step
protonation
C–C
coupling,
thus
switching
target
product
HCOOH
in
Faraday
efficiency
(FE:
90.6%)
on
FeN2S2
CH3COOH
82.3%)
Fe4S4/FeN2S2.
The
strength
*OCHO
upon
solitary
site
is
linearly
related
coordination
number
Fe–S,
with
predominantly
produced
over
single-atom
(ortho-substituted
S
atoms).
Fe4S4
cluster
functions
as
switch
reduction
product,
can
not
only
optimize
electronic
structure
neighboring
but
also
impel
complete
hydrocarbon
intermediate
*CH3,
followed
coupling
CO2*
*CH3
via
synergistic
catalysis
This
strategy
provides
new
avenue
modulate
reactant
model
desirable
pathways,
potential
applications
diverse
multistep
electrochemical
processes
controlled
selectivity.
Nature Communications,
Journal Year:
2025,
Volume and Issue:
16(1)
Published: Feb. 19, 2025
Abstract
Acidic
electrochemical
CO
2
conversion
is
a
promising
alternative
to
overcome
the
low
utilization.
However,
over-reliance
on
highly
concentrated
K
+
inhibit
hydrogen
evolution
reaction
also
causes
(bi)carbonate
precipitation
interfere
with
catalytic
performance.
In
this
work,
under
screening
and
guidance
of
computational
simulations,
we
present
carbon
coated
tip-like
O
3
electrocatalyst
for
stable
efficient
acidic
synthesize
formic
acid
(HCOOH)
concentration.
The
layer
protects
oxidized
species
higher
intrinsic
activity
from
reductive
corrosion,
peripherally
formulates
tip-induced
electric
field
regulate
adverse
H
attraction
desirable
enrichment.
an
electrolyte
at
pH
0.94,
only
0.1
M
required
achieve
Faradaic
efficiency
(FE)
98.9%
300
mA
cm
−2
HCOOH
long-time
stability
over100
h.
By
up-scaling
electrode
into
25
electrolyzer
setup,
total
current
7
A
recorded
sustain
durable
production
291.6
mmol
L
−1
h
.
Journal of the American Chemical Society,
Journal Year:
2025,
Volume and Issue:
unknown
Published: Feb. 10, 2025
The
electrochemical
coupling
of
CO2
and
NO3–
on
copper-based
catalysts
presents
a
sustainable
strategy
for
urea
production
while
simultaneously
addressing
wastewater
denitrification.
However,
the
inefficient
random
adsorption
copper
surface
limits
interaction
key
carbon
nitrogen
intermediates,
thereby
impeding
efficient
C–N
coupling.
In
this
study,
we
demonstrate
that
residual
lattice
oxygen
in
oxide-derived
nanosheets
(OL-Cu)
can
effectively
tune
electron
distribution,
thus
activating
neighboring
atoms
generating
electron-deficient
(Cuδ+)
sites.
These
Cuδ+
sites
enhance
stabilize
*CO
which
enables
directional
at
adjacent
This
mechanism
shortens
pathway
achieves
yield
up
to
298.67
mmol
h–1
g–1
−0.7
V
versus
RHE,
with
an
average
Faradaic
efficiency
31.71%
high
current
density
∼95
mA
cm–2.
situ
spectroscopic
measurements
confirmed
formation
tracked
evolution
intermediates
(i.e.,
*CO,
*NO,
*OCNO,
*NOCONO)
during
synthesis.
Density
functional
theory
calculations
revealed
promote
coadsorption
*NO3,
as
well
*OCNO
significantly
improving
kinetics.
study
underscores
critical
role
facilitating
selectivity.
Advanced Science,
Journal Year:
2025,
Volume and Issue:
unknown
Published: Feb. 27, 2025
Abstract
The
electrocatalytic
conversion
of
CO
2
into
valuable
multi‐carbon
(C
2+
)
products
using
Cu‐based
catalysts
has
attracted
significant
attention.
This
review
provides
a
comprehensive
overview
recent
advances
in
catalyst
design
to
improve
C
selectivity
and
operational
stability.
It
begins
with
an
analysis
the
fundamental
reaction
pathways
for
formation,
encompassing
both
established
emerging
mechanisms,
which
offer
critical
insights
design.
In
situ
techniques,
essential
validating
these
by
real‐time
observation
intermediates
material
evolution,
are
also
introduced.
A
key
focus
this
is
placed
on
how
enhance
through
manipulation,
particularly
emphasizing
catalytic
site
construction
promote
C─C
coupling
via
increasing
*
coverage
optimizing
protonation.
Additionally,
challenge
maintaining
activity
under
conditions
discussed,
highlighting
reduction
active
charged
Cu
species
materials
reconstruction
as
major
obstacles.
To
address
these,
describes
strategies
preserve
sites
control
including
novel
utilization
mitigation
reconstruction.
By
presenting
developments
challenges
ahead,
aims
guide
future
conversion.
Angewandte Chemie International Edition,
Journal Year:
2024,
Volume and Issue:
unknown
Published: Dec. 28, 2024
Abstract
The
high
entropy
alloy
(HEA)
possesses
distinctive
thermal
stability
and
electronic
characteristics,
which
exhibits
substantial
potential
for
diverse
applications
in
electrocatalytic
reactions.
nanosize
of
HEA
also
has
a
significant
impact
on
its
catalytic
performance.
However,
accurately
controlling
synthesizing
small
nanomaterials
remains
challenge,
especially
the
ultrasmall
nanoparticles.
Herein,
we
firstly
calculate
illustrate
size
structure
as
well
adsorption
energies
crucial
intermediates
involved
typical
processes,
such
hydrogen
evolution
reaction
(HER),
oxygen
reduction
(ORR),
CO
2
electroreduction
(CO
RR)
NO
3
−
(NO
RR).
Under
guidance
theoretical
calculations,
synthesize
range
PtRuPdCoNi
nanoparticles
with
adjustable
sizes
(1.7,
2.3,
3.0,
3.9
nm)
using
one‐step
spatially
confined
approach,
without
any
further
treatment.
Experimentally,
smaller
HEAs
is
more
favorable
HER
ORR
performances,
aligning
predictions.
Specifically,
sized
at
1.7
nm
(HEA‐1.7)
endows
16
mV
overpotential
current
density
10
mA
cm
−2
,
yielding
mass
activity
31.9
A
mg
NM
−1
noble
metal
HER,
significantly
outperforming
commercial
Pt/C
catalyst.
This
strategy
can
be
easily
applicable
to
other
reactions
(e.g.
)
attributed
richness
components
adjustability,
presenting
promising
platform
various
advanced
catalysts.