Advanced Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Май 2, 2025
Abstract
To
achieve
the
ideal
non‐noble‐metal
HER
electrocatalyst
in
alkaline
media,
developing
conductive
systems
with
multiple
active
sites
targeting
every
elementary
step
HER,
is
highly
desirable
but
remains
a
great
challenge.
Herein,
noble
metal‐free
antiperovskite
CdNNi
3
reported
intrinsic
metallic
characteristics
as
efficient
electrocatalyst,
which
designed
by
facile
A‐site
tuning
strategy
modulation
electronic
structures
and
interfacial
water
configurations
of
antiperovskites.
Impressively,
performance
superior
to
various
state‐of‐the‐art
non‐noble
metal
catalysts
ever
reported,
also
outperforms
commercial
Raney
Ni
catalyst
when
assemble
cathode
practical
anion
exchange
membrane
electrolyzer
(AEMWE)
device.
With
insights
from
comprehensive
experiments
theoretical
calculations,
can
create
synergistic
dual
for
catalyzing
different
steps
HER;
namely,
site
effectively
facilitate
H
2
O
dissociation
OH
−
desorption,
while
unusual
Cd–Ni
bridge
optimal
*
adsorption
evolution.
Such
multifunction‐site
synergy,
together
inherent
high
electrical
conductivity,
enables
fulfill
essential
criteria
an
excellent
performance.
ABSTRACT
Double
perovskite
oxides
(POs)
are
effective
electrode
materials
for
supercapacitors
(SCs).
Nevertheless,
adapting
their
unique
architectures
to
boost
the
electrochemical
performance
remains
tricky.
Herein,
we
present
exceptional
La
2
MnXO
6
(X
=
Co,
Fe)
double
perovskites
as
SC
materials.
The
sol–gel
method
has
prepared
MnCoO
(LMCO)
and
MnFeO
(LMFO)
nanorods.
XRD
revealed
that
LMCO
LMFO
have
monoclinic
crystal
structures
with
lattice
constants
of
a
5.517
Å,
b
5.528
c
7.805
β
89.926°,
5.549
5.557
7.783
89.931°,
respectively.
Scanning
electron
microscopy
indicated
existence
uniformly
distributed
bandgap
using
Tauc's
plot
was
determined
1.38
1.24
eV
,
Fourier‐transform
infrared
spectroscopy
further
characterized
X‐ray
photoelectron
investigation
confirmed
3+
Mn
Fe
O
2−
Co
ions
on
surface
specific
capacitance
achieved
333.86
880.5
F/g
@
2.5
A/g
respectively,
1
M
KOH
electrolyte.
demonstrated
excellent
energy
power
density
30.5
Wh/kg
625
W/kg.
asymmetric
CV
curve
shape
proved
battery‐type
behavior
due
indication
redox
reactions.
Furthermore,
Dunn's
technique
evaluated
percentage
contribution
capacitive
diffusion
behavior.
Our
strategy
nanorods
material
improved
activity
significantly
offered
facile
guideline
targeting
electrodes
applications.
Compared
with
acidic
environments,
promoting
the
water
dissociation
process
is
crucial
for
speeding
up
hydrogen
evolution
reaction
(HER)
kinetics
in
alkaline
electrolyte.
Although
construction
of
heterostructured
electrocatalysts
by
hybridizing
noble
metals
metal
(hydr)oxides
has
been
reported
as
a
feasible
approach
to
achieve
high
performance,
cost,
complicated
fabrication
process,
and
unsatisfactory
mass
activity
limit
their
large-scale
applications.
Herein,
we
report
single-phase
HER
electrocatalyst
composed
single-atom
ruthenium
(Ru)
incorporated
into
cobalt
oxide
spine
structure
(denoted
Ru
SA/Co3O4),
which
possesses
exceptional
performance
media
via
unusual
atomic-scale
Ru-Co
pair
sites.
In
particular,
SA/Co3O4
exhibits
very
low
overpotential
44
mV
at
10
mA
cm-2
an
outstanding
4700
mg-1
50
overpotential,
superior
those
commercial
Pt/C,
nanoparticles
supported
on
Co3O4
NP/Co3O4)
other
Ru-based
electrocatalysts.
With
insights
from
theoretical
calculations,
synergistic
interactions
between
Co
active
sites
are
revealed
catalyze
diverse
fundamental
steps
HER;
i.e.,
can
effectively
accelerate
adsorption/dissociation
OH-
desorption,
whereas
favorable
H*
adsorption
H2
evolution.
Advanced Functional Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Фев. 26, 2025
Abstract
As
a
key
reaction
in
water
electrolysis
and
fuel
cells,
the
oxygen
evolution
(OER)
involves
sluggish
four‐electron
proton
transfer
process.
Understanding
OER
pathways
kinetics
is
critical
for
designing
efficient
electrocatalysts.
In
this
study,
through
density
functional
theory
(DFT)
calculations,
it
demonstrated
that
incorporation
of
Gd
into
Fe‐doped
NiO
elevates
O
2
p
band
center
generates
more
unoccupied
states.
Furthermore,
promotes
formation
vacancies,
which,
together,
enhance
lattice
oxidation
mechanism
(LOM)
pathway
OER.
The
adsorption‐free
energy
diagrams
confirm
doping
significantly
lowers
theoretical
overpotentials
at
both
Fe
Ni
sites
NiO,
thereby
improving
activity.
Based
on
these
findings,
co‐doped
ultrathin
nanosheets
are
synthesized
via
spray
combustion.
an
catalyst,
material
exhibited
low
overpotential
227
mV,
which
40
mV
lower
than
long‐term
catalytic
stability
over
150
h.
anion
exchange
membrane
system,
stable
performance
120
h
current
20
mA
cm
−2
.
Advanced Functional Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Март 20, 2025
Abstract
The
electrochemical
oxidation
(EO)
process
has
the
unique
advantage
of
in
situ
generation
reactive
oxygen
species
for
organic
synthesis
and
wastewater
purification.
However,
strong
binding
H
2
O
anode
inhibits
desorption
species,
exacerbating
their
peroxidation
into
thus
weakening
EO
performance.
In
this
work,
an
electron
delocalization
strategy
is
proposed
by
introducing
Cu
2+
tetrahedral
sites
(A
Td
)
Co
3
4
(Cu
x
3‐x
to
trigger
super‐exchange
effect
─O─Co
Oh
3+
,
constructing
electron‐rich
accelerating
*OH
promotion
Experimental
results
confirm
electron‐delocalized
disrupts
kinetic
equilibrium
evolution
reaction
balances
energy
barriers
adsorption,
dehydrogenation,
over
sites,
realizing
•OH‐mediated
process.
required
free
•OH
decreases
from
1.14
0.70
eV.
extraordinary
activity
elimination
multiple
aromatic
contaminants
demonstrates
feasibility
practical
landfill
leachate
treatment.
This
study
offers
in‐depth
understanding
active
formation
systems
guides
design
superior
stable
electrodes
efficient
conversion
matter.
Inorganic Chemistry,
Год журнала:
2025,
Номер
unknown
Опубликована: Март 27, 2025
Rationally
optimizing
the
atomic
and
electronic
structure
of
electrocatalysts
is
an
effective
strategy
to
improve
activity
electrocatalytic
oxygen
evolution
reaction
(OER),
yet
it
remains
challenging.
In
this
work,
heterointerface
engineering
developed
accelerate
OER
by
decorating
iridium
atoms
on
low-crystalline
cobalt
hydroxide
nanosheets
(Ir–Co(OH)x)
via
oxygen-coordinated
bonds
modulate
local
structure.
Leveraging
detailed
spectroscopic
characterizations,
Ir
species
were
proved
promote
charge
transfer
through
Ir–O–Co
coordination
between
atom
Co(OH)x
support.
As
a
result,
optimized
Ir–Co(OH)x
exhibits
excellent
with
low
overpotential
251
mV
drive
10
mA
cm–2,
which
63
lower
than
that
pristine
Co(OH)x.
The
experimental
results
density
functional
theory
calculations
reveal
isolated
can
regulate
environment
configuration
Co(OH)x,
thus
accelerating
catalytic
kinetics.
This
work
provides
atomistic
for
modulation
metal
active
sites
in
design
high-performance
electrocatalysts.
