Mechanistic
understanding
of
how
electrode-electrolyte
interfaces
evolve
dynamically
is
crucial
for
advancing
water-electrolysis
technology,
especially
the
restructuring
catalyst
surface
during
complex
electrocatalytic
reactions.
However,
perovskite
fluorides,
mechanistic
exploration
influence
dynamic
on
their
chemical
property
and
catalytic
mechanism
unclear
due
to
poor
conductivity
that
makes
definition
electrocatalyst
structure
difficult.
Herein,
oxygen
evolution
reaction
(OER),
various
operando
characterizations
are
employed
investigate
structure-activity
relationships
KNi
Advanced Science,
Год журнала:
2025,
Номер
unknown
Опубликована: Янв. 9, 2025
Abstract
Understanding
the
oxygen
evolution
reaction
(OER)
mechanism
is
pivotal
for
improving
overall
efficiency
of
water
electrolysis.
Despite
methylammonium
lead
halide
perovskites
(MAPbX
3
)
have
shown
promising
OER
performance
due
to
their
soft‐lattice
nature
that
allows
lattice‐oxygen
oxidation
active
α‐PbO
2
layer
surface,
role
A‐site
MA
or
X‐site
elements
in
electrochemical
reconstruction
and
mechanisms
has
yet
be
explored.
Here,
it
demonstrated
perovskite@zeolite
composites
intrinsically
dominated
by
group
lead‐halide
perovskites,
while
type
halogen
crucial
kinetics
composites.
Using
CsPbBr
x
I
3‐
@AlPO‐5
(
=
0,
1,
2,
3)
as
a
model
catalyst,
found
behaves
oxygen‐intercalation
pseudocapacitance
during
surface
restructuring
absence
halogen‐ion
migration
phase
separation
,
achieving
larger
diffusion
rate
OH
−
within
core‐shell
structure.
Moreover,
distinct
from
single‐metal‐site
MAPbBr
@AlPO‐5,
experimental
theoretical
investigations
reveal
soft
lattice
triggers
oxygen‐vacancy‐site
via
/α‐PbO
interface,
resulting
excellent
performance.
Owing
variety
easy
tailoring
perovskite
compositions,
these
findings
pave
way
development
novel
catalysts
efficient
electrocatalysis.
Advanced Energy Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Янв. 22, 2025
Abstract
Nickel‐based
double
perovskites
AA′BB′O
6
are
an
underexplored
class
of
oxygen
evolution
reaction
(OER)
catalysts,
in
which
B‐site
substitution
is
used
to
tune
electronic
and
structural
properties.
BaSrNiWO
,
with
a
comprised
alternating
Ni
W,
exhibits
high
activity,
attributed
the
highly
OER
active
surface
phase.
The
redox
transformation
2+
(3d
8
)
3+
7
combined
partial
W
dissolution
into
electrolyte
from
linear
Ni(3d)‐O(2p)‐W(5d)
chains
drives
situ
reconstruction
amorphized,
NiO‐like
layer,
promoting
mechanism.
However,
valence
6+
(5d
0
acts
as
stabilizing
influence
bulk,
preventing
mobilization
lattice
bound
covalent
W─O
bonds.
It
proposed
that
generated
during
can
support
mechanism
(LOEM)
vacancies
created
preferentially
refilled
by
electrolytic
OH
−
while
bulk
O
species
remain
stable.
This
LOEM
(sLOEM)
allows
retain
integrity
catalysis.
With
Tafel
slope
45
mV
dec
−1
0.1
m
KOH,
illustrates
potential
Ni‐based
offer
both
efficiency
stability
alkaline
electrolysis.
Advanced Energy Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Март 5, 2025
Abstract
Mo‐based
palmeirite
oxide
A
2
Mo
3
O
8
is
an
emerging
electrocatalyst,
exhibiting
a
bipartite
honeycomb
lattice
consisting
of
tetrahedral
and
octahedral
sites
with
good
conductivity.
However,
as
promising
catalyst
in
electrocatalytic
remains
rarely
touched.
The
rational
design
clarification
the
correlation
between
geometrical
configuration
modulation
properties
are
challenging.
Herein,
innovative
strategy
reported
to
anchor
thiospinel
Co
S
4
nanoparticles
onto
surface
nanosheet,
which
can
trigger
spin
electrons
rearrangement,
thus
activating
inert
sites.
According
X‐ray
absorption
spectroscopy,
2+
─O─Co
3+
bimetallic
bridging
asymmetric
bond
polarization
constructed
interface,
triggers
favorable
transition
from
low
intermediate
spin.
Interestingly,
/Co
exhibits
remarkable
oxygen
evolution
reaction
performance
overpotential
227
mV
at
10
mA
cm
−2
.
At
industrial
process
temperature,
it
takes
only
2.37
V
for
overall
water
splitting
obtain
large
current
density
1
theoretical
calculation
results
confirm
that
distortion‐related
optimizes
energy,
enhancing
adsorption
*
OOH.
This
work
highlights
potential
achieving
seawater
by
rearrangement.
Advanced Science,
Год журнала:
2025,
Номер
unknown
Опубликована: Март 19, 2025
Abstract
Developing
diverse
methods
to
approach
highly
crystalline
covalent
organic
frameworks
(COFs)
for
improvement
of
their
electrocatalytic
hydrogen
evolution
reaction
(HER)
activity
is
important
but
very
challenging.
Herein,
the
first
time,
an
electrochemically‐driven
reconstruction
strategy
demonstrated
convert
semi‐polymerized
low‐crystalline
COFs
into
crystalline,
structurally
ordered
with
enhanced
HER
activity.
In
situ
and
ex
characterizations
reveal
that
cyclic
voltammetry
(CV)
cycles
can
promote
crystallinity,
thereby
leading
improved
conductivity,
increased
active
site
density,
superior
stability.
As
a
result,
COF
achieves
low
overpotentials
103.6
219.4
mV
at
10
50
mA
cm
−2
,
respectively,
excellent
stability
(1200
h
).
More
importantly,
this
generalizable
effective
various
imine‐linked
different
bonding
types,
significantly
improving
crystallinity
This
work
not
only
establishes
novel
method
constructing
also
demonstrates
versatility
electrochemically
driven
structural
modulation
in
enhancing
catalytic
performance
COFs.
Advanced Science,
Год журнала:
2025,
Номер
unknown
Опубликована: Март 18, 2025
Abstract
The
hydrogen
oxidation
reaction
(HOR)
in
alkaline
media
is
pivotal
for
the
advancement
of
anion
exchange
membrane
fuel
cells
(AEMFCs),
and
development
single‐atom
catalysts
offers
a
promising
solution
creating
cost‐effective,
highly
efficient
HOR
catalysts.
Although
transition
from
nanoparticle
to
enhances
catalytic
activity,
stability
these
sites
remains
significant
challenge.
In
this
study,
active
stable
catalyst
successfully
designed
by
incorporating
Ru
atoms
into
ZrO
2‐x
/C
nanoparticles,
forming
single
Ru‐SA‐ZrO
/C.
exhibits
an
outstanding
mass
activity
6789.4
mA
mg
−1
at
50
mV,
surpassing
Ru/C
67
fold
commercial
Pt/C
42.5
fold.
Density
functional
theory
(DFT)
simulations
reveal
that
integration
optimizes
both
bonding
energy
(HBE)
hydroxyl
binding
(OHBE),
reducing
toxicity
sites.
This
research
opens
new
pathway
precise
design
metal
hybrids,
offering
direction
developing
electrocatalysts
applications.
