Abstract
Mass
transfer
factor
plays
an
indispensable
role
in
high
current
density
to
accelerate
the
oxygen
evolution
reaction
(OER)
process,
yet
research
on
modulating
reactant
mass
transport
remains
limited.
Herein,
by
leveraging
dual
acid‐base
properties
of
aluminum
sites,
both
activation
electronic
activity
layer
for
layered
double
hydroxides
(LDH)
and
construction
interlayer
hydroxide
coordination
field
(IHCF)
have
been
achieved
through
situ
electrochemical
reconstruction.
It
not
only
facilitates
charge
surface
catalytic
transformation
intermediates
but,
most
notably,
presence
IHCF
significantly
enhances
reactants.
As
a
result,
overpotential
LDHs
with
is
164
mV,
better
than
reported
Ni‐based
catalysts.
Deuterium
kinetic
isotope
effect
experiments
pH‐dependence
measurements
demonstrate
that
effectively
substrate
capability
structural
stability,
thereby
accelerating
proton‐coupled
electron
process.
To
further
validate
characteristics,
stability
tests
alkaline
flow
electrolyzer
show
catalysts
maintain
over
1000
h
at
density.
This
work
suggests
can
be
utilized
design
synthesis
efficient
water
oxidation
practical
application.
Advanced Energy Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Сен. 29, 2024
Abstract
Modulating
the
spin
states
of
FeN
4
moieties
is
critical
for
enhancing
electrocatalytic
oxygen
reduction
reaction
(ORR).
In
this
study,
Ti
N
3
Cl
x
and
O
MXenes
are
synthesized
functionalized
with
iron
phthalocyanine
(FePc)
to
form
model
catalysts
well‐defined
‐Cl‐Ti
‐O‐Ti
structures,
respectively.
The
structure,
formed
within
/FePc
composite,
enables
precise
modulation
from
low
intermediate
spin,
significantly
ORR
performance.
contrast,
structure
in
shows
less
effective
state
modulation,
leading
comparatively
lower
activity.
Compared
FePc
/FePc,
demonstrates
superior
electrochemical
performance,
an
half‐wave
potential
+0.91
V
versus
RHE
doubled
power
densities
Zn–air
batteries
(214.5
mW
cm
−2
).
Theoretical
studies
confirm
that
induced
by
weak‐field
ligand‐modified
facilitate
electron
filling
antibonding
orbital
composed
Fe
3dz
2
π*
orbitals,
greatly
O₂
activation
These
findings
underscore
catalytic
properties
compared
‐O‐Ti,
advancing
understanding
state‐related
mechanisms
guiding
design
high‐performance
catalysts.
Abstract
Alternative
strategies
to
design
sustainable‐element‐based
electrocatalysts
enhancing
oxygen
evolution
reaction
(OER)
kinetics
are
demanded
develop
affordable
yet
high‐performance
water‐electrolyzers
for
green
hydrogen
production.
Here,
it
is
demonstrated
that
the
spontaneous‐spin‐polarized
2D
π‐d
conjugated
framework
comprising
abundant
elements
of
nickel
and
iron
with
a
ratio
Ni:Fe
=
1:4
benzenehexathiol
linker
(BHT)
can
improve
OER
by
its
unique
electronic
property.
Among
bimetallic
NiFe
x:y
‐BHTs
various
ratios
x:y,
‐BHT
exhibits
highest
activity.
The
shows
specific
current
density
140
A
g
−1
at
overpotential
350
mV.
This
performance
one
best
activities
among
state‐of‐the‐art
non‐precious
even
comparable
platinum‐group‐metals
RuO
2
IrO
.
functional
theory
calculations
uncover
introducing
Ni
into
homometallic
Fe‐BHT
(e.g.,
0:1)
emerge
state.
Thus,
this
material
achieve
improved
spin‐polarization
which
previously
required
external
magnetic
fields.
work
rational
frameworks
be
powerful
strategy
synthesize
promising
wide
spectrum
next‐generation
energy
devices.
Abstract
Mass
transfer
factor
plays
an
indispensable
role
in
high
current
density
to
accelerate
the
oxygen
evolution
reaction
(OER)
process,
yet
research
on
modulating
reactant
mass
transport
remains
limited.
Herein,
by
leveraging
dual
acid‐base
properties
of
aluminum
sites,
both
activation
electronic
activity
layer
for
layered
double
hydroxides
(LDH)
and
construction
interlayer
hydroxide
coordination
field
(IHCF)
have
been
achieved
through
situ
electrochemical
reconstruction.
It
not
only
facilitates
charge
surface
catalytic
transformation
intermediates
but,
most
notably,
presence
IHCF
significantly
enhances
reactants.
As
a
result,
overpotential
LDHs
with
is
164
mV,
better
than
reported
Ni‐based
catalysts.
Deuterium
kinetic
isotope
effect
experiments
pH‐dependence
measurements
demonstrate
that
effectively
substrate
capability
structural
stability,
thereby
accelerating
proton‐coupled
electron
process.
To
further
validate
characteristics,
stability
tests
alkaline
flow
electrolyzer
show
catalysts
maintain
over
1000
h
at
density.
This
work
suggests
can
be
utilized
design
synthesis
efficient
water
oxidation
practical
application.
