Advanced Materials,
Journal Year:
2025,
Volume and Issue:
unknown
Published: May 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.
Inorganic Chemistry,
Journal Year:
2025,
Volume and Issue:
unknown
Published: May 2, 2025
Developing
cost-effective
electrocatalysts
for
efficient
seawater
splitting
requires
a
fundamental
understanding
of
the
oxygen
evolution
reaction
(OER)
mechanism.
Herein,
iron-doped
nickel
phosphide
(Fe-Ni2P)
is
synthesized
via
hydrothermal-impregnation-phosphidation
strategy
to
investigate
role
Fe
incorporation
in
modulating
electronic
structure
and
OER
pathways.
Mechanistic
investigations
demonstrate
that
doping
triggers
shift
from
adsorbate
mechanism
(AEM)
lattice
oxygen-mediated
(LOM)
pathways,
evidenced
by
pH-dependent
kinetics,
tetramethylammonium
cation
probing,
situ
electrochemical
impedance
spectroscopy
(EIS).
The
LOM
involves
nonconcerted
proton-electron
transfers,
facilitated
accelerated
hydroxide
adsorption
(ks
=
0.275
s-1)
dynamic
surface
reconstruction
into
amorphous
NiOOH.
reduced
activation
energy
(27.1
kJ
mol-1)
lower
charge-transfer
resistance
Fe-Ni2P
underscore
its
superior
thermodynamics
kinetics.
X-ray
photoelectron
EIS
further
validate
vacancy
accumulation
during
process.
Electrochemical
studies
reveal
exhibits
low
overpotential
220
mV
at
10
mA
cm-2
remarkable
stability
through
phosphate-mediated
Cl-
repulsion
involving
alkaline
seawater.
This
work
establishes
Fe-induced
modulation
as
critical
activating
LOM-dominated
catalysis
transition
metal
phosphides.
Advanced Materials,
Journal Year:
2025,
Volume and Issue:
unknown
Published: May 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.
