Journal of the American Chemical Society,
Год журнала:
2025,
Номер
unknown
Опубликована: Июнь 4, 2025
Efficient
seawater
oxidation
reaction
is
crucial
for
advancing
hydrogen
fuel
production.
Developing
highly
efficient
oxygen
evolution
(OER)
catalysts
that
follow
the
lattice
mechanism
(LOM)
can
effectively
mitigate
undesirable
chloride
side
reactions
in
electrolysis
and
reduce
energy
consumption.
Herein,
we
propose
a
Cl--mediation
strategy
able
to
shift
OER
from
adsorbate
(AEM)
LOM
on
nickel
sites.
By
loading
dispersed
Ir
onto
Ni-based
precursors
(e.g.,
NiSe,
Ni(OH)2,
NiS2
NiSOH),
exploit
robust
coordination
interaction
between
Cl-
establish
Cl-Ir-O-Ni
electron-withdrawing
chain
Ni
Cl,
which
strengthens
Ni-O
covalency
situ
during
OER,
thereby
activating
around
sites
seawater.
As
result,
Cl-modified
Ir/NiOOH-Se@Cl
catalyst
requires
an
overpotential
of
only
313
mV
achieve
current
density
0.5
A
cm-2,
demonstrating
reduction
147
compared
alkaline
condition
(Ir/NiOOH-Se@OH)
also
maintaining
stable
operation
at
cm-2
500
h.
Our
work
provides
novel
intriguing
concept
regulating
local
activity
toward
developing
electrocatalysts
clean
productions.
Advanced Functional Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Апрель 7, 2025
Abstract
The
NiFe‐based
layered
double
hydroxides
(LDH)
undergo
surface
reconstruction,
generating
metal
hydroxyl
oxides
that
act
as
active
species
during
the
alkaline
oxygen
evolution
reaction
(OER).
However,
sluggish
reconstruction
process
and
excessive
oxidation
at
higher
anodic
potentials
frustrate
OER
activity
stability.
Herein,
a
cation–anion
collaborative
coordination
strategy
is
harnessed
to
build
(Ni,
Fe)─S─Zn
structures
in
NiFe
LDH
on
nickel
foam
(S‐NiFeZn
LDH/NF),
which
lowers
energy
barrier
aids
forming
highly
β‐NiOOH
process.
Meanwhile,
also
optimize
adsorption
of
oxygen‐containing
intermediates,
enhancing
kinetics.
As
result,
S‐NiFeZn
LDH/NF
achieves
low
overpotentials
201
mV
10
mA
cm
−2
293
500
1.0
m
KOH.
Moreover,
cell
assembled
with
anode
commercial
NiMo
cathode
demonstrates
excellent
overall
water
splitting
activity,
voltages
1.62
1.81
V
KOH,
exhibits
ultralong‐term
durability
over
h
,
even
operating
stably
for
200
an
electrolyzer
under
industrial
conditions
(30%
KOH
80
°C).
Advanced Functional Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Март 25, 2025
Abstract
The
arrangement
of
atoms
in
the
catalyst
directly
impacts
catalytic
performance.
Herein,
a
heteroatom
doping
strategy
is
found
as
an
effective
approach
for
regulation
MnO
2
crystal
reconstruction
during
oxygen
evolution
reaction
(OER),
thereby
ensuring
and
optimizing
performance
catalyst.
Real‐time
tracking
dynamic
surface
reveals
that
δ‐MnO
transforms
into
less
active
γ‐MnOOH
phase,
while
single‐atom
Fe
facilitates
formation
highly
α‐MnOOH
phase.
asymmetric
Fe─O─Mn
bonds
induce
lattice
distortions
promote
electron
transfer
from
to
Mn
with
increase
3
⁺
content,
which
conducive
intensifying
spillover
crucial
factor
OER
activity.
Theoretical
calculations
also
demonstrate
sites
regulated
representative
can
reduce
energy
barrier
step
process
(the
*O
*OOH
transition),
thus
significantly
enhancing
typical
achieves
successful
processes
through
doping,
holds
significant
implications
developing
new
class
catalysts,
not
limited
catalysts
reported
this
study.
Journal of the American Chemical Society,
Год журнала:
2025,
Номер
unknown
Опубликована: Фев. 12, 2025
The
interest
in
aqueous
energy
storage
devices
is
surging
due
to
their
exceptional
safety
profile.
However,
systems,
interfacial
side
reactions,
predominantly
attributed
the
oxygen
evolution
reaction
(OER),
result
significant
self-discharge,
which
concomitant
with
deterioration
of
both
voltage
and
capacity.
Herein,
we
propose
construction
a
ferrocyanide
"skin"
on
transition
metal
compounds
(TMCs)
mitigate
this
issue.
This
engineered
creates
Fe–C≡N
terminations,
initiating
new
pathway
featured
by
bonding
process
N–O
N–H
bonds.
presents
barrier,
effectively
shielding
active
sites
for
OER
from
H2O
molecules
hydroxyl
ions.
Taking
NiO
as
an
example,
suppresses
undesired
phase
NiOOH
Ni(OH)2
during
idling
fully
charged
electrode,
enabling
as-modified
electrode
achieve
remarkable
retention
80.0%
after
1
week
within
device.
Furthermore,
concept
demonstrates
extensive
applicability,
extending
range
TMC
materials,
including
but
not
limited
manganese
oxide,
vanadium
nickel
cobalt
oxide.
These
findings
highlight
efficacy
design
strategy
broadly
applicable
paradigm
suppressing
H2O-induced
undesirable
transitions
devices.
Abstract
The
production
of
hydrogen
from
seawater
offers
a
potential
pathway
to
accomplish
sustainable
energy
solutions.
However,
this
process
is
impeded
by
the
sluggish
kinetics
evolution
reaction
(HER)
and
corrosive
nature
seawater.
In
work,
an
FeRu
alloy
electrocatalyst
integrated
with
Mo
substrate
(FeRu/MoO
2
@Mo)
developed,
specifically
designed
for
HER
in
both
alkaline
environments.
FeRu/MoO
@Mo
catalyst
demonstrated
remarkable
performance,
achieving
overpotentials
only
22,
42,
65
mV
solution,
simulated
seawater,
real
at
10
mA
cm
−2
.
Moreover,
exhibited
long‐term
stability
HER,
maintaining
its
activity
least
400
h
under
conditions
1
m
KOH.
situ
Raman
spectroscopy
theoretical
calculations
revealed
incorporation
Fe
reduces
density
states
near
Fermi
level
Ru,
thereby
optimizing
adsorption–desorption
behavior
enhancing
activity.
This
work
scalable
cost‐effective
strategy
development
efficient
non‐platinum
catalysts.
