Advanced Functional Materials,
Journal Year:
2025,
Volume and Issue:
unknown
Published: Jan. 10, 2025
Abstract
Developing
overall
water
splitting
non‐noble
metal
electrocatalysts
achieving
long‐term
stability
with
high
activity
at
industrial‐grade
current
density
remains
challenging.
Herein,
a
self‐reconstruction
strategy
of
Co
9
S
8
‐Ni
3
2
/NCF
is
employed
to
fabricate
Ni
x
3‐x
O
4
‐Ov‐
in
which
partial
replaced
by
the
structure.
The
reconstructed
‐Ov
can
enhance
adsorbing
ability
leached
from
initial
phase
compared
spinel,
exceeding
1000‐h
oxygen
evolution
reaction
(OER)
and
600‐h
1000
mA
cm
−2
excellent
activity.
In
situ
Raman
X‐ray
photoelectron
spectroscopy
(XPS)
results
indicate
that
substitution
for
atoms
enhances
adsorption
capacity
on
‐Ov,
facilitating
formation
high‐density
3+
active
sites
(400)
expedited
interfacial
electron
transfer
densities.
Density
functional
theory
(DFT)
calculations
reveal
stabilizes
surface
vacancies
optimizes
energy
intermediates,
thereby
improving
both
catalytic
performance.
findings
provide
new
insights
into
overcoming
activity‐stability
trade‐off
contribute
design
Small,
Journal Year:
2025,
Volume and Issue:
21(7)
Published: Jan. 7, 2025
Abstract
Modulating
electronic
structure
to
balance
the
requirement
of
both
hydrogen
evolution
reaction
(HER)
and
oxygen
(OER)
is
crucial
for
developing
bifunctional
catalysts.
Herein,
phase
transformation
engineering
utilized
separately
regulate
catalyst
structure,
designed
NiFe@Ni/Fe‐MnOOH
schottky
heterojunction
exhibits
remarkable
electrocatalytic
activity
with
low
overpotentials
19
230
mV
at
10
mA
cm
−2
HER
OER
in
1M
KOH,
respectively.
Meanwhile,
an
anion‐exchange
membrane
water
electrolyzer
employing
as
electrodes
shows
voltages
1.487/1.953
V
10/1000
,
operating
over
200
h
1000
.
Combining
theoretical
calculations
experiments
reveal
that
can
differentially
active
phases
HER/OER.
In
HER,
Ni/Fe‐MnOOH
metallic
NiFe
act
*OH
*H
acceptors
respectively
accelerates
dissociation
subsequent
Heyrovsky/Tafel
step.
While
OER,
significant
Jahn‐Teller
effect
Mn
3+
induces
surface
reconstruction
from
Ni/Fe‐MnO
2
The
formative
high
value
4+
modify
M‐O
hybridization
activate
lattice
mechanism,
which
pivotal
breaking
restriction
volcanic
relationship
reducing
overpotential.
These
findings
provide
valuable
design
guidelines
high‐performance
multi‐functional
electrocatalysts
via
engineering.
Advanced Energy Materials,
Journal Year:
2025,
Volume and Issue:
unknown
Published: Feb. 23, 2025
Abstract
Integrating
ferroelectric
materials
with
semiconductor
photocatalysts
offers
a
groundbreaking
strategy
to
enhance
solar‐driven
hydrogen
production
by
improving
charge
separation
and
transfer
efficiency.
Herein,
synergistic
system
is
developed
coupling
the
tunable
polarization
of
BaTiO
3
(BTO)
Z‐scheme
heterojunction
in
Zn
0.5
Cd
S
quantum
dots
(ZCS
QDs).
The
strong
adjustable
built‐in
electric
field
generated
BTO
effectively
drives
carrier
separation,
enhances
interfacial
band
bending,
mitigates
excitonic
effects
commonly
observed
QDs,
facilitating
directional
transfer.
Mechanistic
insights,
validated
situ
X‐ray
photoelectron
spectroscopy
(XPS)
Kelvin
Probe
Force
Microscopy
(KPFM),
highlight
pivotal
role
modulating
dynamics
interactions.
These
attributes,
resulting
from
heterojunction,
enable
ZCS
QDs/BTO
composite
achieve
an
outstanding
evolution
rate
0.83
mmol
g
−1
h
,
surpassing
pure
QDs
factors
20.8
1.7,
respectively.
Notably,
external
further
amplifies
1.19
representing
remarkable
143%
increase
compared
pristine
showcasing
polarization‐enhanced
fields
photocatalysis.
This
work
presents
novel
pathway
for
designing
advanced
photocatalysts,
providing
promising
prospects
sustainable
production.
Designing
a
bimetallic
selenide-based
heterostructure
that
possesses
high
catalytic
efficiency,
capacity,
and
rate
capability
remains
challenging
due
to
constraints
imposed
by
slow
reaction
kinetics,
inadequate
electrode
utilization,
significant
volume
deformation.
In
this
study,
we
successfully
engineer
comprising
carbon
nanotubes
intertwined
with
sea
urchin-like
Bi2Se3@NiSe2
nanostructures
having
electronic
conductivity,
specific
sufficiently
exposed
active
sites,
favorable
charge
carrier
migration.
The
interface
engineering
of
the
multilevel
nanostructure
on
nanotube
(CNT)
framework
synergistically
reduces
energetic
barriers
accelerates
oxygen
evolution
kinetics
as
well
promotes
faster
Faradaic
reactions
enhance
storage.
As
consequence,
as-designed
flexible
supercapacitor
device
(Bi2Se3@NiSe2-CNT/CTs//AC-CNT/CTs)
attains
peak
energy
density
75.93
Wh
kg-1
maximum
power
15.12
kW
kg-1,
demonstrating
remarkable
durability
(94.35%
capacitance
retention)
after
40k
cycles.
higher
states
near
Fermi
level
in
hybrid
enhances
conductivity
mobility,
coupled
efficient
OH-
adsorption
(ΔEa
=
-4.352
eV@Bi
site,
ΔEa
-4.932
eV@Ni
site),
thereby
trapping
more
electrolyte
ions
promoting
redox
reactions.
Additionally,
induced
interactions
between
core
selenides
surface-generated
thin
layers
hydroxide/oxide
accelerate
terms
lower
overpotential
(199
mV@20
mA
cm-2),
Tafel
slope
(59.2
mV
dec-1),
electrochemical
surface
area
(1460.0
cm2)
toward
evolution.
proposed
study
construction
dual
redox-active
site
heterostructures
is
expected
create
avenues
for
advancing
renewable
systems.
Advanced Functional Materials,
Journal Year:
2024,
Volume and Issue:
unknown
Published: Aug. 2, 2024
Abstract
Aiming
to
efficiently
expedite
alkaline
overall
water
splitting
(OWS)
by
addressing
challenges
such
as
sluggish
kinetics
and
limited
stability,
a
hollow
Fe‐doped
Ni(OH)
2
‐NiS@Ni(OH)
nanorod
array
with
surface
nanosheets
is
devised,
featuring
high‐index
(101)‐NiS(211)
heterostructural
interface
an
upshifted
d
‐band
center.
This
nanoarchitecture
intensifies
the
adsorption
interaction
of
H
O
OH
−
reactants
on
electrocatalyst
surface,
suitably
bonds
*
intermediate
in
hydrogen
evolution
reaction
(HER)
accelerates
electron
movement
H,
minimizes
energy
requirement
rate‐limiting
phase
(
→
O)
oxygen
(OER)
facilitating
O─H
cleavage
optimally
adsorbs
O,
amplifies
exposure
surface‐active
centers,
ultimately
reduces
apparent
activation
energy.
Consequently,
overpotentials
are
low
66.4
mV
254.9
at
10
mA
cm
−2
,
alongside
high
turnover
frequencies
142
s
−1
(H
)
279
(O
100
300
mV,
respectively,
markedly
outperforming
direct‐electrodeposited
analogues.
When
functioning
bifunctional
electrode
OWS,
this
material
merely
requires
1.57
V
sustains
operation
for
168
h,
approaching
Pt/C||RuO
benchmark.
ACS Catalysis,
Journal Year:
2024,
Volume and Issue:
14(20), P. 15665 - 15674
Published: Oct. 7, 2024
Understanding
the
sluggish
kinetics
of
hydrogen
evolution
reaction
(HER)
in
neutral
media
is
a
grand
challenge.
The
correlation
between
interfacial
water
structure
and
HER
activity
has
yet
to
be
determined,
particularly
for
catalysts
with
complex
chemical
compositions.
Herein,
we
used
situ
electrochemical
spectroscopic
methods
(e.g.,
surface-enhanced
infrared
absorption
shell-isolated
nanoparticle-enhanced
Raman
spectroscopy)
investigate
bonding
network
molecules
typical
Pt/C
NiCo-phosphide,
-sulfide,
-hybrid
with/without
oxide
impurity)
under
potential
bias
media.
cathodic
potentials
always
influenced
composition
water,
rendering
records
distinct
nominal
tuning
rates
among
different
catalysts.
Interestingly,
found
that
suitable
amount
surface
impurity,
inert
phase,
can
drastically
alter
dynamic
behaviors
promoting
transition
from
ice-like
liquid-like
free
while
leading
an
improved
performance
(j0
>
0.7
mA
cm–2;
η
=
101.7
mV@10
cm–2).
Such
effect
was
presumably
correlated
hydrophilic
moieties,
as
evidenced
by
studies
pure
hydroxide
controls.
This
work
provides
insights
understanding
media,
paving
way
rational
design
electrocatalysts.
Advanced Energy Materials,
Journal Year:
2024,
Volume and Issue:
unknown
Published: Nov. 19, 2024
Abstract
Electrocatalytic
water
splitting
is
an
attractive
approach
for
large‐scale
hydrogen
generation,
critical
global
carbon
neutrality.
However,
the
prevalent
commercialized
alkaline
electrolysis
generally
conducted
at
low
current
densities
due
to
sluggish
kinetics
and
high
overpotential,
severely
hampering
high‐efficiency
production.
Exploration
of
evolution
reaction
(HER)
electrocatalysts
that
can
reliably
operate
ampere‐level
under
overpotentials
thus
a
primary
challenge.
In
contrast
extensive
studies
using
powdery
electrocatalysts,
self‐supported
metallic
catalytic
cathode
has
become
burgeoning
direction
toward
densities,
owing
their
integrated
design
with
intensive
interfacial
binding,
conductivity
mechanical
stability
industrial
tolerance/adaption.
Recent
years
have
witnessed
tremendous
research
advances
in
designing
electrocatalysts.
Therefore,
this
flourishing
area
specially
summarized.
Beginning
introduction
theory
mechanism
HER,
engineering
strategies
on
electrodes
are
systematically
summarized,
including
metal
alloy
construction,
heterostructure
engineering,
doping
manipulation,
surface
design.
Meanwhile,
particular
emphasis
focused
relationship
between
structure,
activity,
HER.
Finally,
existing
challenges,
requirements
industrial‐scale
application,
future
aiming
provide
better
solution
electrolysis.
