Journal of the American Chemical Society,
Год журнала:
2025,
Номер
unknown
Опубликована: Март 5, 2025
Atomic
defects,
e.g.,
vacancies,
substitutions,
and
dopants,
play
crucial
roles
in
determining
the
functionalities
of
two-dimensional
(2D)
materials,
including
spin
glass,
single-photon
emitters,
energy
storage
conversion,
due
to
introduction
abnormal
charge
states
noncentrosymmetric
distortion.
In
particular,
anti-substitutions
are
regarded
as
promising
topological
defect
types,
which
substitution
occurs
at
opposite
sites,
fundamentally
modifying
atomic
electronic
structures
pristine
lattices.
However,
fabrication
large-scale
remains
challenging
high
formation
energies
complex
reaction
paths.
Here,
we
propose
an
approach
for
synthesizing
atomically
dispersed
Pt
defective
1T'-MoTe2
using
electrochemical
exfoliation-assisted
leaching-redeposition
(EELR)
method.
Atomic-resolution
scanning
transmission
electron
microscopy
(STEM)
imaging
reveals
that
atoms
substitute
Te
forming
unconventional
Mo-Pt
bonds.
A
rich
variety
anti-substitution
configurations
coupling
with
vacancies
have
been
fabricated
by
controlled
conditions.
Density
functional
theory
(DFT)
calculations
suggest
preferentially
occupy
vacancy
sites
coupled
neighboring
stabilizing
configurations.
The
Pt-Te
complexes
exhibit
excellent
hydrogen
evolution
reaction,
overpotential
only
12.9
mV
because
paired
cause
redistribution
regulate
d-band
center
active
suggested
DFT.
These
findings
introduce
effective
engineering
2D
presenting
new
opportunities
precise
design
features
targeted
catalytic
other
advanced
applications.
Journal of Materials Chemistry A,
Год журнала:
2023,
Номер
11(44), С. 23653 - 23682
Опубликована: Янв. 1, 2023
Defect
engineering
is
an
effective
strategy
to
control
the
performance
of
photocatalyst
and
electrocatalyst.
This
review
highlights
key
role
cationic
vacancy
from
aspects
synthesis
methods,
testing
techniques
applications.
Chemical Society Reviews,
Год журнала:
2024,
Номер
unknown
Опубликована: Янв. 1, 2024
This
review
focuses
on
the
synthesis
and
characterization
of
defective
electrocatalysts,
internal
correlation
between
defects
catalytic
activity,
development
application
electrocatalysts
in
various
fields.
Advanced Functional Materials,
Год журнала:
2024,
Номер
34(27)
Опубликована: Март 5, 2024
Abstract
Electrocatalytic
hydrogen
evolution
and
(S
2−
)
recycling
present
promising
strategies
for
cost‐effective
production
simultaneous
removal
of
environmental
pollutants.
However,
the
advancement
this
technology
is
hindered
by
limited
availability
affordable,
efficient,
stable
catalysts.
Herein,
study
synthesizes
ultrafine
ruthenium
(Ru)
nanoclusters
on
a
substrate
iron
molybdenum
sulfide
(FeMo‐S)
nanosheets,
creating
new
heterointerface
catalyst
(FeMo‐S/Ru)
reaction
(HER)
sulfion
oxidation
(SOR).
Experimental
theoretical
calculations
suggest
that
strong
electron
interactions
between
Ru
FeMo‐S
substrate,
optimizing
*H
adsorption
promoting
HER
activity
one
side
while
facilitating
sulfur
intermediates
other
side,
effectively
catalyzing
SOR.
Additionally,
assembled
electrocatalytic
coupling
system
with
FeMo‐S/Ru
displays
an
ultralow
cell
voltage
0.57
V
at
100
mA
cm
−2
,
achieving
high
Faradaic
efficiencies
(>96%)
H
2
production,
also
exhibiting
remarkable
durability
over
1
month
(838
h).
This
work
paves
way
development
highly
efficient
durable
supported
catalysts,
enabling
energy‐saving
environmentally
friendly
recycling.
Abstract
The
development
of
a
cost‐competitive
and
efficient
electrocatalyst
is
both
attractive
challenging
for
hydrogen
production
by
evolution
reaction
(HER).
Herein,
facile
glycol
reduction
method
to
construct
Ru
nanoclusters
coupled
with
hierarchical
exfoliated‐MXene/reduced
graphene
oxide
architectures
(Ru‐E‐MXene/rGA)
reported.
structure,
formed
the
self‐assembly
oxides,
can
effectively
prohibit
self‐stacking
MXene
nanosheets.
Meanwhile,
formation
MXene/rGA
interface
strongly
trap
3+
ions,
resulting
in
uniform
distribution
within
Ru‐E‐MXene/rGA.
boosted
catalytic
activity
underlying
mechanism
during
HER
process
are
proved
density
functional
theory.
Ru‐E‐MXene/rGA
exhibits
overpotentials
42
62
mV
at
10
mA
cm
−2
alkaline
acidic
electrolytes,
respectively.
small
Tafel
slope
charge
transfer
resistance
(
R
ct
)
values
elucidate
its
fast
dynamic
behavior.
cyclic
voltammetry
(CV)
curves
chronoamperometry
test
confirm
high
stability
These
results
demonstrate
that
coupling
heterostructure
represents
an
strategy
constructing
MXene‐based
catalysts
enhanced
activity.
Advanced Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Янв. 19, 2025
Abstract
Efficient
charge
separation
at
the
semiconductor/cocatalyst
interface
is
crucial
for
high‐performance
photoelectrodes,
as
it
directly
influences
availability
of
surface
charges
solar
water
oxidation.
However,
establishing
strong
molecular‐level
connections
between
these
interfaces
to
achieve
superior
interfacial
quality
presents
significant
challenges.
This
study
introduces
an
innovative
electrochemical
etching
method
that
generates
a
high
concentration
oxygen
vacancy
sites
on
BiVO
4
surfaces
(Ov‐BiVO
),
enabling
interactions
with
oxygen‐rich
ligands
MIL‐101.
reduces
formation
energy
and
promotes
conformal
growth
.
The
Ov‐BiVO
/MIL‐101
composite
exhibits
ideal
interface,
achieving
impressive
photocurrent
density
5.91
mA
cm
−2
1.23
V
RHE
,
along
excellent
stability.
high‐performing
photoanode
enables
unbiased
tandem
device
/MIL‐101‐Si
cell
system,
solar‐to‐hydrogen
efficiency
4.33%.
integration
mitigates
states
enhances
internal
electric
field,
facilitating
migration
photogenerated
holes
into
MIL‐101
overlayer.
process
activates
highly
efficient
Fe
catalytic
sites,
which
effectively
adsorb
molecules,
lowering
barrier
oxidation
improving
kinetics.
Further
studies
confirm
broad
applicability
vacancy‐induced
molecular
epitaxial
in
various
MOFs,
offering
valuable
insights
defect
engineering
optimizing
enhancing
photocatalytic
activity.
Advanced Functional Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Сен. 2, 2024
Abstract
Given
the
pronounced
dissolution
of
electrocatalysts
in
acidic
environments,
quest
for
effective
oxygen
evolution
reaction
(OER)
suitable
proton
exchange
membrane
(PEM)
water
electrolyzers
persists
as
a
formidable
challenge.
In
this
investigation,
catalysts
are
synthesized
by
creating
vacancies
within
various
metal
oxides
(Nb
2
O
5‐x
,
Ta
ZrO
2‐x
TiO
)
through
plasma‐assisted
method,
thereby
facilitating
immobilization
IrO
onto
these
defect‐rich
surfaces.
The
findings
unveil
that
/Nb
manifests
reduced
overpotentials
during
OER,
achieving
an
overpotential
down
to
225
mV@10
mA
cm
−2
coupled
with
outstanding
durability
at
multicurrent
densities
exceeding
200
h,
attributed
strong
oxide‐support
interaction
(SOSI)
between
catalyst
and
Nb
substrate.
Density
functional
theory
(DFT)
computations
uncover
intensified
binding
affinities
thus
modulating
central
energy
levels
Ir's
d
orbitals
toward
favorable
OER
conditions,
consequently
bolstering
electrocatalytic
activity
stability
composite
catalyst.
Furthermore,
employing
PEM
electrolyzer
anode
enables
consistent
operation
1000
Ir
content
only
0.2852
mg
consumption
4.34
kWh
Nm
−3
H
.
This
achievement
substantially
lowers
cost
hydrogen
production
US$
0.96
per
kilogram,
underscoring
its
potential
practical
applications.
ACS Nano,
Год журнала:
2024,
Номер
18(29), С. 19268 - 19282
Опубликована: Июль 9, 2024
Catalytic
additives
able
to
accelerate
the
lithium–sulfur
redox
reaction
are
a
key
component
of
sulfur
cathodes
in
batteries
(LSBs).
Their
design
focuses
on
optimizing
charge
distribution
within
energy
spectra,
which
involves
refinement
and
occupancy
electronic
density
states.
Herein,
beyond
distribution,
we
explore
role
spin
configuration
polysulfide
adsorption
properties
catalytic
activity
additive.
We
showcase
importance
this
parameter
by
generating
polarization
through
defect
engineering
approach
based
introduction
Co
vacancies
surface
CoSe
nanosheets.
show
change
electron
state
increasing
number
unpaired
electrons
with
aligned
spins.
This
local
rearrangement
enhances
adsorption,
reducing
activation
Li–S
reactions.
As
result,
more
uniform
nucleation
growth
Li2S
an
accelerated
liquid–solid
conversion
LSB
obtained.
These
translate
into
exhibiting
capacities
up
1089
mA
h
g–1
at
1
C
0.017%
average
capacity
loss
after
1500
cycles,
5.2
cm–2,
0.16%
decay
per
cycle
200
cycles
high
loading
cells.
Nano-Micro Letters,
Год журнала:
2025,
Номер
17(1)
Опубликована: Янв. 31, 2025
Transition
metal
carbides,
known
as
MXenes,
particularly
Ti3C2Tx,
have
been
extensively
explored
promising
materials
for
electrochemical
reactions.
However,
transition
carbonitride
MXenes
with
high
nitrogen
content
reactions
are
rarely
reported.
In
this
work,
incorporated
Pt-based
electrocatalysts,
ranging
from
single
atoms
to
sub-nanometer
dimensions,
hydrogen
evolution
reaction
(HER).
The
fabricated
Pt
clusters/MXene
catalyst
exhibits
superior
HER
performance
compared
the
single-atom-incorporated
MXene
and
commercial
Pt/C
in
both
acidic
alkaline
electrolytes.
optimized
sample
shows
low
overpotentials
of
28,
65,
154
mV
at
a
current
densities
10,
100,
500
mA
cm-2,
small
Tafel
slope
29
dec-1,
mass
activity
1203
mgPt-1
an
excellent
turnover
frequency
6.1
s-1
electrolyte.
Density
functional
theory
calculations
indicate
that
can
be
attributed
enhanced
active
sites,
increased
surface
groups,
faster
charge
transfer
dynamics,
stronger
electronic
interaction
between
MXene,
resulting
absorption/desorption
toward
better
HER.
This
work
demonstrates
may
candidates
various
catalytic
by
incorporating
or
clusters.
