ACS Applied Materials & Interfaces,
Год журнала:
2024,
Номер
unknown
Опубликована: Ноя. 6, 2024
High-voltage
LiNixCoyMn(1–x–y)O2
(NCM)
is
one
of
the
most
promising
cathode
materials
for
high-energy-density
lithium
metal
batteries.
Significant
efforts
have
been
made
on
inhibiting
surface
transition
NCM
from
ordered
layered
phase
to
low-ionic-conductivity
rock
salt
phase,
which
facilitates
maintaining
a
low
interfacial
impedance
superior
cycle
performance.
However,
it
often
overlooked
that
also
has
electronic
conductivity,
may
alleviate
notorious
growth
dendrite-induced
short-circuit.
In
this
article,
we
further
demonstrate
effective
in
resisting
pulverization
contact
with
Li
via
situ
transmission
electron
microscopy.
The
experiences
rapid
overlithiation
Li,
triggers
lattice
expansion
and
pulverization.
overlithiation-induced
degradation
retarded
Li-deficient
disorder
surface,
attributed
blocked
Li+
primary
path.
Our
work
revisits
unwanted
layer
cathodes,
provides
guideline
interface
design
long-cycling
high-safety
Advanced Functional Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Фев. 2, 2025
Abstract
The
structural
instability
of
lithium‐based
transition
metal
layered
oxides
during
electrochemical
cycling‐exacerbated
by
phenomena
such
as
dissolution
and
phase
transitions‐induces
rapid
capacity
degradation,
thus
constraining
their
applicability
in
high‐energy‐density
lithium
batteries.
While
coating
these
materials
can
bolster
stability,
the
employment
electrochemically
inactive
coatings
may
inadvertently
undermine
energy
storage
performance,
presenting
a
significant
trade‐off.
In
response
to
this
challenge,
an
innovative
core‐shell
cathode
architecture
is
presented,
wherein
high
entropy
doped
LiNi
1/6
Mn
Al
Ti
Mo
Ta
O
2
serves
shell
nickel‐rich
cobalt‐free
0.89
0.11
constitutes
core,
synthesized
through
simple
two‐step
co‐precipitation
methodology
(designated
LHECNM).
This
high‐entropy
preserves
core's
performance
while
effectively
mitigating
transformations
ion
dissolution,
thereby
enhancing
robustness.
Moreover,
configuration
significantly
diminishes
barrier
for
Li
+
diffusion,
facilitating
superior
transport
dynamics.
Consequently,
LHECNM
demonstrates
remarkable
achieving
discharge
201.57
mAh
g
−1
,
commendable
rate
capability
up
5C,
impressive
92%
retention
over
prolonged
cycling.
investigation
elucidates
promising
paradigm
design
materials,
offering
profound
insights
advancement
future
technologies.
Advanced Functional Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Ноя. 3, 2024
Abstract
Elevating
the
charging
cut‐off
voltage
is
an
effective
strategy
to
increase
energy
density
of
LiCoO
2
.
However,
unstable
interfacial
structures
and
unfavorable
phase
transitions
in
bulk
are
inevitably
triggered
during
deep
de‐lithiation
at
high
voltage.
Herein,
integrated
surface‐to‐bulk
Ti‐modification
applied
,
enabling
uniform
Li
TiO
3
coating
on
surface
gradient
Ti‐doping
toward
structural
bulk.
The
resultant
Ti‐modified
(T‐LCO)
electrode
can
be
stably
cycled
up
4.6
V,
providing
a
high‐rate
capability
137
mAh
g
−1
5C
long‐life
stability
with
80.5%
capacity
retention
after
400
cycles
1C,
far
outperforming
unmodified
only
50.7%
retention.
In
situ
X‐ray
diffraction
characterization
functional
theory
calculation
reveal
that
synergistic
modification
T‐LCO
enhances
+
diffusion,
facilitates
construction
high‐quality
cathode/electrolyte
interphase,
reduces
transition
from
O3
H1‐3
Co3d/O2p
band
overlap,
restrains
layer‐to‐spinel
distortion,
thus
improving
V.
This
work
presents
“two
birds
one
step”
enhance
cycling
achievable
high‐voltage
for
developing
lithium‐ion
batteries.
Advanced Functional Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Ноя. 22, 2024
Abstract
The
development
of
rechargeable
lithium
batteries
(RLBs)
has
made
a
great
contribution
in
solving
the
problems
current
era,
such
as
energy
shortage
and
climate
change.
With
expanding
application
field
RLBs
from
portable
device
to
large‐scale
electric
equipment,
it
is
an
urgent
demand
for
operate
wide
range
temperature.
More
more
attention
been
paid
design
wide‐temperature
RLBs.
Therefore,
timely
critical
overview
latest
operating
at
temperatures
needed.
In
this
review,
in‐depth
understanding
on
how
temperature
affects
thermodynamics
lithium‐ion
transport
electrodes,
electrolytes,
electrode/electrolyte
interfaces
emphasized.
Recent
progress
probing
effects
electrochemical
performance
fading
comprehensively
discussed.
Different
strategies
widen
working
RLBs,
including
regulating
electrode
degradation,
interface
evolution,
electrolyte
solvation
chemistry
are
also
reviewed.
Finally,
outlook
potential
future
research
directions
proposed,
which
sheds
light
novel
electrodes
electrolytes
next‐generation
temperatures.
ACS Applied Energy Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Янв. 23, 2025
Lithium-rich
manganese
layered
(LMR)
materials,
utilizing
the
characteristics
of
both
cation
and
anion
redox,
are
promising
cathodes
for
high-energy-density
lithium-ion
batteries.
However,
capacity
fading
voltage
decay
pose
challenges
to
their
commercial
applications.
In
this
work,
we
employ
chemical
bonding
integrate
Li3VO4
with
Li1.2Mn0.6Ni0.2O2,
leveraging
compatible
properties
form
a
stable
interface
address
related
challenges.
An
epitaxially
grown
coating
on
Li1.2Mn0.6Ni0.2O2
crystals
enhances
stability
at
electrode–electrolyte
while
also
improving
conduction.
Additionally,
strong
metal–oxygen
bonds
between
high-valence
V
element
effectively
lower
surface
oxygen
activity,
further
preventing
release
irreversible
phase
transitions.
assembled
half-cell
tests,
3
wt
%
Li3VO4-coated
exhibits
excellent
electrochemical
performance.
After
150
cycles
200
mA
g–1,
discharge
specific
reaches
188
h
retention
rate
as
high
93%.
Even
under
current
density
1000
remains
128
g–1
after
cycles.
This
study
highlights
significant
impact
bonded
lattice-matching
presenting
viable
design
strategy
developing
high-performance
LMR
cathodes.