Advanced Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Март 6, 2025
Ultra-high
nickel
layered
oxides
are
recognized
as
promising
cathode
candidates
for
high-energy-density
lithium-ion
batteries
due
to
their
enhanced
overall
capacity
and
elevated
operating
voltage.
However,
the
interlayer
sliding
of
transition
metal-oxygen
octahedra
(TMO6)
instability
lattice
oxygen
at
high
voltages
ultra-high
oxide
cathodes
pose
significant
challenges
development.
Herein,
origin
framework
stability
is
investigated
by
incorporating
high-covalent
element
Mo
in
both
bulk
surface
using
a
one-step
integrated
method
material
LiNi0.92Co0.08O2.
It
revealed
that
apart
from
isolation
protection
effect
Mo-enriched
layer,
suppression
Li/Ni
antisite
defects
Mo6+
with
strong
covalency
plays
critical
role
reducing
configurations
activated
anionic
redox
reaction
stabilizing
structure.
Benefiting
this,
reversibility
significantly
enhanced,
enabling
more
oxidized
exist
form
dimer
ions
O2n-$O_2^{n
-
}$
rather
than
being
lost
gaseous
O2.
Consequently,
modified
demonstrates
improved
diffusion
kinetics
optimized
electrochemical
performance
Advanced Energy Materials,
Год журнала:
2023,
Номер
13(34)
Опубликована: Июль 16, 2023
Abstract
Introducing
additional
elements
into
Ni‐rich
cathodes
is
an
essential
strategy
for
addressing
the
instability
of
cathode
material.
Conventionally,
this
doping
considers
only
incorporation
bulk
structure
in
terms
fortifying
crystal
structure.
However,
high‐valence
such
as
Nb
5+
,
Ta
and
Mo
6+
are
likely
to
be
insoluble
structure,
resulting
accumulation
along
interparticle
boundaries.
Herein,
a
new
mechanism
their
effects
on
morphology
investigated
by
calcining
LiNiO
2
(LNO)
X‐doped
LNO
(X
=
Al,
Nb,
Ta,
Mo)
at
various
temperatures.
Operando
X‐ray
diffraction
analysis
reveals
that
temperature
which
content
Li‐X‐O
compounds
declines
higher
dopants
with
high
oxidation
states,
reinforcing
segregation
grain
boundary
widening
calcination
range.
Thus,
highly
aligned
microstructure
crystallinity
maintained
over
wide
range
after
elements,
enhancing
electrochemical
performance.
As
next‐generation
dopants,
can
fortify
not
but
also
microstructure,
maximize
performance
cathodes.
The
development
of
advanced
layered
Ni-rich
cathodes
is
essential
for
high-energy
lithium-ion
batteries
(LIBs).
However,
the
prevalent
are
still
plagued
by
inherent
issues
chemomechanical
and
thermal
instabilities
limited
cycle
life.
For
this,
here,
we
introduce
an
efficient
approach
combining
single-crystalline
(SC)
design
with
in
situ
high-entropy
(HE)
doping
to
engineer
ultrahigh-Ni
cobalt-free
cathode
LiNi
Chemical Society Reviews,
Год журнала:
2024,
Номер
53(9), С. 4707 - 4740
Опубликована: Янв. 1, 2024
The
microstructural
degradation,
stabilization,
and
characterization
of
layered
Ni-rich
cathodes
for
Li-ion
batteries
are
comprehensively
reviewed
in
this
paper.
ACS Energy Letters,
Год журнала:
2024,
Номер
9(2), С. 740 - 747
Опубликована: Янв. 31, 2024
Doping
is
indispensable
for
ensuring
the
long-term
cycling
stability
of
Ni-rich
layered
cathodes.
However,
using
a
single
type
dopant
limits
development
stable,
high-energy
cathode
material
in
shot.
In
this
study,
dual
doping
strategy
Al3+
and
Nb5+
ions
was
adopted
to
improve
Li[Ni0.92Co0.04Mn0.04]O2
(NCM92)
cathode;
fortifies
crystal
structure,
while
optimized
morphology
primary
particles.
The
not
only
combines
benefits
both
dopants
simultaneously
but
also
demonstrates
excellent
performance
enhancement
through
synergistic
effects.
Li[Ni0.905Co0.04Mn0.04Al0.005Nb0.01]O2
(AlNb-NCM92)
cathode,
which
developed
Al
Nb,
exhibited
remarkable
stability,
retaining
88.3%
its
initial
capacity
even
after
1000
cycles.
This
result
suggests
that
needs
comprehensively
consider
structure
microstructure
maximize
materials.
Nano Energy,
Год журнала:
2024,
Номер
126, С. 109620 - 109620
Опубликована: Апрель 18, 2024
The
evolution
of
modern
society
demands
sustainable
rechargeable
lithium-ion
batteries
(LIBs)
with
higher
capacity
and
improved
safety
standards.
High
voltage
Ni-rich
layered
transition
metal
oxides
(i.e.,
LiNi1-x-yCoxMnyO2,
NCM)
have
emerged
as
one
the
most
promising
cathode
materials
in
meeting
this
demand.
However,
instability
NCMs
cathodes
presents
challenges
large-scale
commercialization.
This
review
examines
energy
storage
mechanism,
e.g.,
possible
(electro)chemical
reactions,
occurring
at
bulk
surface
degradation
mechanism
materials.
To
address
challenging
issue,
we
highlight
recent
advances
strategies
for
engineering
NCMs,
including
lattice,
composition,
microstructure
engineering,
electrolyte
interfacial
engineering.
By
addressing
mechanisms
improving
overall
stability,
work
sheds
lights
on
potential
avenues
commercialization
cathode-based
high-performance
LIBs.
Nature Communications,
Год журнала:
2024,
Номер
15(1)
Опубликована: Фев. 19, 2024
Abstract
Nickel-rich
layered
oxide
cathodes
promise
ultrahigh
energy
density
but
is
plagued
by
the
mechanical
failure
of
secondary
particle
upon
(de)lithiation.
Existing
approaches
for
alleviating
structural
degradation
could
retard
pulverization,
yet
fail
to
tune
stress
distribution
and
root
out
formation
cracks.
Herein,
we
report
a
unique
strategy
uniformize
in
via
Kirkendall
effect
stabilize
core
region
during
electrochemical
cycling.
Exotic
metal/metalloid
oxides
(such
as
Al
2
O
3
or
SiO
)
introduced
heterogeneous
nucleation
seeds
preferential
growth
precursor.
The
calcination
treatment
afterwards
generates
dopant-rich
interior
structure
with
central
void,
due
different
diffusivity
between
exotic
element
nickel
atom.
resulting
cathode
material
exhibits
superior
reversibility,
thus
contributing
high
specific
(based
on
cathode)
660
Wh
kg
−1
after
500
cycles
retention
rate
86%.
This
study
suggests
that
uniformizing
represents
promising
pathway
tackle
instability
facing
nickel-rich
cathodes.
Advanced Energy Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Июнь 29, 2024
Abstract
Cathode
materials
are
the
core
components
of
lithium‐ion
batteries
owing
to
determination
practical
voltage
and
effective
energy
battery
system.
However,
advanced
cathodes
have
faced
challenges
related
cation
migration
intermixing.
In
this
review,
study
summarizes
structural
failure
mechanisms
due
mixing
cathodes,
including
Ni‐rich
Li‐rich
layered
spinel,
olivine,
disordered
rock‐salt
materials.
This
review
starts
by
discussing
degradation
caused
intermixing
in
different
focusing
on
electronic
structure,
crystal
electrode
structure.
Furthermore,
optimization
strategies
for
inhibition
rational
utilization
systematically
encapsulated.
Last
but
not
least,
remaining
proposed
perspectives
highlighted
future
development
cathodes.
The
accurate
analysis
using
characterization,
precise
control
material
synthesis,
multi‐dimensional
synergistic
modification
will
be
key
research
areas
provides
a
comprehensive
understanding
emerge
as
pivotal
controllable
factors
further
Angewandte Chemie International Edition,
Год журнала:
2024,
Номер
63(12)
Опубликована: Янв. 31, 2024
Fast
charging
technology
for
electric
vehicles
(EVs),
offering
rapid
times
similar
to
conventional
vehicle
refueling,
holds
promise
but
faces
obstacles
owing
kinetic
issues
within
lithium-ion
batteries
(LIBs).
Specifically,
the
significance
of
cathode
materials
in
fast
has
grown
because
Ni-rich
cathodes
are
employed
enhance
energy
density
LIBs.
Herein,
mechanism
behind
loss
capability
during
extended
cycling
is
investigated
through
a
comparative
analysis
with
different
microstructures.
The
results
revealed
that
microcracks
and
resultant
deterioration
significantly
compromised
over
cycling.
When
thick
rocksalt
impurity
phases
form
throughout
particles
electrolyte
infiltration
via
microcracks,
limited
kinetics
Li
eScience,
Год журнала:
2024,
Номер
4(4), С. 100229 - 100229
Опубликована: Янв. 6, 2024
Ion
exchange
is
a
promising
synthetic
method
for
alleviating
severe
cation
mixing
in
traditional
layered
oxide
materials
lithium-ion
batteries,
leading
to
enhanced
structural
stability.
However,
the
underlying
mechanisms
of
ion
are
still
not
fully
understood.
Such
fundamental
study
ion-exchange
mechanism
needed
achieving
controllable
synthesis
oxides
with
stable
structure.
Herein,
we
thoroughly
unearth
that
triggers
Ni-rich
aqueous
solutions
by
examining
time-resolved
evolution
combined
theoretical
calculations.
Our
results
reveal
reaction
pathway
can
be
divided
into
two
steps:
protonation
and
lithiation.
The
proton
key
charge
balance
process,
as
revealed
X-ray
adsorption
spectroscopy
inductive
coupled
plasma
analysis.
In
addition,
intermediate
product
shows
high
lattice
distortion
during
exchange,
but
it
ends
up
most
energy.
apparent
discrepancies
energy
between
before
after
emphasize
importance
design
This
work
provides
new
insights
materials,
which
advances
development
cathode
high-performance
batteries.
ACS Applied Materials & Interfaces,
Год журнала:
2024,
Номер
16(9), С. 11377 - 11388
Опубликована: Фев. 22, 2024
Ni-rich
layered
oxides
LiNixCoyMn1–x–yO2
(NCMs,
x
>
0.8)
are
the
most
promising
cathode
candidates
for
Li-ion
batteries
because
of
their
superior
specific
capacity
and
cost
affordability.
Unfortunately,
NCMs
suffer
from
a
series
formidable
challenges
such
as
structural
instability
incompatibility
with
commonly
used
electrolytes,
which
seriously
hamper
practical
applications
on
large
scale.
Herein,
Al/Ta
codoping
modification
strategy
is
proposed
to
improve
performance
LiNi0.83Co0.1Mn0.07O2
cathode,
as-prepared
Al/Ta-modified
delivers
exceptional
cycling
stability
retention
97.4%
after
150
cycles
at
1C
an
excellent
rate
high
143.2
mAh
g–1
even
3C.
Based
experimental
study,
it
found
that
NCM
strengthened
due
regulated
coordination
oxygen
by
introducing
robust
Ta–O
covalent
bond,
prevents
structure
collapsing.
Moreover,
reconstructed
rock-salt-like
surface
capable
effectively
inhibiting
interfacial
side
reactions
well
overgrowth
cathode–electrolyte
interface.
Theoretically,
energy
Li/Ni
mixing
significantly
increased
introduction
Al
Ta
elements
in
codoped
NCM,
leading
inhibited
adverse
phase
transition
during
cycling.
A
feasible
pathway
designing
developing
advanced
materials
provided
this
work.