Advanced Functional Materials,
Journal Year:
2024,
Volume and Issue:
unknown
Published: Dec. 15, 2024
Abstract
Ni‐rich
layered
oxides
are
recognized
as
one
of
the
most
promising
candidates
for
cathodes
in
all‐solid‐state
lithium
batteries
(ASSLBs)
due
to
their
intrinsic
merits,
such
high
average
voltage
and
specific
capacity.
However,
application
is
profoundly
hindered
by
sluggish
interfacial
lithium‐ion
(Li
+
)/electron
transfer
kinetics,
which
primarily
caused
surface
residues,
structural
transformation,
Li/Ni
mixing,
H2/H3
phase
transition,
microcracks.
Furthermore,
electro‐chemo‐mechanical
failures
at
cathode/solid‐state
electrolyte
(SSE)
interface,
including
side
reactions,
space‐charge
layer
(SCL)
formation,
physical
disconnection,
accelerate
capacity
fading.
This
work
provides
a
systematic
overview
these
challenges
fundamental
insights
into
utilizing
ASSLBs.
Additionally,
several
key
parameters,
cost,
energy
density,
pressure,
environmental
temperature,
evaluated
meet
requirements
ASSLBs
commercial
applications.
Moreover,
representative
modification
strategies
future
research
directions
exploring
advanced
cathode‐based
outlined.
review
aims
provide
comprehensive
understanding
essential
expedite
Advanced Energy Materials,
Journal Year:
2025,
Volume and Issue:
unknown
Published: Jan. 16, 2025
Abstract
The
surface
reconstruction
from
the
layered
to
rocksalt‐type
phase
represents
a
primary
deterioration
pathway
of
layered‐oxide
cathodes
in
lithium‐ion
batteries,
involving
irreversible
oxygen
loss
and
transition
metal
migration.
This
degradation
mechanism
has
primarily
been
attributed
oxidative
instability
highly
delithiated
at
high
voltages
(>4.3
V
vs
Li/Li
+
).
However,
battery
also
occurs
under
seemingly
stable
voltage
ranges,
origin
which
remains
unclear.
Herein,
hidden
induce
is
proposed,
termed
“quasi‐conversion
reaction”,
revealed
occur
during
electrochemical
reduction
(discharge)
processes
just
below
3.0
(vs
Combined
experiments
first‐principles
calculations
unveil
that
oxygens
can
be
extracted
cathode
lattice
by
forming
lithium
oxides
vacancies,
significantly
higher
potentials
than
conventional
conversion
reaction,
due
coordinated
with
fewer
cations
bulk.
chemical
incompatibility
between
commercial
carbonate‐based
electrolytes
results
electrolyte
decomposition,
an
organic‐rich
blocking
layer
gaseous
byproducts,
further
increases
cell
impedance.
study
emphasizes
necessity
thorough
understanding
upon
develop
long‐lasting
batteries.
ACS Applied Energy Materials,
Journal Year:
2025,
Volume and Issue:
unknown
Published: Feb. 4, 2025
The
transition
to
sustainable
lithium-ion
batteries
is
accelerating
the
quest
for
cobalt-free
(Co-free)
cathodes,
offering
a
promising
avenue
reduce
production
costs
without
compromising
energy
density.
However,
synthesis
of
Co-free
cathodes
impeded
by
challenges,
such
as
cation
disordering,
particle
defects,
and
surface
residues,
which
significantly
degrade
battery
performance.
Although
existing
solutions
have
made
strides
in
addressing
these
issues
individually,
simple
scalable
method
address
them
comprehensively
urgently
needed.
We
introduce
an
efficient
strategy
that
leverages
kinetic
advantages
LiOH-LiNO3
eutectic
salt
mixture
enhance
lithiation
kinetics
during
calcination
LiNi0.8Mn0.2O2
thereby
overcoming
crystallization-related
hurdles.
Our
comparative
study
demonstrates
accelerates
mass
transport
at
lower
temperatures
enhances
Ni-ion
oxidation
higher
temperatures,
broadening
effective
temperature
window
topotactic
phase
transformations.
This
leads
with
reduced
disorder,
diminished
voids,
decreased
residue,
culminating
substantial
improvements
initial
Coulombic
efficiency,
cycling
stability,
rate
capability.
presents
comprehensive
solution
intrinsic
crystallization
challenges
materials,
streamlining
process
enhancing
cathode
performance,
paving
way
large-scale
industrial
production.
Nano Letters,
Journal Year:
2025,
Volume and Issue:
unknown
Published: Feb. 27, 2025
The
low
specific
capacity
and
the
poor
retention
at
extreme
fast
charging/discharging
limit
nickel-rich
layered
cathode
commercialization
in
electric
vehicles,
root
causes
are
interface
instability
loss
induced
by
birth
defects
irreversible
phase
transition.
In
this
work,
we
propose
a
lattice
reconstruction
strategy
combining
polyvinylpyrrolidone-assisted
wet
chemistry
calcination
to
prepare
aluminum-modified
LiNi0.83Co0.11Mn0.06O2
(ANCM).
Our
method
offers
distinct
advantages
tailoring
(residual
alkali
rocksalt
phase),
reducing
Li
vacancies
oxygen
vacancies,
exhibiting
gradient
Ni
concentration
distribution,
suppressing
Li/Ni
intermixing
defects,
lowering
strain
before
after
recycling,
inhibiting
microcracks.
ANCM
constructs
robust
crystal
lattices
delivers
an
initial
discharge
of
155.3
mAh/g
with
89.2%
200
cycles
5
C.
This
work
highlights
importance
synthesis
design
structural
modification
for
materials.
The
practical
application
of
nickel-rich
layered
transition
metal
oxide
is
hampered
by
its
fast
capacity
decay,
deriving
from
the
side
reactions
with
electrolyte,
crack
formation
caused
volume
variation,
and
phase
change
near
surface
during
charging/discharging
processes.
Here,
we
experimentally
realize
mechano-chemo-electrochemical
coupling
effect
nanolayer
on
to
greatly
improve
electrochemical
performance.
According
detailed
atomic
structure
analysis,
this
facilitates
consuming
residual
lithium
left
oxide,
suppressing
reducing
due
variation
long-term
cycles.
This
design
plays
an
in
mechanical,
chemical,
aspects
simultaneously
which
beneficial
for
their
development.
Energy Materials,
Journal Year:
2025,
Volume and Issue:
5(8)
Published: May 9, 2025
To
address
the
detrimental
impact
of
residual
LiOH
on
electrochemical
performance
LiNi0.80Co0.15Al0.05O2
(NCA)
cathode
material,
it
is
imperative
to
optimize
its
surface
structure.
Adding
a
Li-reactant
react
with
not
only
removes
but
also
forms
new
structure
layers.
However,
this
reaction
process
necessitates
evaluating
compatibility
between
newly
formed
layer
and
crystal
NCA
material
requires
careful
determination
optimal
amount
Li-reactant.
Currently,
there
remains
lack
well-established
theoretical
guidance
for
determining
addition
lithium
reactants.
In
study,
quantitative
6,000
ppm
Al2O3
as
3,156
effectively
reduces
facilitates
formation
LiAlO2@NCA
heterostructure
materials.
This
approach
provides
foundation
Li-reactant,
overcomes
limitations
empirical
trial-and-error
methods,
achieves
reconstruction
materials
Based
an
in-depth
analysis
structure,
first-principles
calculations
tests,
serves
efficient
Li+
diffusion
channel
migration
energy
barrier,
stable
protection
thereby
enhancing
stability
reversibility.
Journal of the American Chemical Society,
Journal Year:
2024,
Volume and Issue:
unknown
Published: Dec. 7, 2024
The
thermal
safety
issues
of
currently
available
Ni-rich
cathode-based
power
supplies
brought
in
the
development
all-solid-state
batteries,
yet
cascade
reactions
materials
and
chemo-mechanical
degradation
between
cathode
solid
electrolyte
diminished
cycle
life.
Here,
by
introducing
a
new
heteroatom
chemical
competing
diffusion
strategy,
we
successfully
stabilize
contact
face
with
an
electrolyte.
Combining
extensive
explorations
theoretical
calculation
multiscale
in/ex
situ
characterization,
elucidate
atomic-level
upon
topological
lithiation
layered
materials.
heteroatoms
higher
binding
energy
to
coordinated
oxygen
served
as
"oxygen
anchor"
bulk
alleviated
excessive
oxidation
through
charge
compensation,
thus
easing
aggression
evolved
oxygen.
Comparably,
others
were
enriched
surface
formed
ionic
"diffusion
regulator"
residual
lithium,
special
transfer
regulation
mechanism
piezoelectric
layer
validly
improved
interface
compatibility
weakened
space-charge
solid-state
batteries.
This
helped
designed
sulfide
battery
exhibit
excellent
cyclability
under
4.5
V
(97.3%
after
120
cycles).
Our
findings
unlocked
structure–function
relationship
polarization
field
generated
material
electrode.
