Advanced Energy Materials,
Год журнала:
2022,
Номер
12(20)
Опубликована: Апрель 10, 2022
Abstract
The
safety
issue
of
lithium‐ion
batteries
is
a
crucial
factor
limiting
their
large‐scale
application.
Therefore,
it
practical
significance
to
evaluate
the
impact
overcharge
behavior
because
severe
levels
oxygen
release
cathode
materials
during
this
process.
Herein,
by
combining
variety
in
situ
techniques
spectroscopy
and
electron
microscopy,
work
studies
structural
degradation
LiNi
0.8
Co
0.1
Mn
O
2
(NCM811)
accompanying
It
observed
that
small
amount
evolves
from
initial
surface
at
≈4.7
V.
When
charging
higher
voltage
(≈5.5
V),
large
on
newly
formed
due
occurrence
microcracks.
Based
experimental
results
theoretical
calculations,
determined
mainly
occurs
near‐surface
regions,
where
remaining
vacancies
accumulate
create
voids.
To
suppress
release,
single‐crystalline
NCM811
with
integrated
structure
introduced
serves
as
cathode,
which
can
effectively
inhibit
morphology
destruction
reduce
activation
lattice
region.
These
findings
provide
basis
effective
strategy
for
improving
performance
Ni‐rich
applications.
Advanced Materials,
Год журнала:
2022,
Номер
34(19)
Опубликована: Март 11, 2022
Surface
reconstruction
of
Ni-rich
layered
oxides
(NLO)
degrades
the
cycling
stability
and
safety
high-energy-density
lithium-ion
batteries
(LIBs),
which
challenges
typical
surface-modification
approaches
to
build
a
robust
interface
with
electrochemical
activity.
Here,
strategy
leveraging
low-strain
analogues
Li-
Mn-rich
(LMR)
reconstruct
stable
surface
on
cathodes
is
proposed.
The
new
structure
not
only
consists
gradient
chemical
composition
but
also
contains
defect-rich
regarding
formation
oxygen
vacancies
cationic
ordering,
can
simultaneously
facilitate
lithium
diffusion
stabilize
crystal
during
(de)lithiation.
These
features
in
NLO
lead
dramatic
improvement
properties,
especially
cyclability
under
high
voltage
cycling,
exhibiting
30%
increase
capacity
retention
after
200
cycles
at
current
density
1
C
(3.0-4.6
V).
findings
offer
facile
effective
way
regulate
defect
chemistry
parallel
achieve
high-energy
LIBs.
Joule,
Год журнала:
2022,
Номер
6(11), С. 2535 - 2546
Опубликована: Окт. 12, 2022
Understanding
how
lithium-ion
dynamics
affect
the
(de)lithiation
mechanisms
of
state-of-the-art
nickel-rich
layered
oxide
cathodes
is
crucial
to
improve
electrochemical
performance.
Here,
we
directly
observe
two
distinct
kinetically
induced
lithium
heterogeneities
within
single-crystal
LiNixMnyCo(1−x−y)O2
(NMC)
particles
using
recently
developed
operando
optical
microscopy,
challenging
notion
that
uniform
occurs
individual
particles.
Upon
delithiation,
a
rapid
increase
in
diffusivity
at
beginning
charge
results
with
lithium-poor
peripheries
and
lithium-rich
cores.
The
slow
ion
diffusion
near-full
lithiation
states—and
transfer
kinetics—also
leads
heterogeneity
end
discharge,
surface
preventing
complete
lithiation.
Finite-element
modeling
confirms
concentration-dependent
necessary
reproduce
these
phenomena.
Our
demonstrate
kinetic
limitations
cause
significant
first-cycle
capacity
losses
Ni-rich
cathodes.
Advanced Energy Materials,
Год журнала:
2022,
Номер
12(20)
Опубликована: Апрель 10, 2022
Abstract
The
safety
issue
of
lithium‐ion
batteries
is
a
crucial
factor
limiting
their
large‐scale
application.
Therefore,
it
practical
significance
to
evaluate
the
impact
overcharge
behavior
because
severe
levels
oxygen
release
cathode
materials
during
this
process.
Herein,
by
combining
variety
in
situ
techniques
spectroscopy
and
electron
microscopy,
work
studies
structural
degradation
LiNi
0.8
Co
0.1
Mn
O
2
(NCM811)
accompanying
It
observed
that
small
amount
evolves
from
initial
surface
at
≈4.7
V.
When
charging
higher
voltage
(≈5.5
V),
large
on
newly
formed
due
occurrence
microcracks.
Based
experimental
results
theoretical
calculations,
determined
mainly
occurs
near‐surface
regions,
where
remaining
vacancies
accumulate
create
voids.
To
suppress
release,
single‐crystalline
NCM811
with
integrated
structure
introduced
serves
as
cathode,
which
can
effectively
inhibit
morphology
destruction
reduce
activation
lattice
region.
These
findings
provide
basis
effective
strategy
for
improving
performance
Ni‐rich
applications.