Advanced Materials,
Год журнала:
2023,
Номер
36(14)
Опубликована: Дек. 25, 2023
Lithium-metal
batteries
(LMB)
employing
cobalt-free
layered-oxide
cathodes
are
a
sustainable
path
forward
to
achieving
high
energy
densities,
but
these
exhibit
substantial
transition-metal
dissolution
during
high-voltage
cycling.
While
crossover
is
recognized
disrupt
solid-electrolyte
interphase
(SEI)
formation
on
graphite
anodes,
experimental
evidence
necessary
demonstrate
this
for
lithium-metal
anodes.
In
work,
advanced
high-resolution
3D
chemical
analysis
conducted
with
time-of-flight
secondary-ion
mass
spectrometry
(TOF-SIMS)
establish
spatial
correlations
between
the
transition
metals
and
electrolyte
decomposition
products
found
cycled
Insights
into
localization
of
various
chemistries
linked
crucial
processes
that
define
LMB
performance,
such
as
lithium
deposition,
SEI
growth,
deposition
deduced
from
precise
elemental
SEI.
Heterogenous
perpetuate
both
heterogeneous
growth
These
confirmed
across
anodes
different
electrolytes.
An
stable
higher
voltages
shown
minimize
its
effects
Overall,
results
highlight
importance
maintaining
uniform
coverage
which
disrupted
by
operation
at
voltages.
Advanced Energy Materials,
Год журнала:
2023,
Номер
13(12)
Опубликована: Фев. 9, 2023
Abstract
Li‐ion
batteries
adopting
layered
cathodes
can
effectively
alleviate
the
range
limitations
of
electric
vehicles.
Unfortunately
scarcity
Co
inhibits
massive
deployment
cathodes.
Eliminating
from
is
necessary
to
make
a
breakthrough
in
global
application
However,
Co‐free
face
challenges
delithiation/lithiation
reversibility
since
plays
pivotal
role
suppressing
Li/Ni
mixing.
Many
metals
have
been
proposed
replace
cathodes,
and
sophisticated
compositional
designs
always
consider
mixing
as
top
priority.
Here,
authors
show
that
be
suppressed
by
Al
cation
vacancies
different
manners;
however,
irreversible
capacities
are
prominently
given
similar
In‐situ
X‐ray
diffraction
monitored
potentiostatic‐intermittent‐titration
measurements
reveal
decreases
lattice
strain
between
H2
H3
phase
13.6%,
but
has
an
adverse
impact
on
structure
reversibility.
While
together
not
only
significantly
reduce
H2/H3
78%
also
greatly
enhance
Furthermore,
first‐principles
calculation
shows
remarkably
Li
migration
energy
barrier
order
magnitude.
Reversibility
newly
designed
cathode
enhanced
through
synergic
effect
vacancies.
Abstract
Great
attention
has
been
given
to
high‐performance
and
inexpensive
lithium‐ion
batteries
(LIBs)
in
response
the
ever‐increasing
demand
for
explosive
growth
of
electric
vehicles
(EVs).
High‐performance
low‐cost
Co‐free
Ni‐rich
layered
cathodes
are
considered
one
most
favorable
candidates
next‐generation
LIBs
because
current
supply
chain
EVs
relies
heavily
on
scarce
expensive
Co.
Herein,
we
review
recent
research
progress
cathodes,
emphasizing
analyzing
necessity
replacing
Co
popular
improvment
methods.
The
advancements
design
strategies
summarized
detail.
Despite
considerable
improvements
achieved
so
far,
main
technical
challenges
contributing
deterioration
such
as
detrimental
phase
transitions,
crack
formation,
severe
interfacial
side
reactions,
difficult
resolve
by
a
single
technique.
cooperation
multiple
modification
is
expected
accelerate
industrialization
corresponding
synergistic
mechanisms
urgently
need
be
studied.
More
effects
will
aroused
explore
promote
sustainable
development
LIBs.
Angewandte Chemie International Edition,
Год журнала:
2023,
Номер
62(11)
Опубликована: Янв. 19, 2023
High
voltage
can
cost-effectively
boost
energy
density
of
Ni-rich
cathodes
based
Li-ion
batteries
(LIBs),
but
compromises
their
mechanical,
electrochemical
and
thermal-driven
stability.
Herein,
a
collaborative
strategy
(i.e.,
small
single-crystal
design
hetero-atom
doping)
is
devised
to
construct
chemomechanically
reliable
Mo-doped
LiNi0.6
Co0.2
Mn0.2
O2
(SS-MN6)
operating
stably
under
high
(≥4.5
V
vs.
Li/Li+
).
The
substantially
reduced
particle
size
combined
with
Mo6+
doping
absorbs
accumulated
localized
stress
eradicate
cracks
formation,
subdues
the
surface
side
reactions
lattice
oxygen
missing
meanwhile,
improves
thermal
tolerance
at
highly
delithiated
state.
Consequently,
SS-MN6
pouch
cells
are
endowed
striking
deep
cycling
stability
wide-temperature-tolerance
capability.
contribution
here
provides
promising
way
advanced
superb
chemomechanical
for
next-generation
LIBs.
Advanced Materials,
Год журнала:
2023,
Номер
36(14)
Опубликована: Дек. 25, 2023
Lithium-metal
batteries
(LMB)
employing
cobalt-free
layered-oxide
cathodes
are
a
sustainable
path
forward
to
achieving
high
energy
densities,
but
these
exhibit
substantial
transition-metal
dissolution
during
high-voltage
cycling.
While
crossover
is
recognized
disrupt
solid-electrolyte
interphase
(SEI)
formation
on
graphite
anodes,
experimental
evidence
necessary
demonstrate
this
for
lithium-metal
anodes.
In
work,
advanced
high-resolution
3D
chemical
analysis
conducted
with
time-of-flight
secondary-ion
mass
spectrometry
(TOF-SIMS)
establish
spatial
correlations
between
the
transition
metals
and
electrolyte
decomposition
products
found
cycled
Insights
into
localization
of
various
chemistries
linked
crucial
processes
that
define
LMB
performance,
such
as
lithium
deposition,
SEI
growth,
deposition
deduced
from
precise
elemental
SEI.
Heterogenous
perpetuate
both
heterogeneous
growth
These
confirmed
across
anodes
different
electrolytes.
An
stable
higher
voltages
shown
minimize
its
effects
Overall,
results
highlight
importance
maintaining
uniform
coverage
which
disrupted
by
operation
at
voltages.