Advanced Science,
Journal Year:
2025,
Volume and Issue:
unknown
Published: March 16, 2025
Abstract
Lithium
(Li)
penetration
into
solid‐state
electrolytes
(SE)
is
a
major
cause
of
lithium‐metal
battery
(LMSSB)
failure.
However,
no
single
model
fully
explains
experimental
phenomena,
and
many
simulation‐based
conclusions
lack
validation
or
contradict
results,
hindering
the
understanding
failure
mechanisms.
This
study
integrates
simulation
data
to
investigate
Li
deposition
SE
cracking,
introducing
unified
phase‐field
(PF)
model.
Unlike
existing
models,
it
accounts
for
mechanical
constraints,
solid–solid
contact,
large‐strain
mechano‐chemical
coupling.
It
also
distinguishes
from
as
short‐circuiting
cracking
do
not
occur
simultaneously.
Additionally,
crack
initiation
follows
pressurized
model,
while
propagation
occurs
through
wedge‐shaped
opening.
A
counterintuitive
approach
extending
LMSSB
lifespan
reduce
constraints
rather
than
decreasing
defect
size
increasing
hardness
toughness,
provided
that
good
contact
maintained
between
electrode
SE.
because
minimizing
alters
mode,
preventing
rapid
eruption
in
cracks.
Advanced Materials,
Journal Year:
2024,
Volume and Issue:
36(15)
Published: Jan. 13, 2024
Abstract
Solid‐state
electrolytes
(SSEs)
have
attracted
extensive
interests
due
to
the
advantages
in
developing
secondary
batteries
with
high
energy
density
and
outstanding
safety.
Possessing
ionic
conductivity
lowest
reduction
potential
among
state‐of‐the‐art
SSEs,
garnet
type
SSE
is
one
of
most
promising
candidates
achieve
performance
solid‐state
lithium
(SSLBs).
However,
elastic
modulus
electrolyte
leads
deteriorated
interfacial
contacts,
increasing
electronic
conduction
at
either
anode/garnet
interface
or
grain
boundary
results
Li
dendrite
growth.
Here,
recent
developments
solid
interfaces
for
electrolytes,
including
strategies
suppression
chemical/electrochemical/mechanical
stabilizations
are
presented.
A
new
viewpoint
double
edges
lithiophobicity
proposed,
rational
design
interphases,
as
well
effective
stacking
methods
garnet‐based
SSLBs
summarized.
Moreover,
practical
roles
SSLB
industry
also
discussed.
This
work
delivers
insights
into
which
provides
not
only
promotion
SSLBs,
but
a
comprehensive
understanding
stabilization
whole
family.
Advanced Energy Materials,
Journal Year:
2024,
Volume and Issue:
14(25)
Published: April 13, 2024
Abstract
The
pursuit
of
high‐performance
energy
storage
devices
has
fueled
significant
advancements
in
the
all‐solid‐state
lithium
batteries
(ASSLBs).
One
strategies
to
enhance
performance
ASSLBs,
especially
concerning
high‐voltage
cathodes,
is
optimizing
structure
composite
polymer
electrolytes
(CPEs).
This
study
fabricates
a
high‐oriented
framework
Li
6.4
La
3
Zr
2
Al
0.2
O
12
(o‐LLZO)
ceramic
nanofibers,
meticulously
addressing
challenges
both
metal
anode
and
LiNi
0.8
Co
0.1
Mn
(NCM811)
cathode.
as‐constructed
electrolyte
features
highly
efficient
+
transport
robust
mechanical
network,
enhancing
electron
ion
transport,
ensuring
uniform
current
density
distribution,
stress
effectively
suppressing
dendrite
growth.
Remarkably,
symmetric
cells
exhibit
outstanding
long‐term
lifespan
9800
h
at
mA
cm
−2
operate
over
800
even
1.0
under
30
°C.
CPEs
design
results
from
formation
gradient
LiF‐riched
SEI
CEI
film
Li/electrolyte/NCM811
dual
interfaces,
conduction
maintaining
electrode
integrity.
coin‐cells
pouch
demonstrate
prolonged
cycling
stability
superior
capacity
retention.
sets
notable
precedent
advancing
high‐energy
ASSLBs.
Chemical Society Reviews,
Journal Year:
2024,
Volume and Issue:
53(6), P. 3134 - 3166
Published: Jan. 1, 2024
The
utilization
of
computational
approaches
at
various
scales,
including
first-principles
calculations,
MD
simulations,
multi-physics
modeling,
and
machine
learning
techniques,
has
been
instrumental
in
expediting
the
advancement
SSEs.
SusMat,
Journal Year:
2024,
Volume and Issue:
4(1), P. 72 - 105
Published: Feb. 1, 2024
Abstract
Solid‐state
batteries
represent
the
future
of
energy
storage
technology,
offering
improved
safety
and
density.
Garnet‐type
Li
7
La
3
Zr
2
O
12
(LLZO)
solid‐state
electrolytes‐based
lithium
(SSLBs)
stand
out
for
their
appealing
material
properties
chemical
stability.
Yet,
successful
deployment
depends
on
conquering
interfacial
challenges.
This
review
article
primarily
focuses
advancement
engineering
LLZO‐based
SSLBs.
We
commence
with
a
concise
introduction
to
electrolytes
discussion
challenges
tied
in
deeply
explore
correlations
between
structure
design
principles
vital
achieving
an
ideal
electrode/electrolyte
interface.
Subsequently,
we
delve
into
latest
advancements
strategies
dedicated
overcoming
these
challenges,
designated
sections
cathode
anode
interface
design.
In
end,
share
our
insights
opportunities
realizing
full
potential
SSLBs,
ultimately
contributing
development
safe
high‐performance
solutions.
Advanced Energy Materials,
Journal Year:
2024,
Volume and Issue:
14(16)
Published: March 3, 2024
Abstract
Solid‐state
batteries
(SSBs)
have
garnered
significant
attention
as
promising
and
safe
electrochemical
solutions
for
high‐energy
storage.
Despite
their
advantageous
characteristics,
the
widespread
adoption
of
SSBs
encounters
obstacles.
Foremost
among
these
challenges
is
inadequate
solid‐state
electrolyte
(SSE)‐electrode
contact,
particularly
under
typical
operating
conditions
with
moderate
pressures.
Consequently,
substantial
external
pressures
are
conventionally
applied
to
establish
a
tightly
bonded
low‐impedance
interfacial
connection.
Unfortunately,
high
pressure
concurrently
precipitates
detrimental
effects,
such
SSE
structural
fractures
premature
short
circuits.
Moreover,
parameters
that
currently
employed
in
laboratory‐scale
research
lack
consistency
far
exceed
current
industrial
requirement
(<
1
MPa),
which
undermines
objective
evaluation
SSBs’
actual
performance
hampers
practical
utilization.
This
review
aims
construct
comprehensive
perspective
on
effect
SSBs,
specific
focus
decoupling
interfacial/bulk
electrochemo‐mechanical
dynamics.
In
particular,
adverse
consequences
fundamental
causes
highly‐pressure‐reliance
behavior
scrutinized,
followed
by
systematic
summarization
strategies
toward
low‐pressure
SSBs.
Based
insights,
it
put
forth
directions
better
disentangling
interplay
within
inspiring
development
pressure‐independent
eScience,
Journal Year:
2024,
Volume and Issue:
4(4), P. 100247 - 100247
Published: Feb. 9, 2024
Solid-state
batteries
(SSBs)
have
received
widespread
attention
with
their
high
safety
and
energy
density
characteristics.
However,
solid-solid
contacts
in
the
internal
electrode
material
material/solid
electrolyte
(SE)
interfaces,
as
well
severe
electrochemo-mechanical
effects
caused
by
stress
due
to
volume
change
of
active
material,
these
problems
hinder
ion/electron
transport
within
SSBs,
which
significantly
deteriorates
electrochemical
performance.
Applying
fabrication
pressures
stack
are
effective
measures
improve
contact
solve
problems.
Herein,
influences
different
on
cathode
anode
SEs,
electrode/SEs
interface
briefly
summarized
from
perspective
ion
diffusion,
transmission
electrons
ions
particles,
current
diffusion
kinetics,
changes
Li+
stripping/plating
based
two
physical
models,
point
out
direction
for
future
research
SSBs
advancing
industrialization
building
relationship
between
electrochemistry.
Advanced Energy Materials,
Journal Year:
2024,
Volume and Issue:
14(39)
Published: July 14, 2024
Abstract
Solid‐state
lithium
metal
batteries
(SSLMBs)
with
polymer
electrolytes
(SPEs)
have
attracted
tremendous
attention
owing
to
their
superior
safety
and
high
energy
density.
However,
the
unstable
solid
electrolyte
interphase
(SEI)
between
Lithium
(Li)
SPEs
hinders
practical
application.
Herein,
an
innovative
interfacial
catalysis
strategy
is
applied
in
situ
construction
of
a
multifunctional
inorganic‐rich
SEI.
The
transfer
unpaired
electrons
adjacent
calcium
vacancies
(V
Ca
)
TFSI
−
anion
promotes
breaking
S─N
C─F
bonds
during
electrochemical
decomposition
,
thus
enhancing
its
kinetics.
SEI
derived
from
super‐stable
kinetically
favorable
for
fast
homogeneous
transport
Li
ions,
thereby
hindering
growth
dendrites.
Consequently,
endows
Li||Li
symmetric
cells,
LFP||Li
NCM811||Li
full
enhanced
cyclability.
Thus,
this
work
expands
platform
designing
long‐life
SSLMB.
Advanced Materials,
Journal Year:
2024,
Volume and Issue:
36(19)
Published: Feb. 7, 2024
Abstract
Unleashing
the
potential
of
lithium‐metal
anodes
in
practical
applications
is
hindered
by
inherent
stress‐related
challenges
arising
from
their
limitless
volume
expansion,
leading
to
mechanical
failures
such
as
electrode
cracking,
solid
electrolyte
interphase
damage,
and
dendritic
growth.
Despite
various
protective
strategies
“combat”
stress
anodes,
they
fail
address
intrinsic
issue
fundamentally.
Here,
a
unique
strategy
proposed
that
leverages
generated
during
battery
cycling
via
piezoelectric
effect,
transforming
adaptive
built‐in
electric
field
accelerate
lithium‐ion
migration,
homogenize
lithium
deposition,
alleviate
concentration.
The
mechanism
effect
modulating
electro‐chemomechanical
evolution
further
validated
decoupled
through
finite
element
method
simulations.
Inspired
this
strategy,
high
sensitivity,
fast
responsive,
strength
adaptability
polymer
used
demonstrate
feasibility
corresponding
protected
anode
shows
stability
over
6000
h
under
current
density
10
mA
cm
−2
extending
life
variety
coin
pouch
cell
systems.
This
work
effectively
tackles
issues
decoupling
also
contributes
developing
more
stable
for
future
research.
Angewandte Chemie International Edition,
Journal Year:
2024,
Volume and Issue:
64(1)
Published: Aug. 29, 2024
Solid
polymer
electrolytes
(SPEs)
are
promising
for
high-energy-density
solid-state
Li
metal
batteries
due
to
their
decent
flexibility,
safety,
and
interfacial
stability.
However,
development
was
seriously
hindered
by
the
instability
limited
conductivity,
leading
inferior
electrochemical
performance.
Herein,
we
proposed
design
ultra-thin
electrolyte
with
long-range
cooperative
ion
transport
pathway
effectively
increase
ionic
conductivity
The
impregnation
of
PVDF-HFP
inside
pores
fluorinated
covalent
organic
framework
(CF
ACS Nano,
Journal Year:
2025,
Volume and Issue:
unknown
Published: Jan. 21, 2025
Since
the
electrochemical
potential
of
lithium
metal
was
systematically
elaborated
and
measured
in
early
19th
century,
lithium-ion
batteries
with
liquid
organic
electrolyte
have
been
a
key
energy
storage
device
successfully
commercialized
at
end
20th
century.
Although
battery
technology
has
progressed
enormously
recent
years,
it
still
suffers
from
two
core
issues,
intrinsic
safety
hazard
low
density.
Within
approaches
to
address
challenges,
development
all-solid-state
(ASSLBs)
based
on
halide
solid-state
electrolytes
(SSEs)
displayed
for
application
stationary
devices
may
eventually
become
an
essential
component
future
smart
grid.
In
this
Review,
we
categorize
summarize
current
research
status
SSEs
different
halogen
anions
perspective
chemistry,
upon
which
synthetic
routes
possessing
high
room-temperature
ionic
conductivity,
compare
detail
performance
terms
activation
energy,
electronic
interfacial
contact
stability,
window
corresponding
optimization
strategies
each
above-mentioned
indicators.
Finally,
provide
outlook
unresolved
challenges
opportunities
ASSLBs.