Small,
Journal Year:
2025,
Volume and Issue:
unknown
Published: May 2, 2025
Abstract
The
low
energy
density
and
safety
problems
of
lithium‐ion
batteries
based
on
liquid
electrolyte
have
set
off
a
new
wave
high
specific
capacity
battery
design
to
meet
the
need
future
market.
Solid‐state
lithium
metal
has
been
widely
concerned
for
its
density,
safety,
electrochemical
stability.
Especially,
polymer‐based
solid‐state
electrolytes
(polymer
SSEs)
attracted
much
attention
due
good
interfacial
contact,
flexible
mechanical
properties,
physical/chemical
However,
deficiencies
ionic
conductivity
weak
strength
limit
further
development
polymer
SSEs.
Here,
hybrid
ceramic–polymer
composite
(CSSEs),
specifically
consisted
polymers
inorganic
ceramic
active
fillers,
can
achieve
conductivity,
excellent
Li
dendrite
growth
inhibition.
Based
intrinsic
characteristics
polymers,
this
review
expounds
strategies
improve
performance
CSSEs.
screening
modification
fillers
in
recent
years,
including
structural
design,
surface
modification,
interface
engineering,
are
reviewed.
Finally,
core
ideas
existing
designs,
proposed
feasible
solutions,
aiming
at
providing
industrialization
CSSEs
summarized.
Journal of the American Chemical Society,
Journal Year:
2025,
Volume and Issue:
unknown
Published: Jan. 23, 2025
In
situ
polymerization
strategies
hold
great
promise
for
enhancing
the
physical
interfacial
stability
in
solid-state
batteries,
yet
(electro)chemical
degradation
of
polymerized
interfaces,
especially
at
high
voltages,
remains
a
critical
challenge.
Herein,
we
find
interphase
engineering
is
crucial
process
and
polymer
pioneer
an
polymerization-fluorination
(Poly-FR)
strategy
to
create
durable
interfaces
with
excellent
stabilities,
achieved
by
designing
bifunctional
initiator
both
on-surface
lithium
donor
reactions.
The
integrated
fluorination
converts
Li2CO3
impurities
on
LiNi0.8Co0.1Mn0.1O2
(NCM811)
surfaces
into
LiF-rich
interphases,
effectively
inhibiting
aggressive
(de)lithiation
intermediates
protecting
interface
from
underlying
chemical
degradation,
thereby
surpassing
limitations
alone.
Furthermore,
Poly-FR
mediated
symmetric
Li|Li
cells
achieve
impressive
cycling
up
12,000
h.
Solid-state
NCM811
cathodes
Li
metal
anodes
realize
ultrastable
performance
400
cycles
83.4%
retention
voltage
4.5
V.
This
work
points
toward
advanced
beyond.
Chemical Reviews,
Journal Year:
2025,
Volume and Issue:
unknown
Published: Feb. 4, 2025
Solid-state
batteries
(SSBs)
could
offer
improved
energy
density
and
safety,
but
the
evolution
degradation
of
electrode
materials
interfaces
within
SSBs
are
distinct
from
conventional
with
liquid
electrolytes
represent
a
barrier
to
performance
improvement.
Over
past
decade,
variety
imaging,
scattering,
spectroscopic
characterization
methods
has
been
developed
or
used
for
characterizing
unique
aspects
in
SSBs.
These
efforts
have
yielded
new
understanding
behavior
lithium
metal
anodes,
alloy
composite
cathodes,
these
various
solid-state
(SSEs).
This
review
provides
comprehensive
overview
strategies
applied
SSBs,
it
presents
mechanistic
SSB
that
derived
methods.
knowledge
critical
advancing
technology
will
continue
guide
engineering
toward
practical
performance.
Small,
Journal Year:
2025,
Volume and Issue:
unknown
Published: Feb. 5, 2025
Composite
solid
electrolytes
(CSEs)
based
on
poly(vinylidene
fluoride)-co-hexafluoropropylene
(PVDF-HFP)
and
Li6.4La3Zr1.4Ta0.6O12
(LLZTO)
show
great
potential
in
building
high
energy
density
all-solid-state
lithium
metal
batteries
(ASSBs).
Nevertheless,
the
Li2CO3
passivation
layer
formed
LLZTO
surface
not
only
induces
dehydrofluorination
of
PVDF-HFP
but
also
blocks
Li+
transport
at
interfaces
PVDF-HFP/LLZTO
CSE/electrodes.
Herein,
acetate-assisted
surficial
indiumization
with
a
thickness
4
nm
is
carried
out
to
convert
detrimental
into
stable
conductor
LiInO2
(LIO)
LLZTO.
With
this
modification,
air
stability
CSEs
achieved
which
prevents
regeneration
effectively.
Attributed
unblocked
paths
LLZTO@LIO/PVDF-HFP
(LIO-CSE)
interface,
ionic
conductivity
3.1
×
10-4
S
cm-1
transference
number
0.673
are
attained.
The
Li2CO3-free
contributes
constructing
robust
electrolyte
interphase
predominantly
inorganic
components,
successfully
decreases
side
reactions
ultimately
realizes
good
compatibility
LLZTO/polymer
electrolyte/electrode
interfaces.
assembled
Li|LIO-CSE|Li
cells
exhibit
excellent
electrochemical
for
3100
h
0.5
mA
cm-2.
Li/LIO-CSE/LiFePO4
ASSB
delivers
high-capacity
retention
81.8%
after
1000
cycles
25
°C.
This
work
provides
promising
method
toward
remarkable
interfacial
ASSBs.
Energy & Fuels,
Journal Year:
2024,
Volume and Issue:
38(22), P. 21674 - 21700
Published: Nov. 5, 2024
Solid-state
lithium
batteries
(SSLBs)
utilize
solid
electrolytes
(SEs)
instead
of
their
liquid
counterpart,
providing
higher
energy
density
and
safety,
are
considered
as
potential
storage
technology.
Among
the
various
kinds
SEs,
garnet
(Li7La3Zr2O12,
LLZO)
electrolyte
has
considerable
Li-ion
conductivity
robust
air/chemical
stability,
rendering
it
an
excellent
candidate
for
commercialization
SSLBs.
In
recent
years,
numerous
efforts
have
been
made
to
improve
ionic
SEs.
These
successfully
achieved
a
high
∼10–3
S
cm–1
at
room
temperature.
Nevertheless,
emerging
issue
pertains
interfacial
stability
garnet-based
electrolytes.
Therefore,
our
focus
lies
on
challenges
associated
with
SSLBs,
including
(i)
interface
between
metal
anode
SE,
(ii)
SE
high-voltage
cathodes,
(iii)
polymeric
additives
SE.
The
solution
strategies
these
target-oriented
issues
briefly
discussed.
light
discourse
enhanced
performance,
principle
designing
high-performance
interfaces
is
proposed.
A
future
perspective
also
offered
development
Advanced Functional Materials,
Journal Year:
2024,
Volume and Issue:
unknown
Published: July 18, 2024
Abstract
In
situ
formation
of
gel
polymer
electrolytes
(GPE)
has
been
a
promising
candidate
to
address
individual
limitations
liquid/solid
and
interfacial
stability.
However,
the
controllable
conversion
liquid
electrolyte
(LE)
precursor
GPE
remains
great
challenge
with
lower
lithium‐ion
transport,
which
is
far
from
demand
for
fast‐charging
properties.
Herein,
strategy
gradient
polymerization
forming
pioneered,
stabilizing
electrolyte/electrode
interface
an
accelerated
Li
+
migration
feature.
As
demonstrated
by
theoretical
simulations
visualization
experiment
results,
mechanism
via
partial
inhibitory
Lithium
nitrate
(LiNO
3
)
control
solvent
comprehensively
investigated,
exhibiting
preferential
interaction
between
anion
(NO
−
Lewis
acidic
site
in
lithium
bis(fluorosulfonyl)imide
(LiFSI).
Consequently,
stable
amorphous
high
conductivity
(5.10
mS
cm
−1
inorganic
solid
interphase
(SEI)‐dominate
layer
derived
spectroscopical
measurements
are
achieved
on
graphite
electrode
surface.
The
as‐prepared
iron
phosphate
(LFP)||graphite
pouch
cell
stabilizes
capacity
109.80
mAh
g
(capacity
retention:
80.02%)
after
715
cycles
at
5
C/1
C
(charge/discharge),
corresponding
energy
density
277.64
Wh
kg
.
This
work
provides
facile
but
practical
approach
designing
highly
batteries.
Advanced Functional Materials,
Journal Year:
2024,
Volume and Issue:
35(1)
Published: Oct. 31, 2024
Abstract
The
use
of
all‐solid‐state
lithium
metal
batteries
(ASSLMBs)
has
garnered
significant
attention
as
a
promising
solution
for
advanced
energy
storage
systems.
By
employing
non‐flammable
solid
electrolytes
in
ASSLMBs,
their
safety
profile
is
enhanced,
and
the
anode
allows
higher
density
compared
to
traditional
lithium‐ion
batteries.
To
fully
realize
potential
solid‐state
(SSEs)
must
meet
several
requirements.
These
include
high
ionic
conductivity
Li
+
transference
number,
smooth
interfacial
contact
between
SSEs
electrodes,
low
manufacturing
cost,
excellent
electrochemical
stability,
effective
suppression
dendrite
formation.
This
paper
delves
into
essential
requirements
enable
successful
implementation
ASSLMBs.
Additionally,
representative
state‐of‐the‐art
examples
developed
past
5
years,
showcasing
latest
advancements
SSE
materials
highlighting
unique
properties
are
discussed.
Finally,
provides
an
outlook
on
achieving
balanced
improved
addressing
failure
mechanisms
solutions,
critical
challenges
such
reversibility
plating/stripping
thermal
runaway,
characterization
techniques,
composite
SSEs,
computational
studies,
ASS
lithium–sulfur
lithium–oxygen
With
this
consideration,
ASSLMBs
can
be
realized.
