Electrolytes
based
on
carbonic
acid
esters
and
organic
ethers
are
used
in
commercially
available
lithium-ion
batteries.
High-energy-density
anodes
high-voltage
cathodes
crucial
components
for
enhancing
the
energy
density
of
batteries
while
also
imposing
higher
requirements
electrolyte
system.
Solid-state
(SSBs)
utilizing
solid-state
electrolytes
show
excellent
features
both
high
safety.
A
solid
is
a
type
ionic
conductor.
Ion
migration
an
driven
by
chemical
gradient
electrochemical
Ionic
conductivity
parameter
evaluating
ion
transport
ability
systems,
it
plays
pivotal
role
determining
performance
SSBs.
Solid
generally
classified
into
inorganic
polymer
electrolytes.
With
speedy
growth
sectors
like
electric
vehicles
storage,
materials
associated
with
SSBs
ripe
extensive
development
opportunities.
Energy & Fuels,
Год журнала:
2024,
Номер
38(22), С. 21674 - 21700
Опубликована: Ноя. 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
Materials,
Год журнала:
2025,
Номер
18(7), С. 1536 - 1536
Опубликована: Март 28, 2025
In
this
study,
we
investigated
the
structural
effect
of
composite
solid
electrolytes
Al-doped
LLZO
and
PVDF-HFP
(0D_Al-LLZO@PVDF-HFP
1D_Al-LLZO@PVDF-HFP)
on
electrochemical
(EC)
performance
fire
safety
through
a
systematic
evaluation
comparative
tests.
The
unique
structure
advantageous
features
(1D_Al-LLZO@PVDF-HFP)
were
highlighted
by
comparing
controls
(PVDF-HFP
0D_Al-LLZO@PVDF-HFP)
with
physicochemical
analyses
tests
morphology
LLZO/PVDF-HFP
composites
analyzed
X-ray
diffraction
(XRD)
scanning
electron
microscopy
(SEM),
while
their
chemical
functionalities
free
ion
clusters
examined
Fourier
transform
infrared
(FT-IR)
spectroscopy
Raman
spectroscopy,
respectively.
1D_Al-LLZO@PVDF-HFP
1D
structured
Al-LLZO
filler
network
in
matrix
could
effectively
regulate
crystallinity
facilitated
lithium
salt
dissociation,
resulting
high
lithium-ion
transference
number
ionic
conductivity.
As
result,
electrolyte
an
optimized
low
content
(~5.1
wt%)
exhibited
enhanced
conductivity
(σ:
1.40
×
10−4
S/cm)
interfacial
resistance,
broadened
EC
stability
(voltage
window:
4.75
V
vs.
Li/Li+),
(0.75)
superior
to
that
0D_Al-LLZO@PVDF-HFP.
characterizations,
1D_Al-LLZO@PVDF-HFP-based
cell
demonstrated
symmetric
(>2000
h)
full
(LiFePO4|electrolyte|Li)
reversible
capacity
102.7
mAh/g
at
2C
retention
85.7%
over
200
cycles,
better
than
0D_
Al-LLZO@PVDF-HFP-based
cell.
flammability
tests,
Al-LLZO@PVDF-HFP
(nonflammability)
compared
PVDF-HFP-based
regardless
structure,
suggesting
importance
inorganic
rather
composite.
Advanced Science,
Год журнала:
2025,
Номер
unknown
Опубликована: Апрель 17, 2025
Abstract
Polymeric
solid‐state
electrolytes
(SSEs)
with
environmentally
friendly
processes
deliver
safer
and
cleaner
energy
storage
devices
without
fires
leakages
than
conventional
liquid
electrolytes.
Here,
water‐processable
halogen‐free
polymeric
SSEs
are
demonstrated
high
ion
conductivity
(≈6
mS
cm
−1
),
prepared
from
aqueous
solutions
consisting
of
branched
poly(ethylene
imine)
(bPEI),
lithium
hydroxide
(LiOH),
poly(4‐styrene
sulfonic
acid)
(PSSA).
The
bPEI:LiOH:PSSA
(PLP)
various
PSSA
molar
ratios
applied
to
asymmetric
supercapacitors
graphite‐based
anodes
indium
tin
oxide
(ITO)
counter
electrodes.
ratio
strongly
affected
the
PLP
SSEs,
leading
a
maximum
at
=
40
mol%,
owing
role
in
controlling
size
LiOH
domains
for
better
Li
+
transport
pathways.
enhanced
enabled
PLP‐supercapacitors
build
potential
2.24
V
compared
1.64
0
upon
galvanostatic
charge/discharge
current
density
0.2
mA
g
.
endurance
test
shows
that
(PSSA
mol%)
can
function
stably
capacitance
retention
(96.2%)
more
5000
cycles,
≈80%
80
°C,
supporting
their
practical
use
high‐safety
batteries.
Garnet
Li6.5La3Zr1.5Ta0.5O12
(LLZTO)
has
emerged
as
a
promising
candidate
for
solid-state
lithium-metal
batteries
(SSLMBs).
However,
the
air
susceptibility
with
Li2CO3
impurity
and
severe
electron
leakage
lead
to
inferior
cycling
performance,
remaining
critical
challenge.
Herein,
contradictory
interface
chemistry
been
proposed
in
which
normally
undesired
is
deliberately
retained
delicately
adopted,
can
effectively
enhance
interfacial
stability
of
Li|LLZTO.
The
growth
behavior
on
LLZTO
systematically
investigated,
while
its
formation
residual
controllable,
serves
an
insulating
layer
blocks
leakage.
Moreover,
porous
lithiophilic
Li3PW12O40
(POMs)
ensures
enhanced
contact
provides
three-dimensional
Li+-channels
accelerate
Li+
migration.
This
structure
efficiently
inhibit
Li-dendrite
penetration
at
grain
boundaries.
Therefore,
Li|POMs-LLZTO|NCM
full-cell
achieve
97.7%
capacity
retention
after
100
cycles.
facile
strategy
innovatively
repurposes
into
functional
interlayer,
offering
prospects
develop
large-scale
garnet-based
SSLMBs.
