Advanced Functional Materials,
Journal Year:
2024,
Volume and Issue:
unknown
Published: Dec. 29, 2024
Abstract
Achieving
fast
ion
transport
kinetics
and
high
interfacial
stability
simultaneously
is
challenging
for
polymer
electrolytes
in
solid‐state
lithium
batteries,
as
the
coordination
environment
optimal
Li
+
conduction
struggles
to
generate
desirable
interphase
chemistry.
Herein,
adjustable
property
of
organic
ligands
exploited
metal–organic
frameworks
(MOFs)
develop
a
hierarchical
composite
electrolyte,
incorporating
heterogeneous
spatially
confined
MOF
nanofillers
into
poly‐1,3‐dioxolane
matrix.
The
defect‐engineered
University
Oslo‐66
MOFs
(UiO‐66d)
with
tailored
Lewis
acidity
can
separate
pairs
optimize
migration
through
weakened
solvation
effects,
thereby
enhancing
conductivity
by
over
sixfold
(0.85
mS
cm
−1
@25
°C).
At
anode
side,
densified
Oslo‐67
(UiO‐67)
layer
conjugated
π
electrons
facilitates
anion
participation
sheath,
promoting
reduction
forming
LiF/Li
3
N‐dominated
solid
electrolyte
isotropic
deposition.
as‐assembled
Li||LiFePO
4
full
cell
delivers
superior
cycling
92.7%
capacity
retained
2000
cycles
at
2
C.
Notably,
developed
demonstrates
excellent
compatibility
high‐voltage
cathodes,
achieving
80%
retention
LiNi
0.5
Co
0.2
Mn
0.3
O
630
cycles.
This
work
provides
valuable
insights
decoupling
challenges
paving
way
advanced
battery
technologies.
ACS Nano,
Journal Year:
2025,
Volume and Issue:
unknown
Published: Jan. 8, 2025
The
widespread
application
of
anode-free
lithium
metal
batteries
(AFLMBs)
is
hindered
by
the
severe
dendrite
growth
and
side
reactions
due
to
poor
reversibility
Li
plating/stripping.
Herein,
our
study
introduces
an
ultrathin
interphase
layer
covalent
cage
3
(CC3)
for
highly
reversible
AFLMBs.
subnano
triangular
windows
in
CC3
serve
as
a
Li+
sieve
accelerate
desolvation
transport
kinetics,
inhibit
electrolyte
decomposition,
form
LiF-
Li3N-rich
solid-electrolyte
interphases.
Moreover,
lithiophilic
backbone
homogenizes
distribution
deposition
with
mitigated
growth.
Thus,
promotes
plating/stripping
kinetics
reversibility,
achieving
ultralong
stability
over
8000
h
Cu@CC3
electrode.
Furthermore,
practical
Cu@CC3/LiFePO4
AFLMBs
deliver
capacity
retention
(66%)
600
cycles.
This
work
emphasizes
effectiveness
regulate
behavior,
demonstrating
potential
porous
organic
cages
enhancing
cycle
life
Advanced Energy Materials,
Journal Year:
2025,
Volume and Issue:
unknown
Published: April 10, 2025
Abstract
Solvents
in
liquid
and
gel
polymer
electrolytes
are
recognized
for
contributing
to
high
ionic
conductivity
high‐energy‐density
lithium
metal
batteries.
However,
parasitic
reactions
involving
solvents
induce
safety
risks
under
thermal
abuse
conditions
poor
lifespan
during
room‐temperature
cycles,
which
rarely
investigated.
This
study
introduces
a
thermoresponsive
mono‐solvent
electrolyte
as
built‐in
switch.
The
polymerizes
at
elevated
temperatures,
creating
passivate
network
without
residue
solvents.
exhibits
stability
with
91%
mass
retention
200
°C
significantly
suppresses
side
between
the
electrolyte,
reducing
runaway
risks.
Ah‐level
Li||LiNi
0.8
Co
0.1
Mn
O
2
pouch
batteries
employing
this
can
efficiently
improve
critical
temperature
of
by
75
compared
electrolyte.
At
ambient
promotes
formation
stable
solid
interphase
(SEI)
rich
LiF
Li
O,
effectively
dendrite
growth
on
anode.
Consequently,
0.5
0.2
0.3
cells
retain
capacity
after
152
even
high‐loading
cathodes
(19.7
mg
cm
−2
,
3
mAh
).
research
offers
valuable
insights
into
inhibiting
electrochemical
cycle
runaway,
enhancing
National Science Review,
Journal Year:
2024,
Volume and Issue:
12(2)
Published: Dec. 3, 2024
ABSTRACT
In-situ
fabricated
polyether
electrolytes
have
been
regarded
as
one
of
the
most
promising
solid
electrolyte
systems.
Nevertheless,
they
cannot
match
high-voltage
cathodes
over
4.3
V
due
to
their
poor
oxidative
stability.
Herein,
we
propose
an
effective
local
charge
homogenization
strategy
based
on
triglycidyl
isocyanurate
(TGIC)
crosslinker,
achieving
ultra-high-voltage
electrochemical
stability
(viz.
PTIDOL)
at
cutoff
voltages
up
4.7
V.
The
introduction
TGIC
optimizes
Li+
solvation
environment,
thereby
homogenizing
distribution
ether
oxygen
(EO)
sites,
resulting
in
significantly
enhanced
main
chain.
Consequently,
Li|PTIDOL|LiNi0.6Co0.2Mn0.2O2
(NCM622)
cell
achieves
long-term
operation
ultra-high
voltage
with
a
capacity
retention
81.8%
after
400
cycles,
best
results
reported
for
date.
This
work
provides
significant
insights
development
tolerance
and
advancement
high-energy-density
batteries.
Advanced Materials,
Journal Year:
2025,
Volume and Issue:
unknown
Published: March 23, 2025
Abstract
Solid
polymer
electrolytes
are
emerging
as
a
key
component
for
solid‐state
lithium
metal
batteries,
offering
promising
combination
of
large‐scale
processability
and
high
safety.
However,
challenges
remain,
including
limited
ion
transport
the
unstable
solid
electrolyte
interphase,
which
result
in
unsatisfactory
ionic
conductivity
uncontrollable
dendrite
growth.
To
address
these
issues,
high‐throughput
Li‐ion
pathway
is
developed
by
incorporating
tungsten
sulfide
enriched
with
sulfur
vacancies
(SVs)
into
poly(vinylidene
fluoride‐co‐hexafluoropropylene)‐based
composite
(CPEs).
The
SVs
strong
interaction
CPEs
facilitates
homogeneous
1.9
×
10
−3
S
cm
−1
at
25
°C)
enhancing
dissociation
salts
effectively
creates
ample
interfaces
chains
to
reduce
formation
inner
vacuities.
Moreover,
confine
FSI
−
anions,
while
electron‐rich
environment
induced
atoms
promotes
preferential
degradation
bis(trifluoromethanesulfonyl)imide
ensuring
uniform
deposition.
This
fosters
inorganic
nanocrystals
on
anode
suppresses
growth,
enabling
an
ultra‐long
lifetime
over
5500
h
Li||Li
symmetric
cells.
When
paired
sulfurized
polyacrylonitrile
cathode,
pouch
cell
capacity
0.524
Ah
achieved,
demonstrating
effectiveness
homogeneous,
Li‐ions
mechanism.
