Advanced Materials,
Journal Year:
2025,
Volume and Issue:
unknown
Published: March 27, 2025
Pursuing
high
energy/power
density
lithium
metal
batteries
(LMBs)
with
good
safety
and
lifespan
is
essential
for
developing
next-generation
energy-storage
devices.
Nevertheless,
the
uncontrollable
degradation
of
electrolyte
subsequent
formation
inferior
electrolyte/electrode
interfaces
present
formidable
challenges
to
this
endeavor,
especially
when
paring
transition
oxide
cathode.
Herein,
a
fireproof
polymeric
matrix
local
conjugated
structure
constructed
by
4,4'-methylenebis
(N,
N-diglycidylaniline)
(NDA)
monomer
via
in
situ
polymerization,
which
promotes
use
ester-based
liquid
highly
stable
LMBs.
The
tertiary
anilines
PNDA
effectively
tune
Li+
solvation
sheath
generate
conformal
protective
layers
on
electrode
surfaces,
resulting
excellent
compatibility
both
high-voltage
cathodes
Li-metal
anodes.
Moreover,
accumulated
electron
endows
powerful
capability
seize
eliminate
corrosive
hydrofluoric
acid,
strikingly
mitigates
irreversible
transformation
LiNi0.8Mn0.1Co0.1O2
(NMC)
particles.
As
result,
PNDA-based
Li||LiFePO4
Li||NMC
cells
reach
electrochemical
performance.
This
study
provides
promising
strategy
macromolecular
design
electrolytes
emphasizes
importance
"local
conjugation"
within
polymers
Advanced Materials,
Journal Year:
2025,
Volume and Issue:
unknown
Published: March 30, 2025
Abstract
Quasi‐solid‐state
polymer
electrolytes
(QSPEs)
have
been
considered
as
one
of
the
most
promising
for
high‐safety
high‐energy‐density
lithium
metal
batteries
(LMBs).
However,
their
inadequate
mechanical
properties
and
instability
under
high
voltages
pose
significant
challenges
practical
applications.
Herein,
robust
antioxidative
QSPEs
are
developed
based
on
a
polymer‐brush‐based
rigid
supporting
film
(BC‐
g
‐PLiMTFSI‐
b
‐PPFEMA,
BC:
bacterial
cellulose,
PLiMTFSI:
poly(lithium
(3‐methacryloyloxypropylsulfonyl)
(trifluoromethylsulfonyl)imide),
PPFEMA:
poly(2‐(perfluorohexyl)ethyl
methacrylate)).
The
BC
nanofibril
backbone
can
produce
highly
porous
structure
with
outstanding
strength.
More
importantly,
PLiMTFSI‐
‐PPFEMA
side‐chains
not
only
obviously
increase
conversion
ratio
easily
oxidized
monomers
in
QSPEs,
but
also
possess
strong
interaction
unstable
electrolyte
components.
With
such
solid‐state
electrolytes,
Li/LiNi
0.8
Mn
0.1
Co
O
2
full
cell
cathode
loading
(20.3
mg
cm
−2
)
exhibits
specific
discharge
capacity
200.7
mAh
−1
at
0.5
C
demonstrates
long
lifespan
137
cycles
retained
170.7
cut‐off
voltage
4.5
V.
4.6
V,
147.0
after
187
be
Li/LiCoO
cells.
This
work
provides
feasible
development
strategy
long‐cycling
high‐voltage
LMBs.
Advanced Materials,
Journal Year:
2025,
Volume and Issue:
unknown
Published: April 7, 2025
Abstract
The
advancement
of
lithium
metal
batteries
toward
their
theoretical
energy
density
potential
remains
constrained
by
safety
and
performance
issues
inherent
to
liquid
electrolytes.
Quasi‐solid‐state
electrolytes
(QSSEs)
based
on
poly‐1,3‐dioxolane
(poly‐DOL)
represent
a
promising
development,
yet
challenges
in
achieving
satisfactory
Coulombic
efficiency
long‐term
stability
have
impeded
practical
implementation.
While
nitrate
addition
can
enhance
efficiency,
its
incorporation
results
prohibitively
slow
polymerization
rates
spanning
several
months.
In
this
work,
high‐polymerization‐enthalpy
1,1,1‐trifluoro‐2,3‐epoxypropane
is
introduced
as
co‐polymerization
promoter,
successfully
integrating
into
poly‐DOL‐based
QSSEs.
resulting
electrolyte
demonstrates
exceptional
with
2.23
mS
cm
−1
ionic
conductivity
at
25
°C,
99.34%
Li|Cu
cells,
stable
interfaces
sustained
through
1300
h
symmetric
cell
cycling.
This
approach
also
suppresses
poly‐DOL
crystallization,
enabling
Li|LiFePO
4
cells
maintain
beyond
2000
cycles
1C.
Scale‐up
validation
≈1
Ah
Li|NCM811
pouch
achieves
94.4%
capacity
retention
over
60
cycles.
strategy
establishes
new
pathway
for
developing
high‐performance,
situ
polymerized
quasi‐solid‐state
storage
applications.
Advanced Energy Materials,
Journal Year:
2025,
Volume and Issue:
unknown
Published: April 25, 2025
Abstract
Highly
flammable
carbonate
electrolytes
induce
significant
safety
risk
for
lithium‐ion
batteries
(LIBs),
raising
concerns
about
their
suitability
large‐scale
applications.
In
contrast,
non‐flammable
phosphate
offer
a
potential
solution,
yet
the
untamed
strong
interaction
of
Li
+
‐phosphates
and
inefficient
diffusion
result
in
sluggish
reaction
kinetics,
which
restricts
operation
Ah‐level
LIBs
to
rates
below
0.2C.
Herein,
chelating
solvent‐mediated
ion‐solvent
coordinated
structure
is
designed
modulate
interaction.
This
innovative
approach
enables
high‐efficiency
pseduo‐structrural
diffusion,
similar
that
observed
high
concentration
electrolytes,
while
maintaining
standard
1
mol
L
−1
achieving
Li⁺
conductivity.
The
operating
rate
graphite|LiFePO
4
cells
increased
from
0.2C
2C,
with
Ah
25
retaining
73.9%
71.0%
capacity
after
1000
600
cycles,
respectively.
Additionally,
maximum
temperature
during
nail
penetration
significantly
reduced
338.9
200
°C.
strategy
provides
promising
tuition
developing
advanced
electrolytes.
Advanced Materials,
Journal Year:
2025,
Volume and Issue:
unknown
Published: April 25, 2025
Abstract
The
practical
application
of
quasi‐solid‐state
ether‐based
electrolytes
is
hindered
by
lithium
dendrite
formation
and
poor
oxidation
stability,
which
reduce
the
cycle
life
energy
density
battery.
Here,
taking
advantage
ionic
liquids’
high
interactions
structural
flexibility
in
forming
an
optimized
electrode/electrolyte
interface,
a
pyrrolidinium‐based
liquids
with
trifluorotoluylation
cationic
segment
designed
developed.
anions
induced
to
form
robust
inorganic
LiF‐rich
interphase
at
cathode,
thereby
effectively
achieving
stability
suppressing
dissolution
transition
metal
ions.
In
addition,
LiF
interphases
derived
from
cations
increase
modulus
anode
interface
suppress
growth
dendrites.
Therefore,
Li‐LiFePO
4
,
Li‐LiCoO
2
Li‐LiNi
0.8
Co
0.1
Mn
O
full
cells
demonstrate
remarkable
performance
improvements
current
(10
C),
wide
voltage
range
4.5
V,
mass
loading
11.1
mg
cm
−2
temperature
−20–80
°C.
Furthermore,
2.66
Ah‐level
pouch
cell
high‐energy‐density
exceeding
356
Wh
kg
‒1
excellent
cyclic
demonstrates
potential
strategy
providing
path
for
batteries.
Advanced Materials,
Journal Year:
2025,
Volume and Issue:
unknown
Published: April 29, 2025
Abstract
Anode‐free
lithium
metal
battery
(AFLMB)
has
become
an
excellent
candidate
for
long
endurance
electric
vehicles
and
low
altitude
aircraft,
profiting
from
its
high
energy
density
as
well
outstanding
manufacturing
safety.
However,
the
limitation
at
discharge
rates
of
AFLMBs
is
shrouded
in
mystery,
yet
to
achieve
more
attention.
Herein,
fast
dissected
exhaustively,
a
symptomatic
strategy
break
limit
put
forward,
order
eliminate
inevitable
mismatch
that
lies
inferior
performance
AFLMBs.
A
“volcano‐type”
curve
capacity
retention
discovered
with
rate
increased.
Systematic
investigation
revealed
overlapped
spatial
relationship
between
fresh
deposited
Li
residue
0
facilitated
utilization
“recoverable
”
(Li
)
prophase
increase.
further
enhanced
induced
large
concentration
polarization
(
η
conc
),
reflecting
limited
+
diffusion.
Enabling
electrolyte
rapidly
transport
by
lowering
increased
optimal
cycling
stability
This
work
reveals
rate‐determining
step
high‐rate
expands
employment
boundary
under
harsh
conditions,
providing
significant
complement
present
knowledge
respect
power
