Advanced Functional Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Май 30, 2025
Abstract
Poly(vinylidene
fluoride)
(PVDF)‐based
solid‐state
electrolytes
face
critical
challenges
of
sluggish
ion
transport
and
interfacial
instability
in
lithium
metal
batteries,
exacerbated
by
crystalline
rigidity
residual
organic
solvents.
Herein,
a
composite
electrolyte
(M
3‐x
PVH)
integrating
oxygen‐vacancy‐rich
nanowires
into
PVDF‐HFP
matrix,
which
establishes
the
abundant
continuous
pathways
customized
ionic
microenvironments,
is
designed.
MoO
(SNWs)
with
oxygen
vacancies
not
only
promote
flexibility
polymer
chains
capture
Li⁺
to
form
for
obtaining
high
conductivity
7.58×10
−4
S
cm
−1
,
but
also
selectively
bind
dimethylformamide
customize
microenvironment
accelerating
desolvation
enhancing
stability.
Importantly,
repel
anions
via
charge
repulsion
favor
anion
decomposition,
thus
forming
an
inorganic‐rich
SEI.
Remarkably,
Li
anode
achieves
ultra‐long
cycling
(>8000
h
at
0.1
mA
−2
)
demonstrates
excellent
performance
paired
high‐voltage
cathode
NCM811.
This
work
pioneers
novel
strategy
designing
high‐performance
synergistically
engineering
material
dimensionality
defect
chemistry,
unlocking
new
possibilities
next‐generation
lithium‐metal
batteries.
New Journal of Chemistry,
Год журнала:
2025,
Номер
unknown
Опубликована: Янв. 1, 2025
A
novel
two-dimensional
silicon-containing
organic
framework
(2D
SiOF)
enhances
the
Li-ion
migration
of
PEO-based
solid-state
polymer
electrolytes
(SPE).
Li//LiFePO
4
full
cell
with
SiOF-modified
PEO
SPE
exhibits
superior
cycling
performance.
Abstract
The
development
of
solid
polymer
electrolytes
(SPEs)
has
been
significantly
impeded
by
two
primary
challenges:
low
ionic
conductivity
and
the
inhomogeneous
deposition
lithium
metal
anode.
Overcoming
these
limitations
needs
to
reduce
crystallization
design
continuous,
stable,
fast
ion
transport
pathways.
In
this
study,
incorporation
covalent
organic
framework
colloid
(COF‐C)
as
a
multifunctional
additive
SPEs
is
proposed,
aiming
regulate
construct
stable
electrolyte‐electrode
interphases.
interaction
COF‐C
with
anions
poly(ionic
liquid)
(PIL)
restricts
growth
PIL
spherical
crystals
reduces
crystallinity
electrolyte.
Acting
an
anion
receptor,
promotes
uniform
Li
+
distribution
enhances
kinetics.
Additionally,
demonstrates
coordination
create
solid‐state
electrolyte
interphases
between
SPEs.
As
result,
optimized
SPE
enables
2.70
×
10
−4
S
cm
−1
at
25
°C.
Li/PIL‐COF‐C/LiFePO
4
/
batteries
demonstrate
exceptional
cycle
stability,
evidenced
notable
discharge
specific
capacity
142.4
mAh
g
1
C,
along
commendable
retention
93.1%
following
500
cycles.
addition,
PIL‐COF‐C
can
be
adapted
higher
mass
loading
LiFePO
.
Advanced Functional Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Апрель 21, 2025
Abstract
Solid–state
sodium
metal
batteries
with
solid
polymer
electrolytes
face
significant
challenges
due
to
low
ionic
conductivity
and
limited
electrochemical
window.
This
study
presents
an
innovative
interface
regulation
strategy
expose
Lewis–acidic
hydroxyl
(–OH)
fluoride
(F
−
)
on
the
(110)
(111)
planes
of
ZnOHF
nanorods.
By
modulating
Lewis–acid
intensity
at
polymer–inorganic
interface,
Na
+
ion
transfer
number
are
increased,
while
dendrite
is
suppressed.
Density
Functional
Theory
(DFT)
calculations
indicate
that
a
engages
four
–OH
plane,
or
one
three
F
plane.
The
plane
demonstrates
lower
adsorption
energy
for
ions
(−2.93
eV)
compared
(−3.85
eV),
but
shows
stronger
capability
FSI
ions,
facilitating
efficient
transport
strengthening
interactions.
Experimentally,
PN@ZnOHF–30
electrolyte,
incorporating
ZnOHF–30
nanorods
primarily
oriented
planes,
achieves
5.74×10
−4
S
cm
−1
0.42
80
°C.
Na|PN@ZnOHF–30|Na
symmetric
cell
maintains
stable
plating/stripping
1000
h.
3
V
2
(PO
4
|PN@ZnOHF–30|Na
|PN@ZnOHF–30|NaTi
cells
show
excellent
rate
performance
cycling
stability.
Advanced Functional Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Май 7, 2025
Abstract
Lithium
metal
anodes
are
considered
as
optimal
choice
for
high‐energy
batteries;
however,
uncontrollable
dendritic
growth,
low
Coulombic
efficiency,
and
safety
concerns
limit
their
practical
applications.
Herein,
a
concept
of
pseudo
ultralow
concentration
electrolyte
featuring
high
ion
conductivity,
Li
+
transference
number,
nonflammability,
broad
electrochemical
window
is
proposed
via
incorporating
ratio
fluoroether
inert
cosolvent
into
phosphate‐based
active
solvent
high‐voltage
lithium
batteries.
Intermolecular
dipole–dipole
interactions
between
the
phosphate
trigger
competitive
solvation
effect
among
cosolvent,
phosphate,
,
which
can
effectively
regulate
structure,
thereby
weakening
‐phosphate
interaction
promoting
anionic
participation
in
sheath.
Such
enriched
‐anion
configuration
facilitates
preferred
decomposition
anions
formation
highly
conductive
mechanically
robust
solid
interphase,
induces
dense
homogeneous
deposition
achieves
plating/stripping
efficiency.
Consequently,
Li||Cu
cell
with
an
as‐designed
obtains
efficiency
99.1%.
Additionally,
Li||NCM622
exhibits
initial
specific
capacity
>170.8
mAh
g
−1
over
200
cycles
99.4%
retention.
This
work
presents
novel
strategy
designing
ultralow‐concentration
electrolytes
