Advanced Functional Materials,
Journal Year:
2025,
Volume and Issue:
unknown
Published: May 9, 2025
Abstract
Both
phosphate‐based
high‐concentration
electrolytes
and
localized
effectively
address
safety
concerns
interfacial
compatibility
issues
in
Ni‐rich
lithium
metal
batteries
(LMBs).
However,
their
high
cost
viscosity
have
hindered
further
practical
applications.
Here,
an
intrinsically
nonflammable
low‐concentration
electrolyte
is
delicately
presented,
employing
0.7
M
difluoro(oxalato)borate
the
flame‐retardant
trimethyl
phosphate
solvent,
to
overcome
aforementioned
challenges.
The
weak
interactions
between
anions
facilitate
formation
of
anions‐induced
solvation
structures
protective
layers
that
are
rich
boron
oxides
LiF.
as‐designed
has
been
employed
build
LiNi
0.9
Co
0.05
Mn
O
2
/Li
cell
which
demonstrates
stable
cycling
for
over
180
cycles.
Additionally,
battery
also
able
operate
successfully
a
wide
temperature
range,
from
‐20
60
°C,
displays
elevated
thermal
runaway
temperatures,
enhanced
high‐temperature
charge
retention
capability,
reduced
gas
evolution.
Moreover,
20.0
Ah
pouch
achieves
energy
density
533.8
Wh
kg
−1
,
showcasing
great
potential
commercial
Furthermore,
this
compatible
with
both
layered
spinel
cathodes.
delicate
molecular
design
strategy
work
provides
promising
avenue
development
high‐safety
high‐energy‐density
LMBs.
Advanced Functional Materials,
Journal Year:
2025,
Volume and Issue:
unknown
Published: May 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
Advanced Functional Materials,
Journal Year:
2025,
Volume and Issue:
unknown
Published: May 9, 2025
Abstract
Both
phosphate‐based
high‐concentration
electrolytes
and
localized
effectively
address
safety
concerns
interfacial
compatibility
issues
in
Ni‐rich
lithium
metal
batteries
(LMBs).
However,
their
high
cost
viscosity
have
hindered
further
practical
applications.
Here,
an
intrinsically
nonflammable
low‐concentration
electrolyte
is
delicately
presented,
employing
0.7
M
difluoro(oxalato)borate
the
flame‐retardant
trimethyl
phosphate
solvent,
to
overcome
aforementioned
challenges.
The
weak
interactions
between
anions
facilitate
formation
of
anions‐induced
solvation
structures
protective
layers
that
are
rich
boron
oxides
LiF.
as‐designed
has
been
employed
build
LiNi
0.9
Co
0.05
Mn
O
2
/Li
cell
which
demonstrates
stable
cycling
for
over
180
cycles.
Additionally,
battery
also
able
operate
successfully
a
wide
temperature
range,
from
‐20
60
°C,
displays
elevated
thermal
runaway
temperatures,
enhanced
high‐temperature
charge
retention
capability,
reduced
gas
evolution.
Moreover,
20.0
Ah
pouch
achieves
energy
density
533.8
Wh
kg
−1
,
showcasing
great
potential
commercial
Furthermore,
this
compatible
with
both
layered
spinel
cathodes.
delicate
molecular
design
strategy
work
provides
promising
avenue
development
high‐safety
high‐energy‐density
LMBs.