Advanced Functional Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Май 19, 2025
Abstract
Electrolytes
engineering
plays
a
crucial
role
in
determining
electrode/electrolyte
interfacial
chemistry
for
developing
high‐voltage
lithium
metal
batteries
(HV‐LMBs).
Although
great
progress
has
been
made
on
electrolytes
anodes,
the
realization
of
HV‐LMBs
severely
hindered
due
to
lack
advanced
that
can
simultaneously
support
stable
Li
anode
and
cathode
(>
4.6
V
vs
+
/Li).
Herein,
through
molecular
via
strategic
monofluorination
design,
two
terminal
monofluorinated
siloxanes
including
(2‐fluoroethoxy)trimethylsilane
(MFS)
bis(2‐fluoroethoxy)dimethylsilane
(F2DEO)
are
designed
synthesized.
Compared
with
nonfluorinated
counterparts,
siloxane‐based
not
only
exhibit
higher
dielectric
constant
oxidative
stability
but
also
allow
weaker
solvation
ability
better
compatibility.
With
“4S”
(single
salt
single
solvent)
at
standard
concentration,
1.0
M
LiFSI/F2DEO
electrolyte
endows
operation
590
h
Li||Li
symmetric
cells
high
coulombic
efficiency
99.3%
Li||Cu
half
cells.
Moreover,
Li||LiCoO
2
full
achieve
high‐capacity
retention
85.9%
after
200
cycles,
which
may
be
attributed
F2DEO
synergistic
effect
FSI
−
regulating
interphase.
This
design
strategy
provides
promising
approach
future
exploration
HV‐LMBs.
Advanced Energy Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Июль 14, 2024
Abstract
Lithium‐ion
batteries
(LIBs)
have
emerged
as
vital
elements
of
energy
storage
systems
permeating
every
facet
modern
living,
particularly
in
portable
electronic
devices
and
electric
vehicles.
However,
with
the
sustained
economic
social
development,
new‐generation
LIBs
high
density,
wide
operating
temperature
range,
fast
charge,
safety
are
eagerly
expected,
while
conventional
ethylene
carbonate
(EC)‐based
electrolytes
fail
to
satisfy
corresponding
requirements.
Comparatively,
ether‐based
electrolyte
fascinating
properties
recently
been
revived
fields,
many
advanced
exciting
performances
under
developed.
This
review
provides
an
extensive
overview
latest
breakthroughs
concerning
applied
intercalation
cathodes.
To
systematically
outline
progression
electrolytes,
this
is
categorized
from
perspective
anodes
follows:
i)
graphite
anode‐based
LIBs;
ii)
silicon
iii)
lithium
metal
LIBs.
Advanced Functional Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Сен. 13, 2024
Abstract
Solid‐state
lithium
metal
batteries
(SSLMBs)
with
poly
(ethylene
oxide)
(PEO)‐based
electrolytes
have
increasingly
become
one
of
the
most
promising
battery
technologies
due
to
high
energy
density
and
safety.
However,
adverse
electrode/electrolyte
interface
compatibility
issues
hinder
further
application.
Herein,
a
PEO‐based
composite
solid
electrolyte
excellent
anode
cathode
interfacial
is
designed
via
coordination
modulation
strategy
induced
by
difluorobis(oxalato)phosphate
(DFBOP).
By
utilizing
this
electrolyte,
robust
inorganic‐rich
interphase
involving
LiF,
Li
x
PO
y
F
z
,
P─O
components
in
situ
generated
on
(Li)
LiNi
0.8
Co
0.1
Mn
O
2
(NCM811)
surfaces
forceful
among
PEO,
bis(trifluoromethanesulphonyl)imide,
DFBOP
subsequent
adjustment
front
orbital
levels.
It
contributes
homogeneous
deposition
an
effective
impediment
PEO
oxidation
decomposition
at
voltage,
promoting
superior
stability.
Consequently,
Li‐symmetric
cells
modified
can
achieve
stable
cycle
over
7000
h
0.2
mA
cm
−2
.
Specially,
unique
organic–inorganic
interpenetration
network
structure
enables
4.5
V
Li/NCM811
steadily
100
cycles,
discharge
capacity
215.4
mAh
g
−1
initial
coulombic
efficiency
91.23%.
This
research
has
shed
light
design
from
perspective
regulation
construct
high‐performance
SSLMBs.
Journal of Materials Chemistry A,
Год журнала:
2024,
Номер
12(26), С. 15792 - 15802
Опубликована: Янв. 1, 2024
We
developed
a
computational
protocol
combining
DFT,
COSMO-RS,
and
machine
learning
to
investigate
the
thermodynamic
properties
of
190
binary
solvent
mixtures.
This
approach
demonstrates
high
potential
for
guiding
electrolyte
design.
Angewandte Chemie International Edition,
Год журнала:
2024,
Номер
64(1)
Опубликована: Авг. 29, 2024
Fluorinated
ether-based
electrolytes
are
commonly
employed
in
lithium
metal
batteries
(LMBs)
to
attenuate
the
coordination
ability
of
ether
solvents
with
Li
Advanced Functional Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Июль 11, 2024
Abstract
High‐voltage
lithium‐metal
batteries
(LMBs)
are
promising
for
energy
storage
applications
but
suffer
from
poor
electrochemical
window
of
solid
polymer
electrolytes
(SPEs),
which
difficult
to
achieve
via
a
single
polymeric
functionality.
Herein,
hybrid
Si/F‐based
3D
network
is
reported
bearing
polysiloxane
backbone
with
fluorinated
pendants
tune
the
highest
occupied
molecular
orbital
(HOMO)/the
lowest
unoccupied
LUMO
energies,
thermodynamically
expanding
intrinsic
electrolyte
(SPE).
Meanwhile,
Si/F
functionalities
high
fluorine
abundance
identified
furnish
dual
interfacial
kinetic
stability
at
both
anode
and
cathode
interfaces
stabilized
interface
(SEI)
(CEI),
respectively.
As
result,
stable
cycling
in
solid‐state
high‐voltage
LMBs
achieved
up
an
ultrahigh
operating
voltage
4.9
V.
Furthermore,
it
shows
that
situ
blending
SPE
eutectic
(EE)
form
non‐flammable
gel
can
mitigate
parasitic
reactions
EE
against
metallic
Li
highly
reversible
charge–discharge
4.2
4.8
V
25
°C.
Angewandte Chemie International Edition,
Год журнала:
2024,
Номер
unknown
Опубликована: Окт. 9, 2024
Abstract
Lithium‐ion
batteries
(LIBs)
with
conventional
carbonate‐based
electrolytes
suffer
from
safety
concerns
in
large‐scale
applications.
Phosphates
feature
high
flame
retardancy
but
are
incompatible
graphite
anode
due
to
their
inability
form
a
passivated
solid
electrolyte
interphase
(SEI).
Herein,
we
report
monofluorinated
co‐solvent,
diethyl
fluoridophosphate
(DEFP),
featuring
unique
P−F
bond
that
allows
trade‐off
between
and
electrochemical
performance
LIBs.
The
DEFP
weakens
ion‐dipole
interactions
Li
+
ions,
lowering
the
desolvation
barrier,
simultaneously
reduces
lowest
unoccupied
molecular
orbital
(LUMO)
of
DEFP,
promoting
formation
robust
inorganic‐rich
SEI.
Additionally,
exhibits
improved
thermal
stability
both
SEI
inherent
flame‐retardant
properties
bond.
Consequently,
optimized
DEFP‐based
cyclability
rate
capacity
LiNi
0.8
Co
0.1
Mn
O
2
||graphite
full
cells
compared
triethyl
phosphate‐based
commercial
carbonate
electrolytes.
Even
at
low
E/C
ratio
3.45
g
Ah
−1
,
1.16
NCM811||Gr
pouch
achieve
retention
94.2
%
after
200
cycles.
This
work
provides
promising
approach
decouple
phosphate
compatibility,
paving
way
for
safer
high‐performance
lithium‐ion
batteries.