Abstract
Composite
polymer‐ceramic
electrolytes
have
shown
considerable
potential
for
high‐energy‐density
Li‐metal
batteries
as
they
combine
the
benefits
of
both
polymers
and
ceramics.
However,
low
ionic
conductivity
poor
contact
with
electrodes
limit
their
practical
usage.
In
this
study,
a
highly
conductive
stable
composite
electrolyte
high
ceramic
loading
is
developed
batteries.
The
electrolyte,
produced
through
in
situ
polymerization
composed
polymer
called
poly‐1,3‐dioxolane
poly(vinylidene
fluoride)/ceramic
matrix,
exhibits
excellent
room‐temperature
1.2
mS
cm
−1
stability
Li
metal
over
1500
h.
When
tested
Li|electrolyte|LiFePO
4
battery,
delivers
cycling
performance
rate
capability
at
room
temperature,
discharge
capacity
137
mAh
g
500
cycles
1
C.
Furthermore,
not
only
+
transference
number
0.76
but
also
significantly
lowers
resistance
(from
157.8
to
2.1
Ω)
relative
electrodes.
used
battery
high‐voltage
LiNi
0.8
Mn
0.1
Co
O
2
cathode,
140
achieved.
These
results
show
solid‐state
provide
strategy
designing
polymer‐in‐ceramic
electrode‐compatible
interfaces.
Advanced Energy Materials,
Год журнала:
2021,
Номер
12(2)
Опубликована: Дек. 1, 2021
Abstract
Solid‐state
batteries
(SSBs)
are
an
emerging
technology
for
safe
and
high‐energy‐density
electrochemical
energy
storage.
Unfortunately,
SSBs
suffer
from
inadequate
ionic
conductivity
sluggish
interfacial
transport
at
subzero
temperatures,
which
limit
their
widespread
application.
Herein,
a
flexible,
stable,
highly
conductive
quasi‐solid
polymer
electrolyte
(QSPE)
is
developed
that
allows
low‐temperature
(LT)
operation.
The
in
situ
polymerized
QSPE
has
integrated
battery
structure,
outstanding
(e.g.,
1.0
mS
cm
−1
−30
°C),
exhibits
favorable
compatibility
with
Li
metal
(>2000
h
Li|QSPE|Li).
Li|QSPE|LiFePO
4
high‐voltage
Li|QSPE|LiNi
0.8
Mn
0.1
Co
O
2
demonstrate
excellent
long‐term
stability
cycles
room
temperature)
can
operate
effectively
LT
°C).
Furthermore,
pouch
cells
LiNi
(14.5
mg
−2
)
cathode
show
flexibility,
safety,
high
capacity.
performance
of
this
ascribed
to
its
unique
multilayer
solvation
structure
provides
fast
+
stability.
Thus,
the
newly
chemistry
enables
practical
high‐voltage,
solid‐state
batteries.
SusMat,
Год журнала:
2021,
Номер
1(4), С. 506 - 536
Опубликована: Дек. 1, 2021
Abstract
The
pursuit
of
sustainable
energy
has
a
great
request
for
advanced
storage
devices.
Lithium
metal
batteries
are
regarded
as
potential
electrochemical
system
because
the
extremely
high
capacity
and
most
negative
lithium
anode.
Dead
formed
in
stripping
process
significantly
contributes
to
low
efficiency
short
lifespan
rechargeable
batteries.
This
review
displays
critical
on
current
research
status
about
electrochemistry
significance
robust
anode
is
emphasized.
models
different
scenarios
discussed.
Specific
attention
paid
understanding
principles
atom
diffusion,
reaction,
ion
diffusion
solid
electrolyte
interphase
(SEI),
electron
transfer
with
purpose
strengthen
insights
into
behavior
electrode
stripping.
factors
affecting
processes
corresponding
solutions
summarized
categorized
follows:
surface
physics,
SEI,
operational
external
factors.
affords
fresh
explore
design
based
comprehensive
electrochemistry.
Advanced Energy Materials,
Год журнала:
2023,
Номер
13(10)
Опубликована: Янв. 20, 2023
Abstract
The
low
ionic
conductivity
of
poly(ethylene
oxide)
(PEO)‐based
polymer
electrolytes
at
room
temperature
and
the
undesired
lithium‐dendrite
growth
Li|PEO
interface
impede
their
further
application.
Herein,
a
PEO
is
regulated
molecular
level
through
copper
ion
(Cu
2+
)
coordination
effect
with
both
Li
salts
to
achieve
high
+
0.2
mS
cm
−1
transference
number
0.42
30
°C.
Moreover,
Cu‐coordinated
electrolyte
neither
sticky
nor
hygroscopic
because
hydrophilic
oxygen
groups
in
are
terminated
by
Cu
ions.
Furthermore,
situ
formed
F/Li‐rich
inorganic
layer
induced
CuF
2
additive
accelerates
transport
kinetics
enables
uniform
deposition
during
plating/stripping.
As
result,
‐coordinated
deliver
critical
current
density
1.5
mA
−2
An
all‐solid‐state
Li‐LiNi
0.83
Co
0.12
Mn
0.05
O
(NCM83)
battery
such
coordinated
exhibits
long
cycle
life
over
500
cycles
capacity
retention
71%
under
0.6
C
When
mass
loading
increases
record
7
mg
,
Li‐NCM83
cell
delivers
areal
1.07
mAh
0.1
Journal of the American Chemical Society,
Год журнала:
2023,
Номер
145(47), С. 25632 - 25642
Опубликована: Ноя. 9, 2023
Owing
to
high
ionic
conductivity
and
mechanical
strength,
poly(vinylidene
fluoride)
(PVDF)
electrolytes
have
attracted
increasing
attention
for
solid-state
lithium
batteries,
but
highly
reactive
residual
solvents
severely
plague
cycling
stability.
Herein,
we
report
a
free-solvent-capturing
strategy
triggered
by
reinforced
ion-dipole
interactions
between
Li+
solvent
molecules.
Lithium
difluoro(oxalato)borate
(LiDFOB)
salt
additive
with
electron-withdrawing
capability
serves
as
redistributor
of
the
electropositive
state,
which
offers
more
binding
sites
solvents.
Benefiting
from
modified
coordination
environment,
kinetically
stable
anion-derived
interphases
are
preferentially
formed,
effectively
mitigating
interfacial
side
reactions
electrodes
electrolytes.
As
result,
assembled
battery
shows
lifetime
over
2000
cycles
an
average
Coulombic
efficiency
99.9%
capacity
retention
80%.
Our
discovery
sheds
fresh
light
on
targeted
regulation
extend
cycle
life
batteries.
Advanced Energy Materials,
Год журнала:
2023,
Номер
13(37)
Опубликована: Авг. 3, 2023
Abstract
Lithium
metal‐based
batteries
(LMBs)
have
garnered
significant
attention
due
to
their
exceptional
energy
density
and
lightweight
characteristics.
However,
the
electrochemical
performance
of
LMBs
often
falls
short,
particularly
in
extreme
temperature
conditions.
To
address
these
challenges,
development
electrolytes
capable
withstanding
wide
ranges
has
emerged
as
a
highly
promising
strategy
for
enhancing
operational
capabilities
LMB
across
diverse
weather
This
comprehensive
review
aims
explore
degradation
mechanisms
wide‐temperature
electrolytes,
establishing
fundamental
understanding
failure
that
impede
at
harsh
temperatures.
Essential
properties
required
are
elucidated,
latest
advancements
electrolyte
technologies
tailored
specifically
all‐climate
operations
comprehensively
discussed.
Particular
emphasis
is
placed
on
unique
role
solvation
structure
interfacial
offers
valuable
insights
proposes
directions
practical
implementation
LMBs,
contributing
significantly
existing
knowledge
base
while
concurrently
paving
way
developing
robust
rigors
environments.
Nano-Micro Letters,
Год журнала:
2024,
Номер
16(1)
Опубликована: Янв. 12, 2024
Composite
solid
electrolytes
(CSEs)
have
emerged
as
promising
candidates
for
safe
and
high-energy-density
solid-state
lithium
metal
batteries
(SSLMBs).
However,
concurrently
achieving
exceptional
ionic
conductivity
interface
compatibility
between
the
electrolyte
electrode
presents
a
significant
challenge
in
development
of
high-performance
CSEs
SSLMBs.
To
overcome
these
challenges,
we
present
method
involving
in-situ
polymerization
monomer
within
self-supported
porous
Li
Abstract
Solid‐state
Li‐ion
batteries
have
emerged
as
the
most
promising
next‐generation
energy
storage
systems,
offering
theoretical
advantages
such
superior
safety
and
higher
density.
However,
polymer‐based
solid‐state
face
challenges
across
wide
temperature
ranges.
The
primary
issue
lies
in
fact
that
polymer
electrolytes
exhibit
relatively
low
ionic
conductivity
at
or
below
room
temperature.
This
sensitivity
to
variations
poses
operating
lithium
sub‐zero
temperatures.
Moreover,
elevated
working
temperatures
lead
shrinkage
deformation,
ultimately
resulting
battery
failure.
To
address
this
challenge
of
batteries,
review
presents
an
overview
various
electrolyte
systems.
provides
insights
into
temperature‐dependent
physical
electrochemical
properties
polymers,
aiming
expand
range
operation.
also
further
summarizes
modification
strategies
for
suited
diverse
final
section
performance
different
Valuable
potential
future
research
directions
designing
wide‐temperature
are
presented
based
on
differences
performance.
information
is
intended
inspire
practical
applications
batteries.
Nano-Micro Letters,
Год журнала:
2022,
Номер
14(1)
Опубликована: Окт. 31, 2022
The
rapid
improvement
in
the
gel
polymer
electrolytes
(GPEs)
with
high
ionic
conductivity
brought
it
closer
to
practical
applications
solid-state
Li-metal
batteries.
combination
of
solvent
and
enables
quasi-liquid
fast
ion
transport
GPEs.
However,
different
capacity
between
will
cause
local
nonuniform
Li+
distribution,
leading
severe
dendrite
growth.
In
addition,
poor
thermal
stability
also
limits
operating-temperature
window
electrolytes.
Optimizing
environment
enhancing
are
two
major
challenges
that
hinder
application
Here,
a
strategy
by
introducing
ion-conducting
arrays
(ICA)
is
created
vertical-aligned
montmorillonite
into
GPE.
Rapid
on
ICA
was
demonstrated
6Li
nuclear
magnetic
resonance
synchrotron
X-ray
diffraction,
combined
computer
simulations
visualize
process.
Compared
conventional
randomly
dispersed
fillers,
provides
continuous
interfaces
regulate
enhances
tolerance
GPEs
extreme
temperatures.
Therefore,
GPE/ICA
exhibits
room-temperature
(1.08
mS
cm-1)
long-term
stable
Li
deposition/stripping
cycles
(>
1000
h).
As
final
proof,
Li||GPE/ICA||LiFePO4
cells
exhibit
excellent
cycle
performance
at
wide
temperature
range
(from
0
60
°C),
which
shows
promising
path
toward
all-weather