Angewandte Chemie,
Год журнала:
2024,
Номер
unknown
Опубликована: Окт. 10, 2024
Abstract
Solid‐electrolyte
interphase
(SEI)
plays
a
decisive
role
in
building
reliable
Li
metal
batteries.
However,
the
scarcity
of
anions
Helmholtz
layer
(HL)
caused
by
electrostatic
repulsion
usually
leads
to
inferior
SEI
derived
from
solvents,
resulting
dendrites
and
‘dead’
Li.
Therefore,
regulating
distribution
electric
double
(EDL)
continuously
introducing
more
into
HL
tailor
anions‐derived
is
crucial
for
achieving
stable
plating/stripping.
Herein,
jointly
utilizing
controlled
defects
reduced
graphene
oxide
(rGO)
oriented
dipoles
ferroelectric
BaTiO
3
(BTO),
rGO‐BTO
composite
sustainedly
brings
TFSI
−
NO
anion‐defecient
HL,
promoting
favorable
decomposition
guiding
generation
robust
fast‐Li
+
‐transport
containing
inorganics
LiF
N
species.
Thus,
deposit
shows
smooth
dense
morphologies
without
dendrites,
leading
high
average
Coulombic
efficiency.
The
Li//Cu@rGO‐BTO
(10
mAh
cm
−2
plated
Li)
cell
exhibits
an
enhanced
plating/stripping
stability
(2700
h)
higher
rate
capability.
LiFePO
4
full
(N/P≈6.3)
using
displays
capacity
retention
(82.0
%
@
430
cycles).
This
work
provides
new
insight
on
construction
within
EDL.
Advanced Energy Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Окт. 9, 2024
Abstract
To
facilitate
the
use
of
solid
polymer
electrolytes
(SPEs)
with
high‐nickel
(Ni)
cathodes
in
high‐voltage
lithium
(Li)
metal
batteries
(LMBs),
it
is
crucial
to
address
challenges
low
oxidative
stability
and
formation
vulnerable
interphases.
In
this
study,
isocyanate
groups
(−N═C═O)
are
incorporated
develop
an
SPE
a
bi‐continuous
structure,
consisting
elastomeric
plastic
crystal
phases.
This
rationally
designed
exhibits
high
ionic
conductivity
(0.9
×
10
−3
S
cm
−1
at
25
°C),
excellent
elasticity
(elongation
break
330%),
enhanced
(over
4.8
V
vs.
Li/Li⁺).
A
full
cell,
incorporating
thin
Li
foil
40
µm,
high‐Ni
LiNi
0.8
Co
0.1
Mn
O
2
(NCM811)
cathode
operating
4.7
Li/Li⁺,
demonstrates
cyclability,
retaining
70%
its
initial
capacity
after
200
cycles
under
C‐rate
1C
°C.
The
extended
cycling
isocyanate‐containing
Li/Li⁺
attributed
robust
compact
inorganic‐rich
interphases
enabled
by
antioxidative
−N−C═O
components,
as
well
uniform
deposition
structured
SPE.
study
suggests
that
system
promising
candidate
for
solid‐state
LMBs
constructing
stable
ACS Applied Materials & Interfaces,
Год журнала:
2025,
Номер
17(9), С. 14058 - 14072
Опубликована: Фев. 18, 2025
Poly(vinylidene
fluoride)
(PVDF)
is
promising
for
polymer
solid-state
electrolytes
(PSEs)
but
faces
challenges
such
as
low
ionic
conductivity,
uneven
strain
distribution,
and
poor
lithium
(Li)
dendrite
inhibition.
Herein,
an
effective
strategy
proposed
to
enhance
PVDF-based
PSEs
by
incorporating
a
fast
ion
conductor
LiZr2(PO4)3
(LZP)
with
negative
thermal
expansion
property
NASICON-type
structure,
the
effects
are
investigated
using
multifarious
methods.
The
added
LZP
not
only
enhances
mobility
of
PVDF
chain
concentration
free
Li+,
regulates
heat
release
volume
during
cycles,
thereby
protecting
electrode
morphology
well
improving
interface
between
electrolyte.
Compared
pristine
PSEs,
conductivity
increased
3.3
×
10-4
S
cm-1,
stability
augmented
adding
10
wt
%
LZP.
At
25
°C
0.5
C,
values
discharge
capacity
retention
Li|PVDF-10
%LZP|LiFePO4
%LZP|LiNi0.8Co0.1Mn0.1O2
full
cells
without
liquid
improved
from
61.4
53.4%
90.4
87.7%
after
300
200
respectively.
enhancement
mechanisms
based
on
interactions
heat,
deformation,
interface,
transfer.
It
paves
unique
way
develop
simultaneously
adjusting
mechanics.
An
advanced
structure
capable
of
hosting
large
electrochemical
activity
with
desired
balance
in
ion
diffusion
kinetics,
faradic
charge
storage,
and
robust
stability
is
the
key
to
developing
high-performance
fabric-based
supercapacitors
(FSCs).
Herein,
we
develop
a
hierarchical
multimetal
oxides@graphene
fabric
(Cu-MO@GFF)
as
supercapacitor
electrode
accelerated
ionic
diffusion,
adsorption
energy,
redox
reaction
reversibility.
As
result,
Cu-MO@GFF
presents
excellent
mass
capacitance
(534
F
g-1),
high
rate
performance
(266
g-1
at
10
A
good
cycle
(96.9%
capacitive
retention
after
20,000
cycles)
6
mol
L-1
(M)
KOH
electrolyte.
In
addition,
Cu-MO@GFF-based
solid-state
FSC
delivers
energy
density
(11.875
Wh
kg-1),
much-improved
cyclic
stability,
bending
capability.
On
account
behavior,
this
can
flexibly
power
various
wearable
devices
(such
luminous
tags,
bracelets,
watches),
which
will
offer
new
avenue
for
innovating
next-generation
devices.
Advanced Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Март 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.
ACS Applied Materials & Interfaces,
Год журнала:
2025,
Номер
unknown
Опубликована: Апрель 21, 2025
Improving
the
room
temperature
ionic
conductivity
of
solid-state
polymer
electrolytes
for
lithium
batteries
is
a
big
challenge.
Exploring
new
composite
one
important
solutions.
Herein,
inorganic
two-dimensional
layered
metal
boride
nanomaterial
(MBene)
was
first
applied
to
electrolyte.
The
hyperbranched
cross-linking
electrolyte
prepared
by
free
radical
polymerization
double
bond
modified
MBene
and
ether
with
bonds
in
presence
PVDF-HFP
salt.
c
provided
material
characteristics
adsorbing
salt
anion.
As
result,
DBMBene-DBHPG-PH
CPEs
reaches
9.35
×
10-4
S
cm-1.
Combination
ATR-FTIR
spectra,
XANES
DFT
calculation
reveals
influence
on
ion
transport.
Dendrite-free
growth
high
reversibility
can
be
maintained
more
than
2000
h
plating/stripping
symmetric
batteries.
solid
adapted
LFP
LMFP,
NCM523
high-voltage
cathode
materials.
It
worth
mentioning
that
assembled
pouch
cell
also
run
stably
150
cycles
at
0.1
C,
showing
higher
cycle
capacity.
This
work
not
only
demonstrates
novel
MBene-based
provides
an
effective
strategy
prevent
aggregation
fillers
but
exhibits
excellent
application
prospects
high-energy
density
ACS Nano,
Год журнала:
2024,
Номер
18(27), С. 17890 - 17900
Опубликована: Июнь 25, 2024
Ultrathin
composite
electrolytes
hold
great
promise
for
high
energy
density
solid-state
lithium
metal
batteries
(SSLMBs).
However,
finding
an
electrolyte
that
can
simultaneously
balance
the
interfacial
stability
of
anode
and
high-voltage
cathode
is
challenging.
The
present
study
utilized
both-side
tape
casting
technique
to
fabricate
ultrathin
asymmetric
reinforced
with
polyimide
(PI)
fiber
membrane,
a
thickness
26.8
μm.
implementation
this
structural
design
enables
SSLMBs
attain
favorable
characteristics,
such
as
exceptional
resistance
dendrite
puncture
compatibility
voltages.
suppression
growth
extension
cycle
life
symmetric
by
4000
h
are
both
experimental
theoretically
demonstrated
under
dual
confinement
PI
membrane
Li7La3Zr2O12
ceramic
fibers.
Furthermore,
integration
multicomponent
solid
interphase
interface
layers
into
enhance
theirs
cycling
stability.
With
gravimetric/volumetric
333.1
Wh
kg-1/713.2
L-1,
assembled
LiNi0.8Co0.1Mn0.1O2
pouch
cell
demonstrates
safety.
extensive
application
concept
resolution
electrode/electrolyte
issues.
ACS Applied Materials & Interfaces,
Год журнала:
2024,
Номер
16(17), С. 22482 - 22492
Опубликована: Апрель 23, 2024
Herein,
we
present
the
preparation
and
properties
of
an
ultrathin,
mechanically
robust,
quasi-solid
composite
electrolyte
(SEO-QSCE)
for
solid-state
lithium
metal
battery
(SLB)
from
a
well-defined
polystyrene-b-poly(ethylene
oxide)
diblock
copolymer
(SEO),
Li6.75La3Zr1.75Ta0.25O12
nanofiller,
fluoroethylene
carbonate
plasticizer.
Compared
with
ordered
lamellar
microphase
separation
SEO,
SEO-QSCE
displays
bicontinuous
phases,
consisting
Li+
ion
conductive
poly(ethylene
domain
robust
framework
polystyrene
domain.
Therefore,
12
μm-thick
membrane
exhibits
exceptional
ionic
conductivity
1.3
×
10–3
S
cm–1
at
30
°C,
along
remarkable
tensile
strength
5.1
MPa
elastic
modulus
2.7
GPa.
The
high
mechanical
robustness
self-generated
LiF-rich
SEI
enable
to
have
extraordinary
dendrite
prohibition
effect.
SLB
Li|SEO-QSCE|LiFePO4
reveals
superior
cycling
performances
°C
over
600
cycles,
maintaining
initial
discharge
capacity
145
mAh
g–1
retention
81%
(117
g–1)
after
400
cycles
0.5
C.
high-voltage
Li|SEO-QSCE|LiNi0.5Co0.3Mn0.2O2
good
stability
150
°C.
Moreover,
enables
pouch
cell
flexibility
excellent
safety
features.
current
investigation
delivers
promising
innovative
approach
preparing
electrolytes
features
ultrathin
design,
robustness,
electrochemical
performance
SLBs.