Journal of The Electrochemical Society,
Год журнала:
2024,
Номер
171(10), С. 100522 - 100522
Опубликована: Окт. 1, 2024
In
this
study,
a
series
of
novel
inorganic-organic
hybrid
sulfide
solid
electrolytes
was
synthesized
by
doping
Li
7
P
2
S
8
I
with
selection
tetraalkylammonium
iodides,
including
tetramethylammonium
iodide
(TMAI),
tetraethylammonium
(TEAI),
tetrapropylammonium
(TPAI),
and
tetrabutylammonium
(TBAI).
The
were
prepared
in
varying
compositions,
represented
as
(1−x)
·
x
(TMAI,
TEAI,
TPAI,
TBAI),
where
values
adjusted
to
0,
0.05,
0.1,
0.2
(molar
ratio)
assess
their
influence
on
the
electrolyte
properties.
hybrids
exhibited
predominantly
amorphous
structures.
Tetraalkylammonium
iodides
longer
alkyl
chains
lower
ionic
conductivities.
Mechanical
characterization
via
indentation
tests
indicated
that
incorporation
reduced
elastic
moduli
composites.
This
study
presents
methodological
approach
for
modulating
structural
mechanical
properties
through
strategic
organic
doping.
Advanced Energy Materials,
Год журнала:
2024,
Номер
14(12)
Опубликована: Янв. 18, 2024
Abstract
A
stable
interfacial
design
bridging
Li
metal
and
sulfide
solid
electrolytes
is
imperative
for
deploying
practical
all‐solid‐state
batteries.
Despite
the
extensive
exploration
of
interlayer
materials,
including
inorganic
substances,
lithiophilic
metals,
their
composites,
a
comprehensive
understanding
stability
chemo‐mechanical
evolution,
particularly
those
influenced
by
cell
fabrication
processes,
remains
unexplored.
Herein,
it
meticulously
investigate
formation
evolution
LiF,
Mg,
conversion‐type
multicomponent
MgF
2
ultrathin
interlayers,
each
fabricated
via
thermal
evaporation
deposition.
Unexpectedly,
LiF
Mg
fail
to
enhance
performance,
with
notably
susceptible
external
pressures
during
fabrication,
leading
serious
current
constriction,
while
deposition
results
in
Li‐rich
solution.
Remarkably,
coatings
demonstrate
substantially
superior
performance
both
Li|Li
6
PS
5
Cl|Li
symmetric
cells
(up
2000
h)
LiNi
0.70
Co
0.15
Mn
O
|Li
full‐cells
(82%
capacity
retention
after
800
cycles)
at
30
°C.
These
are
attributed
in‐situ
x
nanograins
through
conversion
reaction,
which,
repeated
cycling,
maintains
fixed
position
interface
ensuring
uniform
+
flux.
Supported
analyses,
these
findings
highlight
pivotal
role
interlayers
mitigating
side
reactions
preventing
penetration.
Advanced Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Авг. 27, 2024
Abstract
The
silicon‐based
anodes
are
one
of
the
promising
to
achieve
high
energy
density
all‐solid‐state
batteries
(ASSBs).
Nano
silicon
(nSi)
is
considered
as
a
suitable
anode
material
for
assembling
sheet‐type
sulfide
ASSBs
using
thin
free‐standing
Li
6
PS
5
Cl
(LPSC)
membrane
without
causing
short
circuit.
However,
nSi
face
significant
challenge
in
terms
rapid
capacity
degradation
during
cycling.
To
address
this
issue,
dual‐function
4.4
Si
modified
sheets
developed,
which
serves
dual
role
by
not
only
providing
additional
+
but
also
stabilizing
structure
with
its
low
Young's
modulus
upon
Sheet‐type
equipped
anode,
LPSC
membrane,
and
LiNi
0.83
Co
0.11
Mn
0.06
O
2
(NCM811)
cathode
demonstrate
exceptional
cycle
stability,
retention
96.16%
at
0.5
C
(1.18
mA
cm
−2
)
after
100
cycles
maintain
stability
400
cycles.
Furthermore,
remarkable
cell‐level
303.9
Wh
kg
−1
achieved
loading
5.22
mAh
,
representing
leading
level
electrolyte
membranes
room
temperature.
Consequently,
chemically
stable
slurry
process
implemented
fabrication
Si‐modified
sheet
paves
way
scalable
applications
high‐performance
ASSBs.
Advanced Energy Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Июнь 12, 2024
Abstract
In
the
ongoing
quest
to
develop
lithium‐ion
batteries
with
superior
capacity
and
enhanced
safety,
focus
has
shifted
toward
all‐solid‐state
(SSBs)
nickel‐rich
cathode
materials.
Despite
their
promise,
these
technologies
face
significant
interface
challenges,
notably
poor
contact
low
ion
transport
efficiency,
leading
substantial
stability
issues.
This
review
aims
provide
a
comprehensive
analysis
of
both
advantages
challenges
associated
batteries.
addition,
it
discusses
benefits
single‐crystal
application
in
SSBs,
terms
kinetic
performance,
mechanical
properties,
stability.
The
concludes
by
proposing
various
strategies
optimize
technologies,
targeting
development
efficient
materials
for
use
These
approaches
offer
potential
address
core
currently
faced
SSBs
pave
way
next
generation
high‐performance
Advanced Functional Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Фев. 5, 2025
Abstract
Understanding
the
interfacial
reaction
mechanism
between
sulfide
solid‐state
electrolytes
(SSEs)
and
metallic
lithium
(Li)
under
thermal
runaway
is
of
great
significance
in
improving
safety
all‐solid‐state
Li
metal
batteries
(ASLMBs).
Herein,
multiscale
methods
including
situ
optical
microscopy‐thermal
infrared
imaging
combination
technique,
cryogenic
electron
microscopy,
thermodynamic
simulation,
ab
initio
molecular
dynamics
are
utilized
to
investigate
chemical
stability
SSEs
10
GeP
2
S
12
(LGPS)
6
PS
5
Cl
(LPSCl)
against
high
temperatures.
The
results
indicate
that
drastic
happened
LGPS
at
300
°C
due
continuous
Li‐Germanium
alloying
reaction.
In
contrast,
LPSCl
maintains
up
400
°C,
which
attributed
formation
S‐LiP‐Li
3
P‐LiCl
stable
interphases
Li.
electrical
insulation
interphase
prevents
further
via
kinetically
decreasing
potential
be
within
electrochemical
window
LPSCl.
This
work
demonstrates
critical
role
electrically
insulated
anode
ASLMBs.
Advanced Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Март 10, 2025
All-solid-state
batteries
(ASSBs)
are
promising
candidates
for
next-generation
energy
storage
devices
due
to
their
high
density
and
enhanced
safety.
Binder
plays
an
irreplaceable
role
in
stabilizing
the
electrode
structure,
enhancing
carrier
transport
modulating
solid
electrolyte
interfaces
by
connecting
each
component
of
electrode.
The
development
functional
binders
is
seen
as
a
key
strategy
achieve
higher
densities
ASSBs.
This
review
systematically
examines
recent
progress
binder
development,
focusing
on
roles,
impacts,
failure
mechanisms
It
begins
outlining
specific
functionalities
required
ASSBs
provides
comprehensive
summary
applications
across
different
components,
including
anode,
cathode,
electrolyte.
Furthermore,
highlights
innovative
design
principles
while
also
summarizing
testing
methods
advanced
characterization
techniques
evaluating
performance.
proposes
future
directions
based
current
developments
emerging
technologies,
with
aim
creating
optimal
systems
high-energy-density
applications.
Advanced Energy Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Апрель 8, 2025
Abstract
All‐solid‐state
lithium–sulfur
batteries
(ASSLSBs)
incorporating
sulfide‐based
superionic
conductors
offer
high
safety
and
energy
density
are
cost‐efficient.
However,
the
effective
utilization
of
sulfur
is
challenging
due
to
difficulties
in
forming
an
intimate
triple‐phase
interface
between
electronic
conductors,
ionic
sulfur.
In
this
study,
high‐performance
ASSLSBs
achieved
through
a
simple
two‐step
mixing
method
that
combines
1)
high‐energy
ball
milling
2)
mild
sulfur/carbon
composite
with
Li
6
PS
5
Cl
(LPSCl).
This
approach
reduces
particle
size,
enhances
uniformity,
activates
redox
reaction
LPSCl
while
preserving
its
conductivity,
ultimately
creating
well‐distributed
conduction
pathways
thick
electrodes.
During
milling,
catenation
leads
formation
inorganic
Li‐ion‐conducting
species,
improving
contact
Moreover,
S–S
bridging
cleavage
reactions
oxidatively
decomposed
contribute
reversibly
additional
capacity
within
operating
voltage
range.
Consequently,
optimal
ASSLSB
demonstrated
areal
10.1
mAh
cm
−2
,
retaining
92.0%
initial
after
150
cycles
at
30
°C.
cathode
design
further
extendable
other
sulfur‐based
cathodes
dry
electrode
fabrication,
offering
viable
pathway
toward
practical
ASSLSBs.
Advanced Energy Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Апрель 28, 2025
Abstract
Designing
a
solid‐state
electrolyte
(SSE)
that
combines
the
lithium‐ion
transport
behavior
found
in
liquid
or
solid
polymer
electrolytes
with
high
transference
number
characteristic
of
inorganic
SSEs
is
an
immensely
appealing
challenge.
Herein,
cost‐effective,
chain‐structured
ZrCl
4
introduced
as
hosting
matrix,
resembling
polyethylene
oxide
(PEO),
to
facilitate
dissociation
lithium
salts
(e.g.,
LiCl,
Li
2
SO
,
and
3
PO
).
The
dissociated
free
Li‐ions
can
be
coordinated
by
[ZrCl
6
]
octahedra,
forming
fast
ion‐conducting
pathways
along
chains
achieve
ionic
conductivity
1.2
mS
cm
−1
.
Simultaneously,
serves
Lewis
acid,
trapping
anions
delivering
approaching
unit.
proposed
exhibits
stable
cycling
performance
when
integrated
into
LiNi
0.8
Mn
0.1
Co
O
||Li‐In
cells.
Moreover,
this
design
strategy
also
extends
synthesis
sodium‐ion
conductors,
achieving
0.3
Demonstrating
previously
unreported
conduction
mechanism,
‐based
offer
versatile
approach
for
tailoring
advanced
SSEs.