Advanced Energy Materials,
Journal Year:
2024,
Volume and Issue:
unknown
Published: Dec. 5, 2024
Abstract
To
advance
the
sustainable
development
of
Li‐ion
batteries,
reducing
Co
content
in
Li[Ni
x
y
(Mn
or
Al)
(1–
–
)
]O
2
has
become
essential,
prompting
exploration
Co‐free
Mn
alternatives.
Among
promising
solutions
are
layered
cathodes
with
compositional
concentration
gradients,
which
offer
significant
potential.
However,
their
unique
microstructure
and
partitioning,
key
to
performance,
highly
sensitive
synthesis
temperatures.
Over‐sintering
can
lead
structural
unpredictability
cathode
materials
detrimental
effects
on
electrochemical
properties.
In
this
study,
a
stable
oxide
is
developed
by
doping
gradient
0.9
0.1
,
high‐valence
ions.
This
innovative
strategy
significantly
reduces
sensitivity
calcination
temperatures,
minimizing
nano‐
microstructural
changes
across
broad
temperature
range
(750–810
°C).
The
particle‐level
gradation
grain‐level
heteroelement
encapsulation
contribute
material's
exceptional
performance.
Mo
doping,
trace
amounts,
plays
pivotal
role
maintaining
stability
cathodes,
enabling
high‐potential
(4.3
V
vs
graphite)
suitable
for
practical
battery
applications.
Advanced Energy Materials,
Journal Year:
2025,
Volume and Issue:
unknown
Published: April 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.
