Advanced Functional Materials,
Journal Year:
2025,
Volume and Issue:
unknown
Published: May 16, 2025
Abstract
Lithium‐sulfur
(Li─S)
batteries
suffer
from
significant
capacity
degradation,
which
is
limited
by
high
barriers
interfacial
desolvation,
Li
+
transportation
to
sulfur
redox
conversions,
exhibiting
the
depressive
kinetics.
Herein,
electron
effect
in
edge
of
catalysts
modulated
and
corresponding
strategy
self‐transform
Schottky
heterojunction
on
MXene
proposed
achieve
delocalized
electronic
density.
As
a
protocol,
electron‐delocalized
boron‐doped
MXene/TiO
2
(SH‐MTB)
fabricated
as
electrochemical
kinetic
accelerators
realize
fast
desolvation
promote
rapid
conversion
kinetics
under
low‐temperature.
Specifically,
with
expedites
dissociation
[Li(solvents)
x
]
generate
free
ions,
well‐confirmed
theoretical
calculations
ex‐situ/in
situ
characterizations.
Encouragingly,
higher
practical
areal
(5.0
mAh
cm
−2
)
negligible
self‐discharge
behaviors
are
achieved
low‐temperature
environments.
A
large
pouch
cell
200
mg
s
exhibits
9.3
lean
electrolyte
amount
(5
µL
−1
),
much
better
than
state‐of‐art
reports.
further
indicated
microscopies,
spectroscopical
measurements
X‐ray
tests,
SH‐MTB
stabilizes
chemical
structure
during
charge/discharge
process,
showing
promising
potential
heterostructure
toward
accelerating
cascade
carrier
metal
battery
Advanced Functional Materials,
Journal Year:
2025,
Volume and Issue:
unknown
Published: Feb. 23, 2025
Abstract
Separators
are
crucial
in
lithium‐sulfur
batteries
(LiSBs)
to
ensure
optimal
ion
transport
and
prevent
internal
short
circuits.
High‐performance
separators
with
excellent
thermal
stability,
electrolyte
wettability,
porosity,
Li
+
selectivity
essential
for
the
safety
enhancing
energy
density
of
LiSBs.
This
is
particularly
important
mitigating
polysulfide
(LiPS)
shuttling,
which
degrades
both
capacity
cycling
stability
In
this
work,
a
novel
separator
design
high‐performance
LiSBs
introduced
that
combines
poly(ether
ether
ketone)
(PEEK)‐based
inverse
opal
(PIO)
architecture
an
situ
grown
cobalt‐imidazole
metal‐organic
framework
ZIF‐67
on
polymeric
surface.
The
PIO
provides
improved
conductivity
due
unique
structural
characteristics
thermal/mechanical
properties
PEEK.
Additionally,
imparts
enhanced
electrochemical
system
through
its
selective
permittivity
LiPS.
chemical
configuration
significantly
suppresses
LiPS
shuttling;
negative
imidazole
sites
accelerate
mobility
while
Lewis
acidic
Co
2+
centers
strongly
interact
S
x
2−
base.
Consequently,
developed
exhibits
remarkable
inhibition
shuttling
synergistic
effects
from
acid‐base
interactions
physical
separator.
It
also
demonstrates
effective
regulation
Li‐dendrite
growth,
leading
With
greatly
performance,
rate
capability,
ZIF‐PIO
presented
work
promising
solution
practical
applications.
ACS Nano,
Journal Year:
2025,
Volume and Issue:
unknown
Published: March 11, 2025
Covalent
organic
frameworks
(COFs)
have
shown
promise
as
bifunctional
catalysts
to
simultaneously
mitigate
shuttle
effects
and
Li
dendrite
issues
of
lithium–sulfur
(Li–S)
batteries.
However,
the
inherent
low
conductivity
COFs
has
significantly
limited
their
catalytic
activity
stability.
Herein,
durability
COF/MXene
heterostructure
are
activated
by
tuning
surface
curvatures
interfaced
with
MXene.
The
increased
curvature
could
induce
enhanced
electron
delocalization
alter
geometry,
which
in
turn
strengthens
lithium
polysulfide
adsorption,
lowers
energy
barriers,
stabilizes
sites
promote
sulfur
redox
reactions.
Concurrently,
hierarchical
structure
improves
electrolyte
penetration
wettability,
facilitates
rapid
ion
transport,
homogenizes
Li-ion
flux
distribution,
thus
achieving
uniform
deposition.
Consequently,
1D-COF/MXene
Li–S
batteries
demonstrate
a
high-rate
capacity
926
mA
h
g–1
at
4C,
stable
cycling
performance
reversible
589
3C
after
500
cycles,
high
604
cm–2
loading
3.5
mg
under
electrolyte-to-sulfur
ratio
10
μL
mg–1.
This
work
offers
an
efficacious
approach
regulate
stability
catalysts.
Advanced Functional Materials,
Journal Year:
2024,
Volume and Issue:
unknown
Published: Nov. 27, 2024
Abstract
Lithium–sulfur
(Li–S)
batteries
are
considered
as
potential
candidates
for
future‐oriented
energy
storage
systems.
However,
their
practical
deployment
is
hampered
by
the
shuttle
effect
and
sluggish
reaction
kinetics
of
lithium
polysulfides
(LiPSs).
A
key
strategy
to
mitigate
these
challenges
develop
efficient
heterojunction
catalysts
enhance
suppress
effect.
In
this
study,
a
NiS
2
‐CoS
introduced
address
with
density
functional
theory
(DFT)
calculations
employed
determine
optimal
combination
from
5
×
crystal
plane
configurations.
The
identified
(210)‐CoS
(200)
demonstrates
excellent
anchoring
effects
catalytic
properties
LiPSs,
significantly
enhancing
rate
performance
(839.9
mAh
g
−1
at
C
730.8
3
C)
cycling
stability.
Furthermore,
in
situ
Raman
X‐ray
diffraction
(XRD)
analyses
reveal
that
rapidly
catalyzes
conversion
reducing
migration
toward
anode
thereby
suppressing
design
transition
metal
sulfide
heterojunctions
offers
an
approach
accelerating
polysulfide
kinetics,
effectively
addressing
limitations
Li–S
batteries.
Rationally
designing
and
constructing
ionic/electronic
coconductor
electrocatalysts
with
adjustable
active
sites
to
enhance
the
redox
kinetics
of
lithium–sulfur
batteries
(LSBs)
in
lean
electrolyte
conditions
is
a
challenge.
Herein,
this
study
presents
promotion
for
lithium
polysulfides
(LiPSs)
through
construction
ion/electron
coconductive
catalytic
triple-phase
interface
using
lanthanum
titanate/carbon
(LLTO/C)
nanofibers,
which
due
manipulating
geometric
torsion
BO6
octahedron
LLTO.
Experiments
theoretical
calculations
demonstrate
that
changes
coordination
environment
O–Ti–O
LLTO
causes
oxygen
vacancy
lattice
distortion.
This
enhances
local
electronic
state
density,
ion
migration
rate,
high
activity
LLTO,
thereby
resulting
synergistic
effect
good
chemisorption
rapid
conversion
LiPSs.
Therefore,
when
modified
separator
used,
LSBs
electrocatalyst
realize
discharge
capacity
1024
mA
h·g–1
at
current
rate
2
C.
Upon
sulfur
loading
9
mg
·cm–2
electrolyte/sulfur
ratio
4
μL·
mg–1,
an
acceptable
areal
9.1
h·
cm–2
achieved.
work
provides
new
perspective
rational
design
catalysts
LSBs.