Advanced Functional Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Март 9, 2025
Abstract
Lithium‐sulfur
batteries
face
three
fundamental
challenges:
uncontrolled
polysulfide
shuttling,
substantial
volumetric
fluctuations
during
cycling,
and
the
inherent
electrical
insulation
of
sulfur.
To
address
these
limitations,
an
asymmetric
self‐supporting
cathode
is
developed,
featuring
TiO₂‐decorated
carbon
nanofibers
synergistically
integrated
with
hollow
shells
encapsulating
vanadium
nitride
catalysts
(VN/C@TCF).
Distinct
from
conventional
configurations,
this
hierarchically
structured
“triple‐nanolayer”
system
establishes
sequential
mitigation
mechanisms:
(I)
TiO
2
nanoparticles
in
inner
layer
provide
chemical
immobilization
polysulfides;
(II)
intermediate
shell
enables
physical
confinement;
(III)
outer
VN
nanosheets
offer
anchoring
capacity.
Combined
density
functional
theory
calculations
experimental
analyses
reveal
that
VN/C@TCF
architecture
simultaneously
enhances
conductivity,
demonstrates
superior
catalytic
activity,
accommodates
volume
variations
electrochemical
cycling.
The
optimized
delivers
exceptional
performance
metrics,
including
a
high
initial
discharge
capacity
1417.9
mAh
g⁻¹
at
0.1
C
remarkable
rate
capability
(803.2
5
C).
Notably,
electrode
can
maintain
impressive
areal
6.30
cm⁻
after
80
cycles
under
stringent
operational
conditions
sulfur
loading
(8.1
mg
)
lean
electrolyte
(E/S
ratio
=
4.8
µL
mg⁻¹).
This
strategic
design
paradigm
provides
new
insights
for
developing
electrocatalytic
systems
advanced
lithium‐sulfur
batteries.
Interdisciplinary materials,
Год журнала:
2023,
Номер
2(3), С. 390 - 415
Опубликована: Май 1, 2023
Abstract
The
chief
culprit
impeding
the
commercialization
of
lithium–sulfur
(Li–S)
batteries
is
parasitic
shuttle
effect
and
restricted
redox
kinetics
lithium
polysulfides
(LiPSs).
To
circumvent
these
key
stumbling
blocks,
incorporating
electrocatalysts
with
rational
electronic
structure
modulation
into
sulfur
cathode
plays
a
decisive
role
in
vitalizing
higher
electrocatalytic
activity
to
promote
utilization
efficiency.
Breaking
stereotype
contemporary
electrocatalyst
design
kept
on
pretreatment,
field‐assisted
offer
strategic
advantages
dynamically
controllable
electrochemical
reactions
that
might
be
thorny
regulate
conventional
processes.
However,
highly
interdisciplinary
electrochemistry
puzzles
researchers
for
fundamental
understanding
ambiguous
correlations
among
structure,
surface
adsorption
properties,
catalytic
performance.
In
this
review,
mechanisms,
functionality
explorations,
including
electric,
magnetic,
light,
thermal,
strain
fields
Li–S
have
been
summarized.
By
demonstrating
pioneering
work
customized
geometric
configuration,
energy
band
engineering,
optimal
microenvironment
arrangement
response
decreased
activation
enriched
reactant
concentration
accelerated
kinetics,
cutting‐edge
insights
holistic
periscope
charge‐spin‐orbital‐lattice
interplay
between
LiPSs
are
scrutinized,
which
aspires
advance
comprehensive
complex
batteries.
Finally,
future
perspectives
provided
inspire
innovations
capable
defeating
existing
restrictions.
Abstract
Lithium−sulfur
(Li–S)
battery
is
of
great
potential
for
the
next
generation
energy
storage
device
due
to
high
specific
capacity
density.
However,
sluggish
kinetics
S
redox
and
dendrite
Li
growth
are
main
challenges
hinder
its
commercial
application.
Herein,
an
organic
electrolyte
additive,
i.e.,
benzyl
chloride
(BzCl),
applied
as
remedy
address
two
issues.
In
detail,
BzCl
can
split
into
Bz·
radical
react
with
polysulfides,
forming
a
Bz–S–Bz
intermediate,
which
changes
conversion
path
improves
by
accelerating
splitting.
Meanwhile,
tight
robust
solid
interphase
(SEI)
rich
in
inorganic
ingredients
namely
LiCl,
LiF,
2
O,
formed
on
surface
metal,
ion
conductivity
blocking
decomposition
solvent
lithium
polysulfides.
Therefore,
Li–S
additive
remains
693.2
mAh
g
−1
after
220
cycles
at
0.5
C
low
decay
rate
0.11%.
This
work
provides
novel
strategy
boost
electrochemical
performances
both
cathode
anode
gives
guide
design
toward
high‐performance
batteries.
