Abstract
Lithium–sulfur
(Li–S)
batteries
are
one
of
the
promising
next‐generation
energy
storage/conversion
devices,
considering
their
high
density
and
low
cost.
However,
shuttle
polysulfides
hinders
practical
application
Li–S
batteries,
which
leads
to
reduced
cycling
stability.
Although
chemical
adsorption
strategies
have
made
significant
progress
in
improving
stability
poor
catalytic
conversion
ability
polysulfide
host
results
an
imbalance
between
conversion.
Recent
studies
revealed
that
metal
oxides
with
adjustable
electronic
structures
exhibit
good
as
hosts.
there
is
currently
no
systematic
review
mechanism
batteries.
Herein,
working
principle
primary
challenge
first
introduced,
followed
by
a
categorization
catalyst
design
strategies.
Furthermore,
comprehensive
recent
advancements
understanding
reaction
oxide
catalysts
also
provided.
Finally,
personal
perspectives
on
future
development
enhanced
catalysis
offered.
It
hoped
this
can
provide
valuable
insights
into
role
accelerating
for
Nano-Micro Letters,
Год журнала:
2023,
Номер
16(1)
Опубликована: Ноя. 10, 2023
Lithium-sulfur
(Li-S)
batteries
are
supposed
to
be
one
of
the
most
potential
next-generation
owing
their
high
theoretical
capacity
and
low
cost.
Nevertheless,
shuttle
effect
firm
multi-step
two-electron
reaction
between
sulfur
lithium
in
liquid
electrolyte
makes
much
smaller
than
value.
Many
methods
were
proposed
for
inhibiting
polysulfide,
improving
corresponding
redox
kinetics
enhancing
integral
performance
Li-S
batteries.
Here,
we
will
comprehensively
systematically
summarize
strategies
from
all
components
First,
electrochemical
principles/mechanism
origin
described
detail.
Moreover,
efficient
strategies,
including
boosting
conversion
rate
sulfur,
confining
or
polysulfides
(LPS)
within
cathode
host,
LPS
shield
layer,
preventing
contacting
anode,
discussed
suppress
effect.
Then,
recent
advances
inhibition
cathode,
electrolyte,
separator,
anode
with
aforementioned
have
been
summarized
direct
further
design
materials
Finally,
present
prospects
development
directions
Advanced Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Окт. 14, 2024
Lithium-sulfur
batteries
(LSB)
with
high
theoretical
energy
density
are
plagued
by
the
infamous
shuttle
effect
of
lithium
polysulfide
(LPS)
and
sluggish
sulfur
reduction/evolution
reaction.
Extensive
research
is
conducted
on
how
to
suppress
effects,
including
physical
structure
confinement
engineering,
chemical
adsorption
strategy,
design
redox
catalysts.
Recently,
rational
mitigate
effects
enhance
reaction
kinetics
based
field
has
been
widely
studied,
providing
a
more
fundamental
understanding
interactions
species.
Herein,
focused
their
methods
mechanisms
interaction
summarized
systematically
LPS.
Overall,
working
principle
LSB
system,
origin
effect,
kinetic
trouble
in
briefly
described.
Then,
mechanism
application
materials
concepts
external
field-assisted
elaborated,
electrostatic
force,
built-in
electric
field,
spin
state
regulation,
strain
magnetic
photoassisted
other
strategies
pivotally
elaborated
discussed.
Finally,
potential
directions
enhancing
performance
weakening
high-energy
anticipated.
Abstract
The
commercialization
of
lithium–sulfur
(Li–S)
battery
is
seriously
hindered
by
the
shuttle
behavior
lithium
(Li)
polysulfide,
slow
conversion
kinetics,
and
Li
dendrite
growth.
Herein,
a
novel
hierarchical
p‐type
iron
nitride
n‐type
vanadium
(p‐Fe
2
N/n‐VN)
heterostructure
with
optimal
electronic
structure,
confined
in
vesicle‐like
N‐doped
nanofibers
N/n‐VN⊂PNCF),
meticulously
constructed
to
work
as
“one
stone
two
birds”
dual‐functional
hosts
for
both
sulfur
cathode
anode.
As
demonstrated,
d‐band
center
high‐spin
Fe
atom
captures
more
electrons
from
V
realize
π*
moderate
σ*
bond
electron
filling
orbital
occupation;
thus,
allowing
adsorption
intensity
polysulfides
effective
d–p
hybridization
improve
reaction
kinetics.
Meanwhile,
this
unique
structure
can
dynamically
balance
deposition
transport
on
anode;
thereby,
effectively
inhibiting
growth
promoting
formation
uniform
solid
electrolyte
interface.
as‐assembled
Li–S
full
batteries
exhibit
conspicuous
capacities
ultralong
cycling
lifespan
over
2000
cycles
at
5.0
C.
Even
higher
S
loading
(20
mg
cm
−2
)
lean
(2.5
µL
−1
),
cells
still
achieve
an
ultrahigh
areal
capacity
16.1
mAh
after
500
0.1
Abstract
The
notorious
lithium
polysulfides
(LiPSs)
shuttle
effect,
which
results
in
low
capacity,
subpar
rate
performance,
and
quick
capacity
deterioration,
has
severely
restricted
the
practical
applications
of
sulfur
(Li‐S)
batteries.
Therefore,
it
is
very
important
for
modified
materials
to
promote
thermodynamics
redox
kinetics
entrapping‐conversion
process
polysulfides.
Density
functional
theory
(DFT)
calculations
show
that
ferric
group
(Fe,
Co,
Ni)
transition
metals
not
only
provide
moderate
binding
contacts
with
LiPSs
but
also
act
as
an
active
catalyst
spontaneous
sequential
lithiation
S
8
Li
2
by
d‐band
energy
level
splitting,
migration
ions
can
be
operated
on
their
surface,
enhancing
utilization
LiPSs.
Experimentally,
felicitously‐fabricated
encapsulated
nitrogen‐doped
carbon
nanotubes
(M@NCNT)
electrocatalysts
were
introduced
into
Li‐S
batteries
via
separator
functionalization.
Actually,
experiments
demonstrated
excellent
effect
hindering
was
enabled.
Consistent
theoretical
predictions,
Ni@NCNT
separators
had
significantly
improved
cycling
stability.
cells
able
achieve
a
high
initial
discharge
1035
mAh
g
−1
retention
70%
at
500
discharges
1.0
C
0.060%
decay
each
cycle,
performing
considerable
cycle‐life
state‐of‐the‐art
separators.
Our
work
realistic
separator‐modified
strategy
splitting
from
high‐performance
long‐life
batteries,
further
propelling
battery
commercialization.
