ACS Nano,
Journal Year:
2024,
Volume and Issue:
18(47), P. 32732 - 32745
Published: Nov. 11, 2024
Managing
the
redox
reactions
of
polysulfides
is
crucial
for
improving
performance
lithium-sulfur
batteries
(LSBs).
Herein,
we
introduce
a
progressive
theoretical
framework:
balanced
d-band
model,
which
based
on
classical
center
theory.
Specifically,
by
optimizing
position
in
middle
between
highest
occupied
molecular
orbital
(HOMO)
and
lowest
unoccupied
(LUMO)
each
sulfur
species,
fast
oxidation
reduction
species
can
be
achieved
simultaneously.
To
validate
this
theory,
synthesized
catalyst
featuring
an
situ
phosphorized
heterostructure
(NOP)
nickel
oxide
(NiO),
effectively
optimizes
at
HOMO
LUMO
species.
Aided
kinetics
NOP-based
cell
high
reversible
capacity,
superior
cycling
stability,
prolonged
cycle
life.
This
study
extends
conventional
theory
introduces
innovative
model
to
expand
our
understanding
internal
reaction
mechanisms
LSBs.
Chemical Reviews,
Journal Year:
2024,
Volume and Issue:
124(8), P. 4935 - 5118
Published: April 10, 2024
Rechargeable
metal-sulfur
batteries
are
considered
promising
candidates
for
energy
storage
due
to
their
high
density
along
with
natural
abundance
and
low
cost
of
raw
materials.
However,
they
could
not
yet
be
practically
implemented
several
key
challenges:
(i)
poor
conductivity
sulfur
the
discharge
product
metal
sulfide,
causing
sluggish
redox
kinetics,
(ii)
polysulfide
shuttling,
(iii)
parasitic
side
reactions
between
electrolyte
anode.
To
overcome
these
obstacles,
numerous
strategies
have
been
explored,
including
modifications
cathode,
anode,
electrolyte,
binder.
In
this
review,
fundamental
principles
challenges
first
discussed.
Second,
latest
research
on
is
presented
discussed,
covering
material
design,
synthesis
methods,
electrochemical
performances.
Third,
emerging
advanced
characterization
techniques
that
reveal
working
mechanisms
highlighted.
Finally,
possible
future
directions
practical
applications
This
comprehensive
review
aims
provide
experimental
theoretical
guidance
designing
understanding
intricacies
batteries;
thus,
it
can
illuminate
pathways
progressing
high-energy-density
battery
systems.
Advanced Functional Materials,
Journal Year:
2023,
Volume and Issue:
33(36)
Published: May 19, 2023
Abstract
Lithium–sulfur
(Li–S)
batteries
are
famous
for
their
high
energy
density
and
low
cost,
but
prevented
by
sluggish
redox
kinetics
of
sulfur
species
due
to
depressive
Li
ion
diffusion
kinetics,
especially
under
low‐temperature
environment.
Herein,
a
combined
strategy
electrocatalysis
pore
sieving
effect
is
put
forward
dissociate
the
+
solvation
structure
stimulate
free
diffusion,
further
improving
reaction
kinetics.
As
protocol,
an
electrocatalytic
porous
diffusion‐boosted
nitrogen‐doped
carbon‐grafted‐CoP
nanosheet
designed
via
forming
NCoP
active
release
more
react
with
species,
as
fully
investigated
electrochemical
tests,
theoretical
simulations
in
situ/ex
situ
characterizations.
result,
cells
booster
achieve
desirable
lifespan
800
cycles
at
2
C
excellent
rate
capability
(775
mAh
g
−1
3
C).
Impressively,
condition
mass
loading
or
environment,
cell
5.7
mg
cm
−2
stabilizes
areal
capacity
3.2
charming
647
obtained
0
°C
after
80
cycles,
demonstrating
promising
route
providing
ions
toward
practical
high‐energy
Li–S
batteries.
Advanced Functional Materials,
Journal Year:
2024,
Volume and Issue:
34(21)
Published: Jan. 29, 2024
Abstract
The
lithium‐sulfur
(Li‐S)
battery
stands
as
a
strong
contender
for
the
next‐generation
energy
storage
system,
characterized
by
abundant
sulfur
resources,
environmental
sustainability,
and
high
specific
capacity.
However,
its
density
remains
constrained
factors
such
low
loading
fraction
in
cathode,
excessive
electrolyte,
an
excess
of
anode.
These
mild
conditions
significantly
limit
Li‐S
batteries,
making
them
less
competitive.
To
achieve
higher
density,
harsh
operation
are
necessary,
but
these
remain
challenging
to
implement,
even
lab‐scale
production.
In
this
comprehensive
review,
emphasis
will
be
on
recent
advancements
specifically
realm
designing
loading,
fraction,
lean
limited
negative
electrode
batteries.
A
visualizable
model
that
illustrates
relationship
between
cell
various
parameters,
underscoring
importance
exploring
batteries
under
extreme
operating
further
development
is
provided.
Furthermore,
it
discussed
possibilities
achieving
challenges
need
addressed
make
practical
real‐world
applications.
Advanced Energy Materials,
Journal Year:
2024,
Volume and Issue:
14(25)
Published: April 5, 2024
Abstract
Lithium‐sulfur
(Li‐S)
batteries
are
considered
a
competitive
next‐generation
electrochemical
energy
storage
device,
while
the
shuttle
effect
of
soluble
lithium
polysulfides
(LiPSs)
resulting
from
sluggish
redox
kinetics
severely
impedes
their
practical
applications.
Herein,
novel
cation
doping
strategy
is
demonstrated
for
substantially
accelerating
sulfur
on
transition
metal
sulfide
(TMS)
electrocatalysts
by
partially
substituting
cobalt
atoms
with
in
situ
dissolved
Ni
dopants
(Ni
x
Co
3‐x
S
4
,
0<x≤1).
Theoretical
calculations
revealed
that
spinel
3
phase
enables
electronic‐state
modulation
active
sites
realizing
upshift
d‐orbital
center,
thus
leading
to
good
chemical
adsorption
intermediates
and
low
conversion
barriers
between
LiPSs
solid
Li
2
products.
This
confirmed
in‐depth
dynamics
Raman
characterizations,
which
obtained
0.5
2.5
hierarchical
nanosheet
structure
delivers
stronger
affinity
6
higher
precipitation/dissociation
capacity
comparison
monometallic
sulfides.
Benefiting
these
outstanding
attributes,
assembled
Li‐S
incorporating
into
S@carbon
nanotube
cathode
(S@Ni
/CNT)
exhibit
high
specific
1189
mAh
g
−1
excellent
rate
performance
596
at
5
C
long‐term
cycling
over
600
cycles
decay
0.06%
per
cycle
1
C.
More
importantly,
an
ultrahigh
reversible
areal
6.6
cm
−2
can
be
achieved
S@Ni
/CNT
even
loading
6.1
mg
.
work
demonstrates
new
insight
designing
TMS
toward
rapid
batteries.
Angewandte Chemie International Edition,
Journal Year:
2024,
Volume and Issue:
63(31)
Published: May 18, 2024
Lithium-sulfur
(Li-S)
batteries
have
many
advantages
but
still
face
problems
such
as
retarded
polysulfides
redox
kinetics
and
Li
dendrite
growth.
Most
reported
single
atom
catalysts
(SACs)
for
Li-S
are
based
on
d-band
transition
metals
whose
d
orbital
constitutes
active
valence
band,
which
is
inclined
to
occur
catalyst
passivation.
SACs
4f
inner
of
rare
earth
challenging
their
great
difficulty
be
activated.
In
this
work,
we
design
synthesize
the
first
metal
Sm
has
electron-rich
promote
catalytic
conversion
uniform
deposition
Li.
enhance
catalysis
by
activated
through
an
f-d-p
hybridization.
Using
Sm-N
ACS Applied Materials & Interfaces,
Journal Year:
2023,
Volume and Issue:
15(42), P. 49223 - 49232
Published: Oct. 15, 2023
Currently,
severe
shuttle
effects
and
sluggish
conversion
kinetics
are
the
main
obstacles
to
advancement
of
lithium-sulfur
(Li-S)
batteries.
Modification
battery
separator
by
a
catalyst
is
promising
approach
tackle
these
problems,
but
simultaneously
obtaining
rich
catalytic
active
sites,
high
conductivity,
remarkable
stability
remains
great
challenge.
Herein,
flower-like
MXene/MoS2/SnS@C
heterostructure
as
functional
intercalation
Li-S
batteries
was
prepared
for
accelerating
synergistic
adsorption-electrocatalysis
sulfur
conversion.
The
MXene
skeleton
constructs
three-dimensional
conductive
network
that
anchors
polysulfides
enhances
charge
transfer.
Meanwhile,
MoS2/SnS
has
sites
polysulfide
conversion,
leading
excellent
electrochemical
performances.
A
with
displays
an
extraordinary
capacity
836.1
mAh
g-1
over
200
cycles
at
0.5C
demonstrates
cycling
attenuation
approximately
0.051%
per
cycle
during
1000
2C.
When
loading
reaches
5.1
mg
cm-2,
still
maintains
722.4
50
cycles.
This
research
proposes
novel
strategy
design
stable
catalysts
extended
lifespan.
Advanced Materials,
Journal Year:
2023,
Volume and Issue:
36(9)
Published: Nov. 4, 2023
Abstract
Here,
a
strategy
to
strengthen
d–p
orbital
hybridization
by
fabricating
π
backbonding
in
the
catalyst
for
efficient
lithium
polysulfides
(LiPSs)
conversion
is
reported.
A
special
interface
structure
of
RuO
x
quantum
dots
(QDs)
anchored
on
graphdiyne
(GDY)
nanoboxes
(RuO
QDs/GDY)
prepared
enable
strong
Ru‐to‐alkyne
backdonation,
which
effectively
regulates
d‐electron
structures
Ru
centers
promote
between
and
LiPSs
significantly
boosts
catalytic
performance
QDs/GDY.
The
affinity
with
Li
ions
fast
Li‐ion
diffusion
QDs/GDY
also
ultrastable
metal
anodes.
Thus,
S@RuO
cathodes
exhibit
excellent
cycling
under
harsh
conditions,
Li@RuO
anodes
show
an
ultralong
life
over
8800
h
without
dendrite
growth.
Lithium‐sulfur
(Li–S)
full
cells
can
deliver
impressive
areal
capacity
17.8
mA
cm
−2
good
stability
practical
conditions
low
negative‐to‐positive
electrode
(N/P)
ratio
(N/P
=
1.4),
lean
electrolyte
(E/S
3
µL
mg
−1
),
high
S
mass
loading
(15.4
).
Advanced Functional Materials,
Journal Year:
2024,
Volume and Issue:
34(38)
Published: April 26, 2024
Abstract
The
applications
of
lithium
(Li)–sulfur
(S)
batteries
are
simultaneously
hampered
by
the
unlimited
dendritic
Li
growth
and
sluggish
redox
kinetics
polysulfides
(LiPSs).
In
this
work,
an
electronic
state‐modulated
Ni
4
N/Zn
3
N
2
heterogeneous
nanosheet
arrays
is
painstakingly
fabricated
on
surface
carbon
cloth
(CC@Ni
)
as
efficient
bi‐service
host
to
promote
uniform
deposition
boost
LiPSs
catalysis.
It
found
that
structure
heterostructure
modulated
realize
a
rational
transition
metal
d‐band
center,
its
built‐in
electric
field
(BIEF)
within
heterointerfaces
facilitates
interfacial
charge
transfer,
resulting
in
low
deposition/migration
energy
barrier
adsorption/catalytic
conversion
kinetics.
As
result,
as‐prepared
CC@Ni
‐Li
anode
can
enable
Li||Li
symmetrical
cells
possess
long‐term
lifespan
over
500
h
even
at
10
mA
cm
−2
/20
mAh
,
as‐assembled
LiNi
0.8
Co
0.1
Mn
O
||CC@Ni
full
cell
also
shows
excellent
cycling
performance
(95.8%
capacity
retention
after
100
cycles).
When
used
for
both
S
loading,
‐S||CC@Ni
exhibits
outstanding
stability
(744
g
−1
1000
cycles
2C).
This
work
highlights
great
potential
heterostructures
fabricating
ideal
bi‐serve
hosts
electrodes.