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.
Advanced Functional Materials,
Journal Year:
2024,
Volume and Issue:
unknown
Published: June 21, 2024
Abstract
Transition
metal
selenides
(TMSes)
are
considered
promising
candidates
for
the
anodes
of
sodium‐ion
batteries
(SIBs)
due
to
their
substantial
theoretical
capacity.
However,
TMSes
still
face
with
inferior
cycling
lifespan
caused
by
sluggish
Na
+
diffusion
kinetics
and
vigorous
volume
variations
during
dis/charge
processes.
Engineering
heterostructure
is
an
attractive
solution
rapid
transfer,
introducing
carbonaceous
materials
also
facilitates
enhanced
conductivity
structural
stability.
Herein,
CoSe/MoSe
2
combined
homogeneous
carbon
composites
rational
designed.
The
kinetic
analysis
calculations
verified
that
heterointerface
engineering
induced
build‐in
electric
field
effect
can
amplifies
kinetics,
while
contributes
electrical
Expectedly,
‐C
exhibits
high
capacity
extremely
ultra‐long
(320.9
mAh
g
−1
at
2.0
A
over
10,000
cycles
average
decay
only
0.01781
per
cycle).
Furthermore,
in
situ
X‐ray
diffraction
(XRD),
ex
photoelectorn
(XPS),
high‐resolution
electron
microscopy
(HRTEM)
exploited
explore
storage
mechanism.
In
addition,
3
V
(PO
4
)
@rGO//CoSe/MoSe
(NVP@rGO//CoSe/MoSe
‐C)
pouch‐type
full‐cells
successfully
assembled
delivered
satisfactory
performance.
This
research
presents
a
viable
strategy
targeted
aimed
enhancing
efficiency
SIBs.
Angewandte Chemie International Edition,
Journal Year:
2024,
Volume and Issue:
63(35)
Published: June 13, 2024
Abstract
The
inevitable
shuttling
and
slow
redox
kinetics
of
lithium
polysulfides
(LiPSs)
as
well
the
uncontrolled
growth
Li
dendrites
have
strongly
limited
practical
applications
lithium‐sulfur
batteries
(LSBs).
To
address
these
issues,
we
innovatively
constructed
carbon
nanotubes
(CNTs)
encapsulated
Co
nanoparticles
in
situ
grown
on
TiN‐MXene
nanosheets,
denoted
TiN‐MXene‐Co@CNTs,
which
could
serve
simultaneously
both
sulfur/Li
host
to
kill
“three
birds
with
one
stone”
(1)
efficiently
capture
soluble
LiPSs
expedite
their
conversion,
(2)
accelerate
nucleation/decomposition
solid
2
S,
(3)
induce
homogeneous
deposition.
Benefiting
from
synergistic
effects,
TiN‐MXene‐Co@CNTs/S
cathode
a
sulfur
loading
2.5
mg
cm
−2
show
high
reversible
specific
capacity
1129.1
mAh
g
−1
after
100
cycles
at
0.1
C,
ultralong
cycle
life
over
1000
1.0
C.
More
importantly,
it
even
achieves
areal
6.3
50
under
8.9
low
E/S
ratio
5.0
μL
.
Besides,
TiN‐MXene‐Co@CNTs
deliver
stable
plating/striping
behavior
h.
ACS Nano,
Journal Year:
2024,
Volume and Issue:
18(12), P. 8839 - 8852
Published: March 11, 2024
Catalytic
conversion
of
polysulfides
emerges
as
a
promising
approach
to
improve
the
kinetics
and
mitigate
polysulfide
shuttling
in
lithium–sulfur
(Li–S)
batteries,
especially
under
conditions
high
sulfur
loading
lean
electrolyte.
Herein,
we
present
separator
architecture
that
incorporates
double-terminal
binding
(DTB)
sites
within
nitrogen-doped
carbon
framework,
consisting
polar
Co0.85Se
Co
clusters
(Co/Co0.85Se@NC),
enhance
durability
Li–S
batteries.
The
uniformly
dispersed
offer
abundant
active
for
lithium
(LiPSs),
enabling
efficient
LiPS
while
also
serving
anchors
through
combination
chemical
interactions.
Density
functional
theory
calculations,
along
with
situ
Raman
X-ray
diffraction
characterizations,
reveal
DTB
effect
strengthens
energy
lowers
barriers
redox
reactions.
batteries
utilizing
Co/Co0.85Se@NC-modified
demonstrate
exceptional
cycling
stability
(0.042%
per
cycle
over
1000
cycles
at
2
C)
rate
capability
(849
mAh
g–1
3
C),
well
deliver
an
impressive
areal
capacity
10.0
cm–2
even
challenging
(10.7
mg
cm–2)
electrolyte
environments
(5.8
μL
mg–1).
site
strategy
offers
valuable
insights
into
development
high-performance
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
Advanced Materials,
Journal Year:
2024,
Volume and Issue:
unknown
Published: Oct. 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.
Energy & Environmental Science,
Journal Year:
2024,
Volume and Issue:
unknown
Published: Jan. 1, 2024
The
high-entropy
TiVNbMoC
3
MXene,
with
its
atom-dominated
relay
catalysis
effect
and
resilient
lattice
configuration,
promotes
a
cascade
of
sulfur
conversions
guides
uniform
Li
+
deposition,
enabling
shuttle-free
dendrite-free
Li–S
batteries.
Small,
Journal Year:
2024,
Volume and Issue:
20(44)
Published: July 6, 2024
The
conductive
carbon-based
interlayer,
as
the
secondary
current
collector
in
self-dissolving
battery
system,
can
effectively
capture
escaping
cathode
active
materials,
inducing
deep
release
of
remaining
capacity.
In
multi-step
reactions
Li─S
batteries,
environmental
tolerance
interlayer
to
polysulfides
determines
inhibition
shuttle
effects.
Here,
a
modified
metal-organic
framework
(Mn-ZIF67)
is
utilized
obtain
nitrogen-doped
carbon-coated
heterogeneous
Co-MnO
(Co-MnO@NC)
with
dual
catalytic
center
for
functional
materials.
synergistic
coupling
mechanism
NC
and
achieves
rapid
deposition
conversion
free
polysulfide
fragmented
sulfur
on
collector,
reducing
capacity
loss
cathode.
Co-MnO@NC/PP
separator
maintains
an
initial
1050
mAh
g
Journal of Materials Chemistry A,
Journal Year:
2024,
Volume and Issue:
12(33), P. 21845 - 21852
Published: Jan. 1, 2024
The
cathode
kinetics
promotion
effectiveness
of
electrocatalysts
is
evaluated
in
lean-electrolyte
lithium–sulfur
batteries.
improvement
polysulfide
conversion
and
battery
performance
more
significant
at
higher
sulfur
concentration.
Advanced Functional Materials,
Journal Year:
2024,
Volume and Issue:
34(44)
Published: July 17, 2024
Abstract
Lithium‐sulfur
batteries
(LSBs)
have
become
one
of
the
most
powerful
candidates
for
next‐generation
battery
technologies
due
to
their
high
theoretical
energy
density
and
low
cost.
However,
notorious
shuttle
effect
soluble
lithium
polysulfides
(LiPSs)
sluggish
conversion
reaction
kinetics
cause
sulfur
utilization
inferior
cycle
life.
Rational
catalyst
design
on
hierarchical
pore
structures
composition
optimization
is
highly
desired
realize
synergetic
enrichment,
accommodation,
catalytic
redox
capacity
species.
In
this
consideration,
hollow
porous
N‐doped
carbon
framework
prepared,
in
which
Co
nanoparticles
(NPs)
are
evenly
embedded
(denoted
as
Co‐HMCF)
modulate
electron
cloud
carbons.
Electrochemical
tests
functional
theory
(DFT)
calculations
demonstrate
that
Co‐HMCF
could
simultaneously
deliver
superior
activity
accelerating
LiPSs
well
Li
2
S
nucleation/decomposition
improve
overall
kinetics.
Consequently,
interlayer
significantly
improves
performance,
including
discharge
output
(1538
mAh
g
−1
at
0.2
C),
stable
long‐term
(0.047%
decay
per
800
cycles
1.0
exceptional
rate
(582
5.0
C).
