The
rapid
catalytic
conversion
toward
polysulfides
is
considered
to
be
an
advantageous
approach
boost
the
reaction
kinetics
and
inhibit
shuttle
effect
in
lithium-sulfur
(Li─S)
batteries.
However,
prediction
of
high
activity
Li─S
catalysts
has
become
challenging
given
carelessness
relationship
between
important
electronic
characteristics
activity.
Herein,
relationships
D-band
regulation
with
are
described.
Through
combination
experimental
theoretical
analysis,
opportune
upward
shift
center
results
a
favorable
interaction
polysulfides,
controlling
adsorption
behavior
polysulfides.
In
addition,
electron
achieved
by
moderately
moving
up
further
reduces
energy
barrier
through
hybridization
Based
on
this,
composite
catalyst
Mo
doped
VS
Suppressing
the
lithium
polysulfide
(LiPS)
shuttling
as
well
accelerating
conversion
kinetics
is
extremely
crucial
yet
challenging
in
designing
sulfur
hosts
for
lithium–sulfur
(Li–S)
batteries.
Phase
engineering
of
nanomaterials
an
intriguing
approach
tuning
electronic
structure
toward
regulating
phase-dependent
physicochemical
properties.
In
this
study,
a
metastable
phase
δ-Mo2C
catalyst
was
elaborately
synthesized
via
boron
doping
strategy,
which
exhibited
transfer
from
hexagonal
to
cubic
structure.
The
hierarchical
tubular
δ-Mo2C-decorated
N-doped
carbon
nanotube
(δ-B-Mo2C/NCNT)
endows
fast
electron
and
abundant
polar
sites
LiPSs.
First-principles
calculations
reveal
strengthened
chemical
adsorption
capability
hybridization
between
d
orbital
Mo
metal
p
S
atoms
LiPSs,
contributing
higher
electrocatalytic
activity.
Moreover,
situ
Raman
analysis
manifests
accelerated
redox
kinetics.
Consequently,
δ-B-Mo2C/NCNT
renders
Li–S
battery
with
high
specific
capacity
1385.6
mAh
g–1
at
0.1
C
superior
rate
property
606.3
4
C.
Impressively,
satisfactory
areal
6.95
cm–2
achieved
under
loading
6.8
mg
cm–2.
This
work
has
gained
research
significance
design
Advanced Functional Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Март 27, 2025
Abstract
In
recent
years,
secondary
batteries
have
emerged
as
a
hot
research
area,
with
electrodes
being
one
of
the
key
components
that
significantly
impact
battery
performance.
However,
traditional
coating‐type
electrode
sheets,
which
limitations
in
terms
energy
and
power
density,
can
no
longer
satisfy
current
demands
for
batteries.
3D
printing
technology,
known
its
low
cost,
simple
operation,
rapid
prototyping,
ease
customization,
has
garnered
widespread
attention.
By
applying
technology
to
optimizing
their
structure
design,
it
is
possible
create
more
active
sites
ion/charge
transport
channels,
thereby
enhancing
electrochemical
performance
Herein,
this
paper
reviews
currently
commonly
used
storage
technologies
standards
ink
formulation.
A
variety
representative
printed
structures
optimization
strategies
are
also
listed.
addition,
materials
use,
ranging
from
0D
3D,
covered,
including
synthesis
methods,
morphology,
contributions
It
anticipated
review
will
provide
valuable
insights
into
rapidly
developing
field.
Abstract
Lithium‐sulfur
(Li–S)
batteries
have
heretofore
raised
burgeoning
interest
due
to
their
cost
effectiveness
and
high
theoretical
energy
densities.
However,
the
inherent
porous
fluffy
structure
of
sulfur
impedes
path
constructing
high‐loading
electrodes
(over
5
mg
cm
−2
)
for
practicability.
Furthermore,
especially
in
thick
electrodes,
challenges
like
retarded
redox
kinetics,
notorious
polysulfide
shuttling,
wanton
electrode
expansion
seriously
give
rise
low
utilization,
poor
rate
performance,
unsatisfactory
cycling
stability.
Constructing
free‐standing
architectures
has
been
demonstrated
as
an
effective
strategy
tackle
aforementioned
issues
Li–S
batteries.
As
emerging
technique,
3D
printing
(3DP)
shows
merits
rapidly
fabricating
precise
microstructures
with
controllable
loadings
rationally
organized
porosity.
For
realm,
3DP
offers
optimized
Li
+
/e
−
transmission
well‐dispersed
electrocatalysts,
which
achieves
efficient
regulation
guarantees
favorable
performance.
This
review
covers
design
principle
preparation
printable
inks,
practical
applications
manufacture
self‐supported
frameworks
(such
cathodes,
anodes,
separators)
Challenges
perspectives
on
potential
future
development
are
also
outlined.
Chemical Communications,
Год журнала:
2025,
Номер
unknown
Опубликована: Янв. 1, 2025
Ammonium
molybdenum
sulfide
hydrate
(N-MoS
x
)
nanospheres
with
a
dual
mechanism
of
Zn
2+
insertion/de-insertion
and
the
breakage/formation
disulfide
bonds
are
reported.
Advanced Energy Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Апрель 18, 2025
Abstract
The
development
of
lithium–sulfur
batteries
is
impeded
by
their
suboptimal
electrochemical
performance
and
significant
self‐discharge
under
practical
conditions,
especially
at
high
sulfur‐to‐host
ratios
low
electrolyte‐to‐sulfur
ratios.
Under
these
improving
necessitates
accelerating
the
polysulfides
conversion,
while
reducing
entails
inhibiting
same
conversion
(disproportionation
reaction,
a
key
contributor
to
self‐discharge).
Herein,
address
this
challenging
contradiction,
an
imprisoning
strategy
designed
that
utilizes
programmable
solid
electrolyte
interphase
(SEI)
layers
formed
only
on
outer
surface
TiO
2−x
coated
hollow
carbon
spheres
(TiO
@C).
@C
chosen
primarily
because
it
supports
regulated
SEI
growth
upon
simple
voltage
control,
leveraging
different
formation
potential
C,
its
conductivity
catalytic
property
ensure
sulfur
reaction
kinetics.
This
functions
effectively
even
conditions.
exposed
internal
provides
abundant
effective
sites
(as
dense
barrier)
prevents
from
migrating
out
spheres,
performance.
These
soluble
polysulfides,
being
confined
within
easily
reach
saturation
concentrations
during
storage,
disproportionation
reaction.
Consequently,
wrapped
@C/sulfur
cathodes
exhibit
both
self‐discharge.
work
new
attempt
achieve
above
simultaneous
optimization
without
compromise.
Enhancing
the
catalytic
activity
of
sulfur
cathode
hosts
is
critical
for
suppressing
shuttle
effect
and
accelerating
polysulfides
redox
kinetics
in
lithium-sulfur
(Li-S)
batteries.
However,
efficient
polysulfide
adsorption
catalysis
conversion
rely
on
synergistic
interactions
between
catalyst
supporting
carrier,
particularly
optimizing
site
density
electron/ion
transport
rates.
Herein,
we
modulate
carrier-catalyst
heterointerface
to
enhance
conversion.
Metallic
1T-phase
MoS2
nanospheres
are
uniformly
dispersed
onto
nitrogen-doped
graphene
(N-G)
sheets,
forming
a
composite
host
material
(1T-MoS2/N-G)
Li-S
N-G
serves
as
both
conductive
substrate
charge
transfer
support
loading,
while
1T-MoS2,
rich
sites,
functions
an
electrocatalyst,
promoting
ion
diffusion,
adsorbing
soluble
polysulfides,
their
transformation
into
solid
lithium
sulfide.
Benefiting
from
these
structural
advantages,
S/1T-MoS2/N-G
exhibits
initial
capacity
1,296.8
mAh
g-1
at
0.2
C
demonstrates
outstanding
cycle
stabilization,
with
decay
rate
only
0.015%
per
over
500
cycles
1.0
C.
Even
under
demanding
conditions,
such
loading
6.5
mg
cm-2
lean
electrolyte
7
µL
mg-1,
provides
areal
7.2
retains
4.8
after
100
cycles.
These
findings
offer
new
insights
design
advanced
materials
high-performance
cathodes
broader
electrocatalytic
applications.