Abstract
Lithium
metal
batteries
(LMBs)
are
highly
valued
due
to
their
high
energy
density.
However,
LMBs
severely
hindered
by
the
unstable
solid
electrolyte
interphase
(SEI),
which
requires
a
rational
design
of
interface
engineering.
Herein,
dual
protection
strategy
Li‐metal
anode
is
proposed
via
coating
black
phosphorus
(BP)
layer
on
separator.
During
battery
assembly
process,
few‐layer
BP
nanosheets
can
be
peeled
off
and
uniformly
modified
lithium
surface,
soft
metallic
properties
lithium,
meanwhile,
remaining
remains
separator,
so
that
they
provide
two
types
during
initial
formation
cycling
processes,
respectively.
lithiation,
stripped
converted
Li
3
P,
beneficial
component
for
stable
fast‐dynamic
SEI.
In
addition,
when
dendrites
dramatically
generated
under
extreme
conditions,
separator
melt
owing
activity
alloying
reaction.
Therefore,
BP‐modified
facilitates
large‐scale
application
metal,
with
generalisability
in
both
ester
ether
electrolytes.
electrolyte,
lifetimes
Li||Li
cells
prolonged
over
2200
h,
Li||LiFePO
4
exhibit
superior
capacity
retention
78%
after
500
cycles
at
1
C.
Metal
batteries
have
captured
significant
attention
for
high-energy
applications,
owing
to
their
superior
theoretical
energy
densities.
However,
practical
viability
is
impeded
by
severe
dendrite
formation
and
poor
cycling
stability.
To
alleviate
these
issues,
a
3D-structured
bimetallic-Mo2Ti2C3Tx
based
fiber
electrode
was
fabricated
in
this
study
analyzed
experimentally
computationally.
The
bimetallic
Mo–Ti
composition
of
MXenes
synergistically
achieved
low
binding
energies
with
lithium.
In
particular,
the
minimal
lattice
mismatch
between
deposited
Li
metal
Mo2Ti2C3Tx
MXene
anode
substrate
led
improved
respect
surface.
Moreover,
synergy
helped
amplify
ion
diffusion
reversible
charge
transfer.
Consequently,
exhibited
an
impressive
Coulombic
efficiency
(99.08%)
even
at
high
current
density
(5
mA
cm–2)
fixed
cutoff
capacity
1
h
cm–2
prolonged
cycle
life
(650
cycles).
This
report
highlights
promising
advancement
addressing
critical
challenges
facing
battery
operation,
thereby
offering
approach
improving
performance
applications.
Discontinuous
and
uneven
Li+
flux
leads
to
inhomogeneous
reactions,
accelerating
lithium
(Li)
dendrite
growth
reducing
the
utilization
of
active
materials,
which
severely
impacts
performance
metal
batteries
(LMBs).
To
address
this
challenge,
we
propose
an
effective
homogeneous
reaction
design
facilitated
by
all-aligned
nanofibrous
architecture,
establishes
continuous,
uniform,
rapid
pathways
throughout
battery.
This
enhances
diffusion
dynamics
ensures
a
uniform
distribution
current
density,
hence
promoting
Li
nucleation
at
anode
efficient
insertion/extraction
cathode.
Moreover,
architecture
exhibits
superior
mechanical
strength
flexibility,
maintaining
structural
stability
during
long-term
cycling
suppressing
growth,
thereby
minimizing
risk
short
circuits.
As
result,
LMBs
incorporating
exhibit
exceptional
electrochemical
performance.
work
provides
valuable
insights
into
reactions
for
high-performance
LMBs.
Angewandte Chemie International Edition,
Год журнала:
2024,
Номер
unknown
Опубликована: Окт. 29, 2024
Abstract
Designing
solid
polymer
electrolytes
(SPEs)
with
high
ionic
conductivity
for
room‐temperature
operation
is
essential
advancing
flexible
all‐solid‐state
energy
storage
devices.
Innovative
strategies
are
urgently
required
to
develop
SPEs
that
safe,
stable,
and
high‐performing.
In
this
work,
we
introduce
photoexcitation‐modulated
heterojunctions
as
catalytically
active
fillers
within
SPEs,
guided
by
photocatalytic
design
principles,
meanwhile
employ
natural
bacterial
cellulose
improve
the
compatibility
poly(ethylene
oxide),
coordination
environment
of
lithium
salts,
optimize
both
ion
transport
mechanical
properties.
situ
photothermal
experiments
theoretical
calculations
reveal
strong
photogenerated
electric
field
produced
trace
oxide)
under
photoexcitation
significantly
enhances
salt
dissociation,
increasing
concentration
mobile
Li
+
.
This
results
in
a
substantial
increase
conductivity,
reaching
0.135
mS
cm
−1
at
25
°C,
transference
number
0.46.
The
lithium‐metal
pouch
cells
exhibit
an
impressive
discharge
capacity
178.8
mAh
g
even
after
repeated
bending
folding,
demonstrate
exceptional
long‐term
cycling
stability,
retaining
86.7
%
their
initial
250
cycles
1
C
(25
°C).
research
offers
novel
approach
developing
high‐performance
batteries.
Angewandte Chemie International Edition,
Год журнала:
2025,
Номер
unknown
Опубликована: Янв. 31, 2025
Efficient
cycling
of
lithium
(Li)
metal
batteries
(LMBs)
under
extremely
high
current
conditions
is
critical
for
their
practical
applications.
Here,
we
report
a
novel
additive
containing
fluorine,
nitrogen,
and
iodine
elements
(designated
as
FCS)
to
stabilize
Li
anodes
in
glyme-based
ether
electrolytes
conditions.
Experimental
results
molecular
dynamics
(MD)
simulations
demonstrate
that
the
cation
FCS
selectively
adsorbs
on
electrode
surface,
optimizing
inner
Helmholtz
plane
(IHP)
structure
effectively
regulating
surface
electric
field,
thereby
promoting
homogeneous
deposition.
Simultaneously,
preferential
decomposition
produces
mechanically
robust
ionically
conductive
solid
electrolyte
interphase
(SEI)
comprising
LiF,
Li3N,
LiI
components.
Consequently,
with
additive,
Li||Cu
cells
remarkably
average
Coulombic
efficiency
(CE)
98.12
%
at
an
20
mA
cm-2
over
400
cycles.
Additionally,
Li||SPAN
maintain
reversible
capacity
1126
mAh
g-1
0.5
A
after
200
This
work
presents
new
approach
simultaneously
tune
SEI
using
trace
amounts
paving
way
stable
efficient
LMBs
high-current
