The
increasing
demand
for
high-energy-density
rechargeable
batteries
has
spurred
significant
advancements
in
lithium
(Li)
metal
employing
solid
polymer
electrolytes.
Extensive
efforts
have
been
devoted
to
tackling
the
crucial
shorting
problem
cycled
electrolytes
via
tuning
chemistries
and
polymer-metal
interfacial
properties.
However,
working
principles
of
these
designs
mainly
focus
on
physical/chemical
suppression,
instead
full
recovery
grown
dendrites.
Here,
we
propose
an
effective
gradient
design
by
introducing
Ga-based
liquid
(LM)
particles
with
a
depth-dependent
content,
enabling
Li
dendrites
spontaneous
alloying
reaction.
Such
asymmetric
electrolyte
configuration
is
capable
fully
chemically
upon
their
puncturing
into
LM-rich
layer,
while
inhibiting
electrical
percolation
at
LM-free
especially
under
mechanical
pressure
during
cell
assembly.
Post-mortem
analyses
reveal
structural
deformation
piercing
spherical
Li-LM
alloys,
thereby
preventing
even
extended
cycles.
Consequently,
ultrastable
cycling
stabilities
are
achieved
both
symmetric
cells
(>2000
h)
Li/LiFePO4
(>400
cycles;
average
CE
99.86%).
These
findings
not
only
exploit
dendrite
functionality
using
LM-based
but
also
highlight
potential
incorporating
various
battery
systems.
ABSTRACT
The
shift
toward
sustainable
energy
has
increased
the
demand
for
efficient
storage
systems
to
complement
renewable
sources
like
solar
and
wind.
While
lithium‐ion
batteries
dominate
market,
challenges
such
as
safety
concerns
limited
density
drive
search
new
solutions.
Liquid
metals
(LMs)
have
emerged
promising
materials
advanced
due
their
unique
properties,
including
low
melting
points,
high
electrical
conductivity,
tunable
surface
tension,
strong
alloying
tendency.
Enabled
by
properties
of
LMs,
four
key
scientific
functions
LMs
in
are
highlighted:
active
materials,
self‐healing,
interface
stabilization,
conductivity
enhancement.
These
applications
can
improve
battery
performance,
safety,
lifespan.
This
review
also
discusses
current
future
opportunities
using
next‐generation
systems.
image
Abstract
Separators
are
critical
components
of
zinc‐metal
batteries
(ZMBs).
Despite
their
high
ionic
conductivity
and
excellent
electrolyte
retention,
the
widely
used
glass
fiber
(GF)
membranes
suffer
from
poor
mechanical
stability
cannot
suppress
dendrite
growth,
leading
to
rapid
battery
failure.
Contrarily,
polymer‐based
separators
offer
superior
strength
facilitate
more
homogeneous
zinc
(Zn)
deposition.
However,
they
typically
sluggish
ion
transport
kinetics
wettability
by
aqueous
electrolytes,
resulting
in
unsatisfactory
electrochemical
performance.
Here
a
dehydroxylation
strategy
is
proposed
overcome
above‐mentioned
limitations
for
polyvinyl
alcohol
(PVA)
separators.
A
dehydroxylated
PVA‐based
membrane
(DHPVA)
synthesized
at
relatively
low
temperature
highly
concentrated
alkaline
solution.
Part
hydroxyl
groups
removed
and,
as
result,
hydrogen
bonding
between
PVA
chains,
which
deemed
responsible
kinetics,
minimized.
At
20
°C,
DHPVA
reaches
12.5
mS
cm
−1
,
almost
4
times
higher
than
that
PVA.
Additionally,
effectively
promotes
uniform
Zn
deposition,
significantly
extended
cycle
life
reduced
polarization,
both
a/symmetric
(Cu/Zn
Zn/Zn)
full
cells
(Zn/NaV
3
O
8
).
This
study
provides
new,
effective,
yet
simple
approach
improve
performance
ZMBs.
Abstract
Aqueous
zinc‐ion
batteries
have
emerged
as
promising
candidates
for
large‐scale
energy
storage,
but
their
cycle
stability
is
limited
by
irreversible
zinc
anodes
due
to
dendrite
growth
and
undesired
side
reactions.
Here,
an
artificial
composite
protective
layer
consisting
of
a
Zn
metal–organic
framework
(MOF)
infiltrated
with
hydrophobic
ionic
liquid
1‐ethyl‐3‐methylimidazoline
bis(trifluoromethyl
sulfonyl)
imide
constructed
on
anodes.
The
unique
porous
structure
the
MOF
enables
uniform
electric
field
distribution,
effectively
inducing
plating
stripping.
Meanwhile,
small
amount
can
isolate
direct
contact
between
anode
aqueous
electrolyte,
thereby
inhibiting
reactions
including
hydrogen
evolution
reaction.
In
addition,
cations
in
act
shielding
suppress
tip
effect.
Consequently,
metal
greatly
improved.
assembled
symmetric
cell
able
stably
over
2600
h
at
0.2
mA
cm
−2
/0.2
mAh
800
1
/1
,
which
also
exhibits
lower
more
stable
overpotentials.
Chemical Science,
Год журнала:
2025,
Номер
unknown
Опубликована: Янв. 1, 2025
To
regulate
interfacial
reactions
on
Zn
anode,
it
is
the
key
to
tune
dielectric
properties
of
interface
via
polarizability,
coordination,
and
solubility
anion.
Chemical Society Reviews,
Год журнала:
2025,
Номер
unknown
Опубликована: Янв. 1, 2025
This
review
explores
the
intrinsic
connection
between
structural
features
of
different
organic
electrode
materials
and
their
charge
storage
performance,
aiming
to
unveil
key
design
principles
for
molecules
used
in
various
multivalent
metal
battery
applications.
