Abstract
The
cyclic
stability
of
aqueous
zinc‐manganese
batteries
(ZMBs)
is
greatly
restricted
by
the
side
reaction
anode
and
irreversibility
cathode.
In
this
work,
a
solid‐liquid
hybrid
electrolyte
mixing
traditional
ZnSO
4
‐based
diatomite
(denoted
as
Dtm)
proposed
that
exhibits
good
compatibility
reversibility
in
both
interface
cathode
interface.
abundant
hydroxyl
groups
at
disturb
hydrogen
bond
network
water
molecule,
which
weakens
corrosion
active
to
Zn
anode.
Moreover,
negatively
charged
surface
able
regulate
electric
field
promote
uniform
deposition
ion
well
inhibit
formation
sulfate
(ZHS)
As
result,
Zn||Zn
symmetric
battery
with
Dtm
achieves
stable
cycling
for
2500
h
1
mA
cm
−2
/1
mAh
,
while
Zn||MnO
2
can
achieve
cycle
time
500
cycles
current
densities
0.2
0.5
A
g
−1
capacities
228
177.6
respectively.
provides
new
ideas
screening
high‐performance
ZMBs.
Advanced Functional Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Март 2, 2025
Abstract
Interface
issues
such
as
parasitic
reactions
and
dendrite
growth
have
long
been
major
obstacles
hindering
the
longevity
of
aqueous
zinc‐ion
batteries
(AZIBs).
The
quest
for
more
effective
strategies
to
regulate
highly
active
interface
remains
a
focal
point
in
AZIBs.
Herein,
novel
interface‐targeted
additive
N‐Acetoacetylmorpholine
(NHM)
is
introduced,
by
lowering
interfacial
tension
modifying
electrical
double
layer,
improve
performance
This
reconfiguration
results
H
2
O‐poor
inner
Helmholtz
plane,
which
suppresses
reactions,
accelerates
kinetics,
fosters
uniform
zinc
deposition.
Consequently,
anode
demonstrates
impressive
cycling
durability,
exceeding
3800
h
plating/stripping
process
400
steady
cycle
at
high
depth
discharge
(DOD)
60%.
Zn/NH
4
V
O
10
full
cell
superior
performance,
achieving
80%
capacity
retention
after
1500
cycles.
Moreover,
pouch
cells
with
highloading
cathodes
(13.5
mg
cm
−2
)
can
maintain
70%
300
cycles
0.5
A
g
−1
.
controlled
N/P
ratio
(2.63:1)
shows
excellent
stability
130
These
findings
provide
valuable
insights
into
design
offer
promising
enhancing
practicality
Advanced Functional Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Фев. 18, 2025
Abstract
Revealing
interlayer
oxygen
charge
is
of
great
significance
in
understanding
the
high‐voltage
and
air
stability
sodium
layered
cathodes,
but
it
currently
lacks
attention.
Particularly,
ion
full
batteries
under
high
cathode
loading
(≥8
mg
cm
−2
)
also
faces
extremely
challenges.
Here,
its
mechanism
for
are
revealed
a
high‐entropy
O3‐Na
0.85
Li
0.1
Al
0.02
Sn
0.08
Cu
Ti
Ni
0.3
Mn
O
2
(HEO)
cathode,
which
enables
robust
high‐cathode‐loading
sodium‐ion
batteries.
The
doping
effectively
maintains
transition
metal
(TM)─O
bond
covalency,
stabilizing
charge.
stable
O─O
repulsion
avoids
structural
collapse,
realizing
P3‐OP2‐P3
reversible
phase
transition.
Moreover,
reduced
achieves
Na
layer
contraction
Na─O
enhancement.
These
features
inhibit
attack
water
loss,
well
stability.
Therefore,
HEO
exhibits
good
up
to
900
cycles
2.0‒4.3
V
high‐capacity
retention
96.12%
after
5
day
exposure.
pouch
cell
with
≈16
≈60
mAh
lasts
100
cycles.
This
work
contributes
new
insights
into
both
cathodes
practical
Aqueous
batteries,
renowned
for
their
high
capacity,
safety,
and
low
cost,
have
emerged
as
promising
candidates
next-generation,
sustainable
energy
storage.
However,
large-scale
application
is
hindered
by
challenges,
such
dendrite
formation
side
reactions
at
the
anode.
Hydrogel
electrolytes,
which
integrate
advantages
of
liquid
solid
phases,
exhibit
superior
ionic
conductivity
interfacial
compatibility,
giving
them
potential
to
suppress
evolution.
This
Perspective
first
briefly
introduces
fundamentals
underlying
unique
features
hydrogels.
It
then
identifies
key
role
water
polymer
networks
in
inhibiting
formation,
highlighting
regulation
activity,
ion
transport,
electrode
kinetics.
By
elucidating
principles
hydrogels
suppression,
this
work
aims
provide
valuable
insights
advance
implementation
aqueous
batteries
incorporating
The
longevity
of
aqueous
batteries
after
scaling
up
is
largely
restricted
by
metal
anodes
(Zn,
Al,
and
Mg).
Parasitic
reactions
uncontrolled
dendrites
dominate
failure
modes,
especially
at
high
current
densities.
To
fully
improve
its
reversibility,
tailored
surface
chemistry
well-designed
ion
transport
channels
are
simultaneously
demanded.
Here,
inspired
the
reticulated
structure
sea
urchin
shell,
an
aligned
porous
coating
assembled
from
graphene
oxide
sodium
alginate
anchored
on
zinc
anodes,
termed
a
unidirectional
sieve.
As
revealed
multiscale
modeling
tests,
this
biomimetic
layer
produces
area,
creating
low-tortuosity
that
greatly
enhance
kinetics
uniform
distribution
ions.
introduction
ion-conductive
natural
polymer
enables
well-tuned
hydration
selectivity,
alleviating
side
reactions.
With
structural-functional
integrity
design,
decorated
symmetrical
cell
presents
reversible
cycling
for
1600
h,
with
reduced
nucleation
potential
21
mV
Coulombic
efficiency.
Aided
Distribution
Relaxation
Time
tool,
different
electrochemical
processes
deconvoluted
to
understand
respective
mechanisms,
thereby
providing
referable
strategy
product
scaling.
In
end,
7Ah
Zn||VO2
pouch
demonstrates
stable
over
500
cycles
1
A·g-1,
capacity
retention
90%.
Abstract
The
practical
application
of
aqueous
zinc‐ion
batteries
(AZIBs)
is
impeded
by
dendrite
formation
and
water‐induced
parasitic
reactions
at
the
anodes.
In
this
article,
a
relatively
hydrophobic
inner
Helmholtz
plane
(IHP)
an
outer
(OHP)
with
abundant
nucleation
sites
are
engineered
through
coating
N,
F,
P
heteroatom
doped
reduced
graphene
oxide/carbon
nanotube
(NFP‐rGO‐CNT)
multifunctional
aerogel
protective
layer.
rGO
certain
hydrophobicity
construct
lean‐water
environment
IHP,
effectively
blocking
adverse
between
water
metallic
Zn,
while
zincophilic
uniformly
distributed
heteroatoms
facilitate
Zn
2+
migration
homogenize
flux
OHP,
thereby
promoting
directional
deposition
along
(002)
crystal
plane.
Consequently,
fabricated
NFP‐rGO‐CNT/Zn//Cu
asymmetric
cell
exhibits
high
Coulombic
efficiency
close
to
100%
for
3200
cycles.
addition,
symmetric
assembled
NFP‐rGO‐CNT/Zn
electrodes
presents
impressive
lifespan
1990
h
5
mA
cm
−2
2
mAh
,
significantly
outperforming
control
group
(about
27
h).
More
remarkably,
NFP‐rGO‐CNT/Zn//V
O
3
pseudo‐pouch
capable
powering
small
fan
rotate
steadily.
This
layer
strategy
offers
novel
perspective
HP
regulation,
enabling
textured
reversible
Nano-Micro Letters,
Год журнала:
2025,
Номер
17(1)
Опубликована: Май 19, 2025
Abstract
Crystallographic
engineering
of
Zn
anodes
to
favor
the
exposure
(002)
planes
is
an
effective
approach
for
improving
stability
in
aqueous
electrolytes.
However,
achieving
non-epitaxial
electrodeposition
with
a
pronounced
texture
and
maintaining
this
orientation
during
extended
cycling
remains
challenging.
This
study
questions
prevailing
notion
that
single
(002)-textured
anode
inherently
ensures
superior
stability,
showing
such
cannot
sustain
their
ZnSO
4
We
then
introduced
novel
electrolyte
additive,
benzyltriethylammonium
chloride
(TEBAC),
which
preserves
over
prolonged
cycling.
Furthermore,
we
successfully
converted
commercial
foils
into
highly
crystalline
without
any
pretreatment.
Experiments
theoretical
calculations
revealed
cationic
TEBA
+
selectively
adsorbs
onto
surface,
promoting
Zn(002)
plane
suppressing
dendrite
formation.
A
critical
discovery
was
pitting
corrosion
caused
by
ions
from
TEBAC,
mitigated
anion
substitution.
modification
leads
remarkable
lifespan
375
days
Zn||Zn
symmetric
cells
at
1
mA
cm
−2
mAh
.
-modified
Zn||VO
2
full
cell
demonstrates
high
specific
capacity
robust
cycle
10.0
g
−1
These
results
provide
valuable
insights
strategies
developing
long-life
ion
batteries.