Abstract
Application
of
an
aqueous
Zn‐ion
battery
is
plagued
by
a
water‐induced
hydrogen
evolution
reaction
(HER),
resulting
in
local
pH
variations
and
unstable
electrode–electrolyte
interface
(EEI)
with
uncontrolled
Zn
plating
side
reactions.
Here,
4‐methyl
pyridine
N‐oxide
(PNO)
introduced
as
redox
non‐innocent
additive
that
comprises
hydrophilic
bipolar
N
+
–O
−
ion
pair
coordinating
ligand
for
hydrophobic
─CH
3
group
at
the
para
position
ring
reduces
water
activity
EEI,
thereby
enhancing
stability.
The
moiety
PNO
possesses
unique
functionality
efficient
push
electron
donor
pull
acceptor,
thus
maintaining
desired
during
charging/discharging.
Intriguingly,
replacing
(electron
pushing
+I
effect)
─CF
pulling
─I
effect),
however,
does
not
improve
reversibility;
instead,
it
degrades
cell
performance.
electrolyte
2
m
ZnSO
4
15
enables
symmetric
plating/stripping
remarkable
>
10
000
h
0.5
mA
cm
−2
exhibits
coulombic
efficiency
(CE)
≈99.61%
0.8
Zn/Cu
asymmetric
cell.
This
work
showcases
immense
interplay
push–pull
additives
on
cycling.
Advanced Functional Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Фев. 12, 2025
Abstract
Despite
the
conspicuous
merits
of
Zn
metal
anodes,
commercialization
anode‐based
electrochemical
energy
storage
devices
is
still
constrained
by
uncontrollable
dendrite
growth
and
serious
parasitic
reactions.
Herein,
an
innovative
strategy
employing
kosmotropic
anions‐intensified
proline
additive
to
regulate
2+
solvation
structure
manipulate
deposition
interface,
thus
achieving
highly
stable
proposed.
The
key
this
lies
in
ingeniously
utilizing
SO
4
2−
anions
enhance
affinity
adsorption
layer
on
anodes
weaken
.
Consequently,
proline‐containing
ZnSO
(ZnSO
‐proline)
electrolyte
deliver
a
remarkable
lifespan
over
2600
h
at
1.0
mA
cm
−2
mAh
Even
under
harsh
plating/stripping
condition
(10
10
),
‐proline
stably
operate
for
650
h.
Meanwhile,
Coulombic
efficiency
designed
as
high
99.9%
1100
cycles.
endows
Zn‐ion
batteries
hybrid
capacitors
with
notably
optimized
long‐term
cycling
stability.
This
work
expected
be
immediate
benefit
design
low‐cost
Zn‐based
systems
ultra‐long
lifespan.
Abstract
This
work
highlights
the
development
of
a
superior
cathode|electrolyte
interface
for
quasi
solid‐state
rechargeable
zinc
metal
battery
(QSS‐RZMB)
by
novel
hydrogel
polymer
electrolyte
using
an
ultraviolet
(UV)
light‐assisted
in
situ
polymerization
strategy.
By
integrating
cathode
with
thin
layer
electrolyte,
this
technique
produces
integrated
that
ensures
quick
Zn
2+
ion
conduction.
The
coexistence
nanowires
direct
electron
routes
and
enhanced
infiltration
diffusion
3D
porous
flower
structure
wide
open
surface
Zn‐MnO
electrode
complements
formation
during
process.
QSS‐RZMB
configured
(i‐Zn‐MnO)
(PHPZ‐30)
as
separator
yields
comparable
specific
energy
density
214.14
Wh
kg
−1
its
liquid
counterpart
(240.38
,
0.5
M
Zn(CF
3
SO
)
2
aqueous
electrolyte).
Other
noteworthy
features
presented
system
include
cycle
life
over
1000
charge‐discharge
cycles
85%
capacity
retention
99%
coulombic
efficiency
at
current
1.0
A
g
compared
to
only
60%
500
displayed
liquid‐state
under
same
operating
conditions.
Abstract
Aqueous
Zn
metal
batteries
are
attracting
tremendous
interest
as
promising
energy
storage
systems
due
to
their
intrinsic
safety
and
cost‐effectiveness.
Nevertheless,
the
reversibility
of
anodes
(ZMAs)
is
hindered
by
water‐induced
parasitic
reactions
dendrite
growth.
Herein,
a
novel
hydrated
eutectic
electrolyte
(HEE)
consisting
Zn(BF
4
)
2
·xH
O
sulfolane
(SL)
developed
prevent
side
achieve
outstanding
cyclability
ZMAs.
The
strong
coordination
between
2+
SL
triggers
feature,
enabling
low‐temperature
availability
HEEs.
restriction
BF
−
hydrolysis
in
system
can
realize
favorable
compatibility
‐based
Besides,
newly‐established
solvation
structure
with
participation
SL,
H
O,
,
induce
situ
formation
desirable
SEI
gradient
B,O‐rich
species,
ZnS,
ZnF
offer
satisfactory
protection
toward
Consequently,
HEE
allows
Zn||Zn
symmetric
cell
cycle
over
1650
h
at
mA
cm
−2
1
.
Moreover,
Zn||NH
V
10
full
deliver
prolonged
lifespan
for
1000
cycles
high
capacity
retention
83.4%.
This
work
represents
feasible
approach
elaborate
design
advanced
next‐generation
batteries.
Dendrite
growth
limits
the
lifespan
of
aqueous
zinc-ion
batteries
(AZIBs).
The
tellurium
complex
treatment
forms
a
layer
on
zinc
anode,
suppressing
dendrite
growth.
This
enables
long-term
stable
and
high-performance
AZIBs.
Automating
electrochemical
analyses
combined
with
artificial
intelligence
is
poised
to
accelerate
discoveries
in
renewable
energy
sciences
and
technologies.
This
study
presents
an
automated
high-throughput
characterization
(AHTech)
platform
as
a
cost-effective
versatile
tool
for
rapidly
assessing
liquid
analytes.
The
Python-controlled
combines
handling
robot,
potentiostat,
customizable
microelectrode
bundles
diverse,
reproducible
measurements
microtiter
plates,
minimizing
chemical
consumption
manual
effort.
To
showcase
the
capability
of
AHTech,
we
screened
library
180
small
molecules
electrolyte
additives
aqueous
zinc
metal
batteries,
generating
data
training
machine
learning
models
predict
Coulombic
efficiencies.
Key
molecular
features
governing
additive
performance
were
elucidated
using
Shapley
Additive
exPlanations
Spearman’s
correlation,
pinpointing
high-performance
candidates
like
cis
-4-hydroxy-
d
-proline,
which
achieved
average
efficiency
99.52%
over
200
cycles.
workflow
established
herein
highly
adaptable,
offering
powerful
framework
accelerating
exploration
optimization
extensive
spaces
across
diverse
storage
conversion
fields.
Abstract
Stabilizing
the
Zn
anode/electrolyte
interface
is
critical
for
advancing
aqueous
zinc
ion
storage
technologies.
Addressing
this
challenge
helps
minimize
parasitic
reactions
and
controls
formation
of
dendrites,
which
fundamental
to
achieving
highly
reversible
electrochemistry.
In
study,
2%
by
volume
dimethyl
sulfoxide
(DMSO)
introduced
into
baseline
sulfate
(ZS)
electrolyte,
acts
as
an
efficient
regulator
form
a
robust
solid–electrolyte
interphase
(SEI)
on
anode.
This
innovative
approach
enables
uniform
deposition
does
not
substantially
modify
2+
solvation
structure.
The
Zn||Zn
symmetric
cell
exhibits
extended
cycle
life
nearly
one
calendar
year
(>8500
h)
at
current
density
0.5
mA
cm
−2
areal
capacity
mAh
.
Impressive
full
performance
can
be
achieved.
Specifically,
Zn||VS
2
achieves
1.7
,
with
superior
negative‐to‐positive
ratio
2.5,
electrolyte‐to‐capacity
101.4
µL
−1
displaying
remarkable
stability
over
1000
cycles
under
high
mass
loading
11.0
mg
without
significant
degradation.
in
electrolyte
engineering
provides
new
perspective
situ
SEI
design
furthers
understanding
anode
stabilization.
Advanced Functional Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Сен. 2, 2024
Abstract
Aqueous
zinc
(Zn)
metal
batteries
are
very
attractive
owing
to
the
high
theoretical
capacity
(820
mAh
g
−1
),
meritable
electrode
potential
(−0.76
V
vs
SHE),
low
cost,
and
environmental
friendliness
of
Zn
anodes.
However,
dendrite
formation,
corrosion,
water
decomposition
on
anodes
should
be
resolved
for
their
practical
applications.
Herein,
conformally
coated
multifunctional
organic/inorganic
hybrid
artificial
layers
demonstrated
reversible
stable
deposition.
These
synthesized
through
polyoxometalate
(POM)
initiated
polymerization
into
poly(1,3‐dioxolane)
(Poly(DOL))
directly
onto
surface.
Moreover,
POM
acted
as
chemical
bridge
connecting
Poly(DOL)
with
anode
construct
mechanically
robust
a
thickness
≈40
nm.
The
fast
selective
2+
ion
transport
POM/Poly(DOL)
layer
(POMDOL)
preferential
growth
(002)
crystalline
plane
attributed
Accordingly,
POMDOL
(PDOLZn)
achieves
an
extended
cycling
period
up
2,876
hours
cumulative
29
Ah
at
20
mA
cm
−2
1
.
depth
discharge
(DOD)
40%
is
achieved.
Consequently,
PDOLZn
||
β‐MnO
2
full
cells
delivered
specific
245
long‐term
stability
over
000
cycles.