Angewandte Chemie,
Год журнала:
2024,
Номер
unknown
Опубликована: Ноя. 12, 2024
Abstract
Despite
aqueous
electrolytes
offer
a
great
opportunity
for
large‐scale
energy
storage
owing
to
their
safety
and
cost‐effectiveness,
practical
application
suffers
from
the
parasitic
side
reactions
poor
temperature
adaptability
stemming
weak
hydrogen‐bond
(HB)
network
in
free
water.
Here,
we
propose
guiding
thought
“strong
replaces
weak”
design
hydrogen
bond‐anchored
electrolyte
by
introducing
sulfolane
(SL)
disrupting
regular
HB
contributing
superior
tolerance.
Judiciously
combined
experimental
characterization
theoretical
calculation
confirm
that
SL
can
remodel
primary
solvation
shell
of
metal
ions,
customize
stable
electrode
interface
chemistry
restrain
reactions.
Consequently,
symmetric
supercapacitor
constructed
activated
carbon
(AC)
electrodes
is
able
fully
work
within
voltage
range
2.4
V
reach
high
capacitance
retention
89.8
%
after
60000
cycles.
Additionally,
Zn
anodes
exhibit
ultra‐stable
plating/stripping
behaviors
wide
(−20–60
°C),
zinc‐ion
capacitor
(Zn//AC)
also
delivers
an
excellent
cycling
stability
with
capacity
99.7
55000
cycles,
implying
designed
has
potential
extreme
environments.
This
proposes
novel
critical
strategy
paves
route
construction
wide‐temperature
devices.
Carbon Neutralization,
Год журнала:
2025,
Номер
4(2)
Опубликована: Фев. 12, 2025
ABSTRACT
Aqueous
zinc‐ion
batteries
(AZIBs)
are
considered
one
of
the
most
viable
options
for
large‐scale
energy
storage
applications
due
to
their
high
theoretical
capacity
and
abundant
reserves.
However,
issues
such
as
dendritic
growth
water‐induced
corrosion
reaction
zinc
anode
have
hindered
commercialization.
To
address
these
challenges,
in
situ
generated
multifunctional
poly(caffeic
acid)
(PCA)
interface
with
confined
Cu
sites
oxygen‐containing
groups
was
constructed
on
surface
metal
via
ultraviolet
(UV)
treatment.
The
smooth
compact
PCA
effectively
prevents
from
by
active
water
electrolyte,
while
synergies
zincophilic
copper
constitute
3D
ion
channels
skeleton
accelerates
migration
Zn
2+
enhance
deposition
kinetics,
thus
lowering
desolvation
energy.
symmetric
cells
using
PCA‐modified
demonstrated
stable
cycling
over
2500
h
2200
at
current
densities
1.0
5.0
mA
cm
−2
,
respectively,
much
better
than
controls.
Additionally,
assembled
PCA@Zn//I
2
full
cell
enabled
continuous
1000
cycles
a
density
A
g
−1
presented
reliable
operation
100
pouch
configuration.
Angewandte Chemie International Edition,
Год журнала:
2024,
Номер
unknown
Опубликована: Ноя. 12, 2024
Abstract
Despite
aqueous
electrolytes
offer
a
great
opportunity
for
large‐scale
energy
storage
owing
to
their
safety
and
cost‐effectiveness,
practical
application
suffers
from
the
parasitic
side
reactions
poor
temperature
adaptability
stemming
weak
hydrogen‐bond
(HB)
network
in
free
water.
Here,
we
propose
guiding
thought
“strong
replaces
weak”
design
hydrogen
bond‐anchored
electrolyte
by
introducing
sulfolane
(SL)
disrupting
regular
HB
contributing
superior
tolerance.
Judiciously
combined
experimental
characterization
theoretical
calculation
confirm
that
SL
can
remodel
primary
solvation
shell
of
metal
ions,
customize
stable
electrode
interface
chemistry
restrain
reactions.
Consequently,
symmetric
supercapacitor
constructed
activated
carbon
(AC)
electrodes
is
able
fully
work
within
voltage
range
2.4
V
reach
high
capacitance
retention
89.8
%
after
60000
cycles.
Additionally,
Zn
anodes
exhibit
ultra‐stable
plating/stripping
behaviors
wide
(−20–60
°C),
zinc‐ion
capacitor
(Zn//AC)
also
delivers
an
excellent
cycling
stability
with
capacity
99.7
55000
cycles,
implying
designed
has
potential
extreme
environments.
This
proposes
novel
critical
strategy
paves
route
construction
wide‐temperature
devices.
Advanced Functional Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Фев. 7, 2025
Abstract
The
undesirable
hydrogen
evolution
reaction
(HER)
primarily
contributes
to
the
instability
of
Zn
anode,
which
exacerbates
corrosion
and
dendrite
growth
impedes
application
metal
battery
in
large‐scale
energy
storage.
Although
engineering
functional
aqueous
electrolyte
prominently
controls
HER,
it
hardly
eradicates
occurrence
HER
from
source.
Herein,
this
research
utilizes
coupling
donor–acceptor
bonds
(H‐bonds)
manipulate
structure
design
a
novel
methanol
(MeOH)‐based
anhydrous
organic
with
propylene
carbonate
(PC)
as
co‐solvent,
fundamentally
eliminating
accompanied
by
suppressed
growth.
PC
molecules
acceptor
strengthen
H‐bonds
networks
between
MeOH
donor
weaken
interaction
cations
anions,
enhancing
stability
reducing
anion‐involved
by‐products
formation.
Meanwhile,
preferential
adsorbed
on
anode
surface
form
favorable
component‐dominated
solid
interface
layer,
inducing
uniform
deposition
along
(002)
orientation.
Consequently,
exhibits
excellent
cycling
high
reversibility.
assembled
cells
also
harvest
satisfactory
low‐temperature
tolerance.
More
importantly,
corresponding
Zn||PANI
full
cell
pouch
behave
an
impressive
capacity
retention
92.4%
91.1%
after
3200
1400
cycles,
respectively.
Advanced Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Фев. 19, 2025
Abstract
The
sustained
hydrogen
evolution
and
zinc
(Zn)
dendrite
growth
greatly
impede
the
practical
application
of
low‐cost
aqueous
Zn
metal
batteries
(ZMBs).
Herein,
for
first
time,
a
microphase
separation
strategy
is
proposed
to
construct
″water‐in‐oil
(W/O)
electrolyte
endow
durable
ZMBs.
As
validated
by
theoretical
modeling
experimental
characterizations,
unique
reverse
micelle
structure
within
not
only
disrupts
water
bonding
efficiently
inhibits
consumption
at
anode,
but
also
undergoes
directed
movement
reversible
demulsification
under
electric
field,
thus
enhancing
anode
desolvation
kinetics
inhibiting
interfacial
side
reactions.
Owing
simultaneous
regulation
molecules
in
both
bulk
interface,
this
W/O
achieves
high
plating/stripping
Coulombic
efficiency
99.76%
over
6000
cycles,
maintains
an
extend
lifespan
Zn||V
10
O
24
·12H
2
(VOH)
cells
with
negligible
formation.
These
key
findings
are
expected
promote
engineering
toward
Zinc-ion
secondary
batteries
have
been
competitive
candidates
since
the
"post-lithium-ion"
era
for
grid-scale
energy
storage,
owing
to
their
plausible
security,
high
theoretical
capacity,
plentiful
resources,
and
environment
friendliness.
However,
many
encumbrances
like
notorious
parasitic
reactions
Zn
dendrite
growth
hinder
development
of
zinc-ion
remarkably.
Faced
with
these
challenges,
eutectic
electrolytes
aroused
notable
attention
by
virtue
feasible
synthesis
tunability.
This
review
discusses
definition
advanced
functionalities
in
detail
divides
them
into
nonaqueous,
aqueous,
solid-state
regard
state
component
electrolytes.
In
particular,
corresponding
chemistry
concerning
solvation
structure
regulation,
electric
double
layer
(EDL)
structure,
solid-electrolyte
interface
(SEI)
charge/ion
transport
mechanism
is
systematically
elucidated
a
deeper
understanding
Moreover,
remaining
limitations
further
are
discussed
electrolyte
design
extended
applications.
ACS Applied Materials & Interfaces,
Год журнала:
2025,
Номер
unknown
Опубликована: Май 17, 2025
Aqueous
zinc-ion
hybrid
supercapacitors
(ZHSCs)
have
stimulated
wide
attention
due
to
their
features
of
low
cost
and
nontoxic
nature.
Nevertheless,
the
growth
zinc
dendrites,
parasitic
reactions,
a
narrow
electrochemical
stable
window
(ESW)
severely
limited
development
ZHSCs.
Here,
distinct
vesicle-like
structure
using
polyethylene
glycol
monomethyl
ether
(MPEG)
ethylene
dimethyl
(DME)
is
creatively
represented,
which
named
bicelle
electrolyte.
In
this
unique
structure,
O
-OH
C-O-C
in
MPEG
extends
interior,
encapsulating
aqueous
Zn(ClO4)2.
The
hydrophobic
groups
DME
accumulate
interactions,
forming
domain.
Due
presence
domain,
internal
active
water
molecules
are
prevented
from
directly
contacting
Zn
foil.
external
hydrophilic
form
hydrogen
bonds
with
free
water,
also
greatly
suppress
activity
thus
inhibiting
harmful
side
reactions
(hydrogen
evolution
reactions)
related
water.
was
widened
3.03
V.
Furthermore,
formed
by
head-to-head
creates
Zn2+
channel
that
promotes
rapid
uniform
deposition
Zn2+,
thereby
dendrite
promoting
cycling
stability
cell.
experiments
show
high
ion
conductivity
51.87
mS
cm-1
transference
number
(tZn2+)
0.70
can
be
achieved
system.
assembled
asymmetric
supercapacitor
specific
capacity
95.47
mAh
g-1
at
5
A
g-1,
it
still
maintains
retention
rate
84.40%
after
8000
cycles.
symmetric
cell
delivers
long
lifespan
over
1300
h
1
mA
cm-2.
