Advanced Functional Materials,
Journal Year:
2024,
Volume and Issue:
unknown
Published: Nov. 14, 2024
Abstract
Garnet‐type
solid‐state
electrolytes
with
exceptional
stability
are
believed
to
promote
the
commercialization
of
all
lithium
metal
batteries.
However,
extensive
application
garnet‐type
is
greatly
impeded
on
account
their
low
ionic
conductivity.
Herein,
a
high‐entropy
fast
lithium‐ion
conductor
Li
7
(La,Nd,Sr)
3
(Zr,Ta)
2
O
12
(LLNSZTO)
high
lattice
distortion
designed.
It
found
that
enhanced
conductivity
entropy
electrolyte
LLNSZTO
achieved
by
introducing
disorder
in
lattice,
which
creates
ion
penetration
paths
flattened
energy
landscapes
within
pristine
ordered
lattice.
Thus,
prepared
solid
exhibits
activation
for
+
migration
(0.34
eV)
and
elevated
(6.26
×
10
−4
S
cm
−1
).
Full
cells
assembled
electrolyte,
anode,
LiFePO
4
(LFP)
cathode
exhibit
excellent
capacity
retention
86.81%
after
200
cycles
at
room
temperature.
Moreover,
superior
enables
battery
high‐loading
LFP
(>12
mg
−2
),
achieving
stable
cycling
exceeding
120
cycles.
The
large
area
pouch
cell
(5.5
8
cm)
long‐term
performance,
showing
96.50%
50
Advanced Energy Materials,
Journal Year:
2023,
Volume and Issue:
13(38)
Published: Aug. 29, 2023
Abstract
Portable
electronic
devices
and
electric
vehicles
have
become
indispensable
in
daily
life
caused
an
increasing
demand
for
high‐performance
lithium‐ion
batteries
(LIBs)
with
high‐energy‐density.
This
work
compares
the
intrinsic
characteristics
Li
+
conduction
mechanisms
of
various
electrolytes,
aiming
at
emphasizing
their
suitability
high‐energy‐density
LIBs.
Among
all
polymer‐based
solid‐state
electrolytes
(SSEs)
are
most
promising
candidates,
as
they
demonstrate
comprehensive
properties.
The
advantages
disadvantages
commonly
used
polymer
matrix
materials
SSEs
discussed,
along
typical
approaches
to
address
limitations.
As
significant
issues
cycle
stability,
development
related
cathode/electrolyte
interfacial
contact
wetting,
electrochemical
compatibility,
LIBs
employing
SSEs,
well
anode/electrolyte
chemical
stability
lithium
dendrite
suppression
comprehensively
reviewed
analyzed.
Finally,
perspectives
on
future
research
directions
developing
highlighted
building
upon
existing
literature.
Advanced Energy Materials,
Journal Year:
2023,
Volume and Issue:
13(13)
Published: Feb. 17, 2023
Abstract
Ultrathin
composite
solid‐state
electrolytes
(CSSEs)
demonstrate
great
promise
in
high‐energy‐density
batteries
due
to
their
ultrathin
thickness
and
good
adaptability
lithium
metal
anodes.
However,
uncontrolled
dendrite
growth
performance
deterioration
caused
by
the
aggregation
of
inorganic
powder
restrict
practical
application
CSSEs.
Herein,
a
flexible,
self‐supporting
Li
6.5
La
3
Zr
1.5
Ta
0.5
O
12
(LLZO)
ceramic
skeleton
is
prepared
tape‐casting
method.
Subsequently,
µm‐thick
CSSE
with
3D
interconnection
structure
achieved
through
situ
UV
curing
ethoxylated
trimethylolpropane
triacrylate
(ETPTA)
(CS‐CSSE).
This
design
includes
sintered
LLZO
ceramic,
which
can
avoid
uneven
distribution
phase
regulate
ion
migration.
Meanwhile,
cross‐linked
ETPTA
polymer
electrolyte
contributes
lower
interfacial
impedance.
In
addition,
continuous
two‐phase
interface
also
provide
fast
transmission
channel
for
+
.
As
result,
CS‐CSSE
demonstrates
superior
transference
number
(0.83)
ionic
conductivity
(1.19
×
10
‐3
S
cm
‐1
)
at
25
°C.
As‐prepared
Li|LiNi
0.83
Co
0.12
Mn
0.05
2
exhibit
high
discharge
specific
capacities
185.4
mAh
g
0.1
C
average
coulombic
efficiency
greater
than
99%.
The
pouch
cells
energy
densities
376
Wh
Kg
1186
L
work
provides
new
insights
into
ceramics
batteries.
ACS Nano,
Journal Year:
2024,
Volume and Issue:
18(3), P. 1969 - 1981
Published: Jan. 11, 2024
The
components
and
structures
of
the
solid-electrolyte
interphase
(SEI)
are
critical
for
stable
cycling
lithium
metal
batteries
(LMBs).
LiF
has
been
widely
studied
as
dominant
component
SEI,
but
Li2O,
which
a
much
lower
diffusion
barrier
Li+,
rarely
investigated
SEI.
effect
Li2O-dominated
SEI
on
electrochemical
performance
still
remains
elusive.
Herein,
an
ultrastrong
coordinated
cosolvation
diluent,
2,3-difluoroethoxybenzene
(DFEB),
is
designed
to
modulate
solvation
structure
tailor
LMBs.
In
DFEB-based
LHCE
(DFEB-LHCE),
DFEB
intensively
participates
in
first
shell
synergizes
with
FSI–
inorganic-rich
different
from
LiF-dominated
formed
conventional
LHCE.
Benefiting
this
special
architecture,
high
Coulombic
efficiency
(CE)
99.58%
Li||Cu
half
cells,
voltage
profiles,
dense
uniform
deposition,
well
effective
inhibition
Li
dendrite
formation
symmetrical
cell,
achieved.
More
importantly,
DFEB-LHCE
can
be
matched
various
cathodes
such
LFP,
NCM811,
S
cathodes,
Li||LFP
full
cell
using
possesses
85%
capacity
retention
after
650
cycles
99.9%
CE.
Especially
1.5
Ah
practical
pouch
achieves
excellent
89%
250
superb
average
CE
99.93%.
This
work
unravels
superiority
feasibility
tailoring
through
modulation
structures.
Advanced Materials,
Journal Year:
2023,
Volume and Issue:
35(38)
Published: June 3, 2023
Ultrathin
and
super-toughness
gel
polymer
electrolytes
(GPEs)
are
the
key
enabling
technology
for
durable,
safe,
high-energy
density
solid-state
lithium
metal
batteries
(SSLMBs)
but
extremely
challenging.
However,
GPEs
with
limited
uniformity
continuity
exhibit
an
uneven
Li+
flux
distribution,
leading
to
nonuniform
deposition.
Herein,
a
fiber
patterning
strategy
developing
engineering
ultrathin
(16
µm)
fibrous
high
ionic
conductivity
(≈0.4
mS
cm-1
)
superior
mechanical
toughness
(≈613%)
durable
safe
SSLMBs
is
proposed.
The
special
patterned
structure
provides
fast
transport
channels
tailoring
solvation
of
traditional
LiPF6
-based
carbonate
electrolyte,
rapid
transfer
kinetics
uniform
flux,
boosting
stability
against
Li
anodes,
thus
realizing
ultralong
plating/stripping
in
symmetrical
cell
over
3000
h
at
1.0
mA
cm-2
,
mAh
.
Moreover,
LiFePO4
loading
10.58
mg
deliver
stable
cycling
life
1570
cycles
C
92.5%
capacity
retention
excellent
rate
129.8
g-1
5.0
cut-off
voltage
4.2
V
(100%
depth-of-discharge).
Patterned
systems
powerful
strategies
producing
SSLMBs.
Chemical Society Reviews,
Journal Year:
2024,
Volume and Issue:
53(10), P. 5291 - 5337
Published: Jan. 1, 2024
Design
principles,
engineering
strategies,
challenges,
and
opportunities
of
gel
polymer
electrolytes
for
rechargeable
batteries
toward
wide-temperature
applications
are
thoroughly
reviewed.
Advanced Materials,
Journal Year:
2023,
Volume and Issue:
35(47)
Published: Aug. 26, 2023
Abstract
The
organic–inorganic
interfaces
can
enhance
Li
+
transport
in
composite
solid‐state
electrolytes
(CSEs)
due
to
the
strong
interface
interactions.
However,
non‐conductive
areas
CSEs
with
inert
fillers
will
hinder
construction
of
efficient
channels.
Herein,
fully
active
conductive
networks
are
proposed
improve
by
composing
sub‐1
nm
inorganic
cluster
chains
and
organic
polymer
chains.
monodispersed
matrix
a
brief
mixed‐solvent
strategy,
their
diameter
ultrafine
dispersion
state
eliminate
interior
filler‐agglomeration,
respectively,
providing
rich
surface
for
Therefore,
3D
connected
finally
construct
homogeneous,
large‐scale,
continuous
fast
Furthermore,
conjecture
about
1D
oriented
distribution
along
is
optimize
pathways.
Consequently,
as‐obtained
possess
high
ionic
conductivity
at
room
temperature
(0.52
mS
cm
−1
),
transference
number
(0.62),
more
mobile
(50.7%).
assembled
LiFePO
4
/Li
cell
delivers
excellent
stability
1000
cycles
0.5
C
700
1
C.
This
research
provides
new
strategy
enhancing
interfaces.
Advanced Functional Materials,
Journal Year:
2024,
Volume and Issue:
34(18)
Published: Jan. 20, 2024
Abstract
Solid‐state
batteries
(SSBs)
are
regarded
as
the
most
promising
next‐generation
energy
storage
devices
due
to
their
potential
achieve
higher
safety
performance
and
density.
However,
troubles
in
preparation
of
ultrathin
solid‐state
electrolytes
(SEs)
well
resultant
compromise
mechanical
strength
greatly
limit
application
SSBs.
Herein,
a
novel
situ
polymerized
integrated
SE/cathode
design
is
developed.
The
ceramic
layer
supported
on
cathode
serves
not
only
rigid
scaffold
prevent
direct
contact
between
anode
but
also
active
inorganic
fillers
enhance
properties
SE
film.
unique
Li‐ion
coordination
environments
Li
hopping
mechanism
profoundly
promote
fast
ion
transport
composite
SEs.
SEs
simultaneously
balance
thickness
(10
µm),
(0.65
mS
cm
−1
),
superior
Young's
modulus
(66.8
GPa),
excellent
interface
contact.
pouch
cells
with
practical
Li||LiNi
0.8
Co
0.1
Mn
O
2
configuration
an
ultrahigh
volumetric
density
1018
Wh
L
performance.
exhibits
great
promise
for
SSBs
high
Journal of the American Chemical Society,
Journal Year:
2024,
Volume and Issue:
146(10), P. 6591 - 6603
Published: Feb. 29, 2024
Polymer-in-ceramic
composite
solid
electrolytes
(PIC–CSEs)
provide
important
advantages
over
individual
organic
or
inorganic
electrolytes.
In
conventional
PIC–CSEs,
the
ion
conduction
pathway
is
primarily
confined
to
ceramics,
while
faster
routes
associated
with
ceramic–polymer
interface
remain
blocked.
This
challenge
two
key
factors:
(i)
difficulty
in
establishing
extensive
and
uninterrupted
interfaces
due
ceramic
aggregation;
(ii)
are
unresponsive
conducting
ions
because
of
their
inherent
incompatibility.
Here,
we
propose
a
strategy
by
introducing
polymer-compatible
ionic
liquids
(PCILs)
mediate
between
ceramics
polymer
matrix.
mediation
involves
polar
groups
PCILs
interacting
Li+
on
surfaces
as
well
interactions
components
chains.
addresses
aggregation
issue,
resulting
uniform
PIC–CSEs.
Simultaneously,
it
activates
interpenetrating
channels
that
promote
efficient
transport
across
phase,
interfaces,
intervening
pathways.
Consequently,
obtained
PIC–CSEs
exhibit
high
conductivity,
exceptional
flexibility,
robust
mechanical
strength.
A
PIC–CSE
comprising
poly(vinylidene
fluoride)
(PVDF)
60
wt
%
PCIL-coated
Li3Zr2Si2PO12
(LZSP)
fillers
showcasing
an
conductivity
0.83
mS
cm–1,
superior
transference
number
0.81,
elongation
∼300%
at
25
°C
could
be
produced
meter-scale.
Its
lithium
metal
pouch
cells
show
energy
densities
424.9
Wh
kg–1
(excluding
packing
films)
puncture
safety.
work
paves
way
for
designing
commercial
viability.
Chemical Society Reviews,
Journal Year:
2024,
Volume and Issue:
53(6), P. 3134 - 3166
Published: Jan. 1, 2024
The
utilization
of
computational
approaches
at
various
scales,
including
first-principles
calculations,
MD
simulations,
multi-physics
modeling,
and
machine
learning
techniques,
has
been
instrumental
in
expediting
the
advancement
SSEs.