Advanced Energy Materials,
Год журнала:
2023,
Номер
14(5)
Опубликована: Ноя. 27, 2023
Abstract
The
interrelation
is
explored
between
external
pressure
(0.1,
1,
and
10
MPa),
solid
electrolyte
interphase
(SEI)
structure/morphology,
lithium
metal
plating/stripping
behavior.
To
simulate
anode‐free
batteries
(AF‐LMBs)
analysis
performed
on
“empty”
Cu
current
collectors
in
standard
carbonate
electrolyte.
Lower
promotes
organic‐rich
SEI
macroscopically
heterogeneous,
filament‐like
Li
electrodeposits
interspersed
with
pores.
Higher
inorganic
F‐rich
more
uniform
denser
film.
A
“seeding
layer”
of
lithiated
pristine
graphene
(pG@Cu)
favors
an
anion‐derived
electrodeposition,
enabling
extended
electrochemical
stability
at
a
lower
pressure.
State‐of‐the‐art
performance
achieved
1MPa:
pG‐enabled
half‐cell
stable
after
300
h
(50
cycles)
1
mA
cm
−2
rate
−3
mAh
capacity
(17.5
µm
plated/stripped),
cycling
Coulombic
efficiency
(CE)
99.8%.
AF‐LMB
cells
high
mass
loading
NMC622
cathode
(21
mg
)
undergo
200
cycles
CE
99.4%
C/5‐charge
C/2‐discharge
(1C
=
178
g
−1
).
Density
functional
theory
(DFT)
highlights
the
differences
adsorption
energy
solvated‐Li
+
onto
various
crystal
planes
(100),
(110),
(111),
versus
lithiated/delithiated
(0001)
graphene,
giving
insight
regarding
role
support
surface
energetics
promoting
heterogeneity.
Abstract
Solid-state
lithium
metal
batteries
show
substantial
promise
for
overcoming
theoretical
limitations
of
Li-ion
to
enable
gravimetric
and
volumetric
energy
densities
upwards
500
Wh
kg
−1
1,000
l
,
respectively.
While
zero-lithium-excess
configurations
are
particularly
attractive,
inhomogeneous
plating
on
charge
results
in
active
loss
a
subsequent
coulombic
efficiency
penalty.
Excess
is
therefore
currently
needed;
however,
this
negatively
impacts
density
thus
limiting
its
thickness
essential.
Here
we
discuss
the
viability
various
technologies
realizing
thin
films
that
can
be
scaled
up
volumes
required
gigafactory
production.
We
identify
thermal
evaporation
as
potentially
cost-effective
route
address
these
challenges
provide
techno-economic
assessment
projected
costs
associated
with
fabrication
thin,
dense
foils
using
process.
Finally,
estimate
solid-state
pack
made
thermally
evaporated
foils.
Advanced Energy Materials,
Год журнала:
2024,
Номер
14(17)
Опубликована: Апрель 3, 2024
Abstract
Anode‐free
manufacturing
holds
promise
to
enable
high
energy
densities
and
lower
Lithium
(Li)‐metal
solid‐state
batteries
(LMSSBs).
Nevertheless,
in
contrast
thick
Li
foil
(>50
µm),
the
stripping
capacity
of
situ‐formed
(10–30
µm)
is
limited
due
diminished
creep
flow,
resulting
reduced
accessible
capacity.
This
study
explores
correlation
between
surface
roughness
garnet
7
La
3
Zr
2
O
12
(LLZO)
solid
electrolyte.
The
results
reveal
that
can
be
enhanced
through
modification
electrolytes.
Additionally,
this
scrutinizes
behavior
situ
under
intermittent‐current
discharge
conditions,
which
are
more
relevant
operational
conditions
electric
vehicles
(EVs).
It
demonstrated
that,
when
compared
constant‐current
stripping,
effectively
suppresses
void
formation
enhances
by
40%.
considered
intermittent
current
inhibits
accumulation
vacancies,
thereby
delaying
formation.
These
findings
provide
valuable
insights
into
development
high‐performance
anode‐free
LMSSBs
for
EVs.
Advanced Materials,
Год журнала:
2024,
Номер
36(47)
Опубликована: Окт. 10, 2024
Abstract
Interest
in
all‐solid‐state
batteries
(ASSBs),
particularly
the
anode‐less
type,
has
grown
alongside
expansion
of
electric
vehicle
(EV)
market,
because
they
offer
advantages
terms
their
energy
density
and
manufacturing
cost.
However,
most
ASSBs,
anode
is
covered
by
a
protective
layer
to
ensure
stable
lithium
(Li)
deposition,
thus
requiring
high
temperatures
adequate
Li
ion
diffusion
kinetics
through
layer.
This
study
proposes
dual‐seed
consisting
silver
(Ag)
zinc
oxide
(ZnO)
nanoparticles
for
sulfide‐based
ASSBs.
dual‐seed‐based
not
only
facilitates
via
multiple
lithiation
pathways
over
wide
range
potentials,
but
also
enhances
mechanical
stability
interface
situ
formation
Ag–Zn
alloy
with
ductility.
The
capacity
retention
during
full‐cell
evaluation
80.8%
100
cycles
when
cycled
at
1
mA
cm
−2
3
mAh
room
temperature.
approach
provides
useful
insights
into
design
multi‐seed
concepts
which,
from
mechanochemical
perspective,
various
lithiophilic
materials
synergistically
impact
upon
interface.
ACS Energy Letters,
Год журнала:
2025,
Номер
10(3), С. 1174 - 1182
Опубликована: Фев. 22, 2025
Lithium-reservoir-free
solid-state
batteries
can
fail
due
to
electrical
shorting
as
a
result
of
fracture
and
lithium
metal
filament
formation.
Mechanical
stress
at
the
solid
electrolyte
surface
induce
fractures,
which
promote
growth.
This
arises
from
both
electrochemical
sources,
electrodeposition,
mechanical
such
external
stack
pressure.
Solid
roughness
applied
pressure
together
affect
development.
study
combines
experiments,
3D
synchrotron
imaging,
mesoscale
modeling
explore
how
influences
failure
mechanisms
in
free
batteries.
At
low
pressure,
irregular
plating
resulting
high
local
current
density
drive
failure.
higher
uniform
is
favored;
however,
notch-like
features
experience
tensile
stress,
leading
fractures
that
cause
premature
short-circuiting.
Advanced Energy Materials,
Год журнала:
2023,
Номер
14(5)
Опубликована: Ноя. 27, 2023
Abstract
The
interrelation
is
explored
between
external
pressure
(0.1,
1,
and
10
MPa),
solid
electrolyte
interphase
(SEI)
structure/morphology,
lithium
metal
plating/stripping
behavior.
To
simulate
anode‐free
batteries
(AF‐LMBs)
analysis
performed
on
“empty”
Cu
current
collectors
in
standard
carbonate
electrolyte.
Lower
promotes
organic‐rich
SEI
macroscopically
heterogeneous,
filament‐like
Li
electrodeposits
interspersed
with
pores.
Higher
inorganic
F‐rich
more
uniform
denser
film.
A
“seeding
layer”
of
lithiated
pristine
graphene
(pG@Cu)
favors
an
anion‐derived
electrodeposition,
enabling
extended
electrochemical
stability
at
a
lower
pressure.
State‐of‐the‐art
performance
achieved
1MPa:
pG‐enabled
half‐cell
stable
after
300
h
(50
cycles)
1
mA
cm
−2
rate
−3
mAh
capacity
(17.5
µm
plated/stripped),
cycling
Coulombic
efficiency
(CE)
99.8%.
AF‐LMB
cells
high
mass
loading
NMC622
cathode
(21
mg
)
undergo
200
cycles
CE
99.4%
C/5‐charge
C/2‐discharge
(1C
=
178
g
−1
).
Density
functional
theory
(DFT)
highlights
the
differences
adsorption
energy
solvated‐Li
+
onto
various
crystal
planes
(100),
(110),
(111),
versus
lithiated/delithiated
(0001)
graphene,
giving
insight
regarding
role
support
surface
energetics
promoting
heterogeneity.