Chemical Communications,
Год журнала:
2025,
Номер
unknown
Опубликована: Янв. 1, 2025
High-Ni
cathodes
promise
high
energy
density
but
suffer
from
interfacial
degradation.
Here,
a
dual-additive
electrolyte-trimethylsilyl
phosphate
to
scavenge
HF
and
adiponitrile
tailor
Li+
solvation-enables
robust,
LiF-rich
CEI,
boosting
NCM811's
stability.
This
strategy
achieves
90.16%
capacity
retention
at
5C,
offering
pathway
durable,
high-performance
batteries.
Advanced Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Апрель 29, 2025
Abstract
Anode‐free
lithium
metal
battery
(AFLMB)
has
become
an
excellent
candidate
for
long
endurance
electric
vehicles
and
low
altitude
aircraft,
profiting
from
its
high
energy
density
as
well
outstanding
manufacturing
safety.
However,
the
limitation
at
discharge
rates
of
AFLMBs
is
shrouded
in
mystery,
yet
to
achieve
more
attention.
Herein,
fast
dissected
exhaustively,
a
symptomatic
strategy
break
limit
put
forward,
order
eliminate
inevitable
mismatch
that
lies
inferior
performance
AFLMBs.
A
“volcano‐type”
curve
capacity
retention
discovered
with
rate
increased.
Systematic
investigation
revealed
overlapped
spatial
relationship
between
fresh
deposited
Li
residue
0
facilitated
utilization
“recoverable
”
(Li
)
prophase
increase.
further
enhanced
induced
large
concentration
polarization
(
η
conc
),
reflecting
limited
+
diffusion.
Enabling
electrolyte
rapidly
transport
by
lowering
increased
optimal
cycling
stability
This
work
reveals
rate‐determining
step
high‐rate
expands
employment
boundary
under
harsh
conditions,
providing
significant
complement
present
knowledge
respect
power
Journal of the American Chemical Society,
Год журнала:
2025,
Номер
unknown
Опубликована: Май 2, 2025
Sulfone-based
electrolytes
offer
unusually
high
anodic
and
thermal
stability
that
in
principle
makes
them
promising
candidates
for
fabricating
energy-dense
lithium
metal
batteries
(LMBs).
Their
uses
practical
are
currently
limited
by
their
inability
to
sustain
long-term
Li
plating/stripping
processes
due
reactivity
toward
the
metal.
Here,
we
report
on
design
synthesis
of
a
unique
family
fluorosulfonyl
group-based
(FSO2-)
molecules,
modified
with
ethyl
(FSE)/N,N-dimethyl
(FSNDM)/N,N-diethyl
(FSNDE)/N-pyrrolidine
(FSNP)
end
groups
create
exceptionally
stable
single-salt
single-solvent
electrolytes.
The
flammability,
solvation
structure,
ion
transport,
deposition
kinetics,
high-voltage
systematically
studied.
It
is
shown
nonflammable,
possess
weak
characteristics,
yet
manifest
room-temperature
ionic
conductivities
(1.6-6.1
mS
cm-1)
low
solution
viscosities.
In
comparison
FSE,
FSNDM-,
FSNDE-,
FSNP-based
exhibit
an
reversible
Coulombic
efficiency
(>99.71%
over
800
cycles)
typical
oxidative
at
voltages
exceeding
4.6
V.
Deployed
as
(20
μm
anode
3
g
A
h-1
electrolyte)
high-loading
(18.5
mg
cm-2)
LiNi0.8Co0.1Mn0.1O2
cathodes,
329
cycles
have
been
achieved
before
80%
capacity
retention.
Six
Ah
pouch
cells
based
designed
also
energy
density
(496
W
h
kg-1)
150
most
2.7%
volume
expansion.
Our
findings
demonstrate
through
intentional
molecular
design,
sulfone
provide
robust
route
nonflammable
compatible
cathodes.
Advanced Functional Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Май 22, 2025
Abstract
Sulfurized
polyacrylonitrile
(SPAN)
recently
emerges
as
a
prospective
cathode
for
lithium–sulfur
(Li–S)
batteries
owing
to
its
high
S
utilization,
remarkable
cycling
stability,
and
liberty
from
shuttle
effect.
Despite
weakly
solvating
ether
electrolytes
exhibiting
simultaneously
compatibility
SPAN
lithium
(Li)
anode,
they
universally
suffer
low
ionic
conductivity
narrow
liquid‐phase
temperature
range.
However,
conventional
ether‐based
with
excellent
cannot
realize
reversible
solid–solid
conversion
of
due
Li
polysulfide
intermediates
(LiPSs)
dissolving
shuttling.
Here,
series
ethers
are
evaluated
by
selectively
methylating
dimethoxymethane
(DMM)
fine‐tune
their
solvation
capability
Enlightened
electrolytes,
the
contact
ion
pair
(CIP)‐dominated
electrolyte
is
designed
satisfactory
over
wide
The
reinforcement
mechanisms
CIP‐dominated
anode
comprehensively
elucidated
through
experimental
characterizations
molecular
dynamics
simulations.
Based
on
optimized
electrolyte,
Li||SPAN
full
cells
can
steadily
operate
range
−20
60
°C.
Furthermore,
120
mAh
pouch
cell
exhibit
85.5%
capacity
retention
after
45
cycles
at
0.2
C.
Chemical Communications,
Год журнала:
2025,
Номер
unknown
Опубликована: Янв. 1, 2025
High-Ni
cathodes
promise
high
energy
density
but
suffer
from
interfacial
degradation.
Here,
a
dual-additive
electrolyte-trimethylsilyl
phosphate
to
scavenge
HF
and
adiponitrile
tailor
Li+
solvation-enables
robust,
LiF-rich
CEI,
boosting
NCM811's
stability.
This
strategy
achieves
90.16%
capacity
retention
at
5C,
offering
pathway
durable,
high-performance
batteries.