ACS Applied Materials & Interfaces,
Год журнала:
2024,
Номер
16(46), С. 64364 - 64376
Опубликована: Ноя. 5, 2024
In
the
pursuit
of
enhancing
performance
and
safety
lithium
(Li)-metal
batteries,
discovery
effective
electrolyte
additives
to
suppress
Li
dendrites
has
emerged
as
a
paramount
objective.
this
study,
we
employ
an
inverse
design
strategy
identify
potential
for
dendrite
mitigation.
Two
key
mechanisms,
namely,
formation
robust
solid
interphase
layers
leveling
mechanism,
serve
foundation
our
investigation.
Our
is
guided
by
molecular
properties
such
lowest
unoccupied
orbital
energy
interaction
upon
surface
adsorption.
An
active
learning
process
utilizing
Bayesian
optimization
(BO)
was
utilized
molecules
with
ideal
properties.
Through
screening
process,
uncover
collection
62
act
SEI-forming
additives,
along
106
both
surpassing
established
reported
in
literature.
This
work
highlights
BO
methods
computationally
based
materials
many
applications,
discovered
could
potentially
boost
commercialization
Li–metal
batteries.
Advanced Energy Materials,
Год журнала:
2023,
Номер
13(39)
Опубликована: Авг. 18, 2023
Abstract
Lithium‐ion
batteries
(LIBs)
and
beyond‐LIB
systems
exhibit
properties
that
are
determined
by
electrochemical
reactions
occurring
in
their
four
essential
components—the
cathode,
anode,
electrolyte,
separator.
Advanced
analytical
methods
such
as
differential
mass
spectrometry
(DEMS)
can
assist
understanding
the
behavior,
which
help
advancing
battery
technologies.
Recent
studies
have
shown
DEMS‐enabled
real‐time
gas
analysis
of
provide
valuable
information
on
aspects
gaseous
reactants
or
(side)
products,
cannot
be
obtained
appropriately
through
other
characterization
techniques.
This
review
aims
to
a
comprehensive
overview
latest
developments
advancements
use
DEMS
rapid,
operando
gas‐monitoring
method
for
advanced
rechargeable
systems.
Moreover,
significance
current
future
development
is
also
discussed
insights
provided
into
various
chemistries
benefit
from
applications.
intended
readers
understand
potential
drive
innovation
industry.
Abstract
The
improvement
of
the
safety,
specific
energy,
cycle
life
and
cost
reduction
Li‐ion
batteries
are
hot
research
topics.
Now,
in
pursuit
high
energy
density,
employed
high‐energy‐density
cathode/anode
materials
increased
operation
voltage
challenge
prevalent
electrolyte
formula,
like
existing
ester
ether
electrolytes
cannot
withstand
high‐voltage
high‐capacity
anode
such
as
lithium
(Li),
silicon
(Si)
silicon‐graphite
(Si−C)
composite
anode.
It
is
recognized
that
stable
electrolyte‐electrode
interfaces
can
avoid
side
reactions
protect
electrode
materials.
Up
to
now,
various
additives
have
been
developed
modify
electrode‐electrolyte
interfaces,
famous
4‐fluoroethylene
carbonate,
vinylene
carbonate
nitrate,
LIBs
metal
(LMBs)
performances
improved
greatly.
However,
lifespan
higher‐energy‐density
with
Li/Si/Si−C
high‐nickel
layer
oxides
cathode
meet
request
due
lack
ideal
formula.
In
this
review,
we
present
a
comprehensive
in‐depth
overview
on
additives,
especially
focused
multifunctional
reaction
mechanisms
fundamental
design.
Finally,
novel
insights,
promising
directions
potential
solutions
for
proposed
motivate
Li
battery
chemistries.
Advanced Functional Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Янв. 13, 2025
Abstract
Li‐O
2
batteries
are
considered
promising
candidates
for
next
generation
high
energy
storage
systems
due
to
their
exceptionally
theoretical
density.
However,
the
accumulation
of
insulating
discharge
product
Li
O
leads
severe
cathode
passivation,
reduced
conductivity,
and
hindered
charge
transfer,
which
seriously
compromise
battery
performance.
This
work
proposes
a
novel
phase‐transfer
catalyst
with
bidirectional
coordination
functionality,
2‐aminopyridine
(AP).
The
AP
molecule
contains
nucleophilic
pyridine
nitrogen
an
electrophilic
amino
hydrogen,
can
interact
+
reactive
oxygen
intermediates
through
electrostatic
attraction
hydrogen
bonding,
respectively.
dual
interaction
facilitates
liquid‐phase
deposition
while
enabling
efficient
decomposition.
uneven
potential
distribution
within
generates
internal
electric
field
that
stabilizes
species,
shields
against
attacks,
suppresses
at
anode
tips,
effectively
preventing
lithium
dendrite
growth.
Therefore,
exhibit
capacity
36419
mAh
g
−1
,
significantly
over‐potential
0.29
V,
extended
cycle
life
exceeding
2256
h.
Through
functional
molecular
structure
design,
catalytic
effect
demonstrated
by
molecules
regulates
migration
substances
during
reactions,
improves
electrochemical
performance
batteries.
The Journal of Physical Chemistry Letters,
Год журнала:
2025,
Номер
unknown, С. 1644 - 1651
Опубликована: Фев. 6, 2025
Lithium-oxygen
(Li-O2)
batteries
have
an
extremely
high
theoretical
specific
energy
but
are
hindered
by
the
sluggish
kinetics
of
oxygen
evolution
reaction
(OER).
Visible-light-assisted
photocatalysts
can
accelerate
OER
kinetics.
However,
photoinvolved
electrochemical
process
at
cathode
remains
insufficiently
understood,
and
interlaboratory
results
not
comparable
reproducible.
In
fact,
sunlight
or
a
xenon
lamp
as
light
source
induces
notable
photothermal
effect
in
batteries,
while
its
impact
on
is
always
underappreciated.
Here,
self-illuminating
photocatalyst
composed
g-C3N4
catalysts
Sr2MgSi2O7:Eu,Dy
phosphors
designed
to
decouple
photo
thermal
effects
Typically,
photocatalytic
dominate
low
external
illumination
powers,
increase
linearly
with
power.
This
work
provides
quantitative
basis
for
benchmarking
catalytic
performance
various
photocatalysts.
Moreover,
proof
concept,
this
study
offers
new
insights
developing
integrated
photoassisted
Li-O2
batteries.
To
overcome
the
energy
limitations
of
conventional
Li‐ion
batteries
(LIB),
renewed
attention
has
been
given
to
Li‐metal
anodes,
which
provide
highest
capacity
and
lowest
anode
potential.
realize
(LMBs),
it
is
crucial
stabilize
unwanted
side
reactions
on
surface
inhibit
problematic
dendrite
growth,
causes
short‐circuit
issues.
Herein,
diverse
pyrrolidone‐based
molecular
dipole
additives
controlled
by
different
functional
groups
are
introduced
as
trifunctional
stabilizers.
It
discovered
that
Li–Li
symmetric
cell
improves
proportionally
with
molar
volume
corresponding
polarizability
values
dipoles.
The
highly
polarizable
dipoles
offer
exceptional
benefits,
including
flattening
Li
metal
anode,
controlling
growth
direction
crystalline
Li,
forming
durable
solid
electrolyte
interface
(SEI)
components.
study
based
polarizability‐controlled
dipoles,
offers
an
effective
approach
for
designing
advanced
stabilizers
develop
high‐performance
LMBs.
Reaching
the
border
of
capable
energy
limit
in
existing
battery
technology
has
turned
research
attention
away
from
rebirth
unstable
Li-metal
anode
chemistry
order
to
achieve
exceptional
performance.
Strict
regulation
dendritic
Li
surface
reaction,
which
results
a
short
circuit
and
safety
issues,
should
be
achieved
realize
batteries.
Herein,
this
study
reports
surface-flattening
interface
product
stabilizing
agent
employing
methyl
pyrrolidone
(MP)
molecular
dipoles
electrolyte
for
cyclable
The
excellent
stability
electrode
over
600
cycles
at
high
current
density
5
mA
cm-2
been
demonstrated
using
an
optimal
concentration
MP
additive.
This
identified
flattening
reconstruction
crystal
rearrangement
behavior
along
stable
(110)
plane
assisted
by
dipoles.
stabilization
anodes
dipole
agents
helped
develop
next-generation
storage
devices
anodes,
such
as
Li-air,
Li-S,
semi-solid-state
Advanced Energy Materials,
Год журнала:
2024,
Номер
14(15)
Опубликована: Март 8, 2024
Abstract
Rechargeable
Li‐O
2
batteries
(LOBs)
are
regarded
as
promising
candidates
for
the
next
generation
of
energy
storage
devices.
One
major
impediments
is
poor
cycle
stability
resulting
from
unreliable
cathode
catalysts
and
serious
corrosion
Li
anode,
hindering
commercial
application
LOBs.
Herein,
a
synergetic
strategy
proposed,
including
design
stable
Co
3
Ru
catalyst
via
d‐band
center
modulation
construction
robust
LiF/Sn/Li
5
Sn
‐PFDTMS
hybrid
protective
layer
on
anode.
Theoretical
calculations
reveal
that
negative
shift
provides
dominant
descriptor
improving
catalysis
activity
Ru‐based
catalysts.
In
situ
PFDTMS‐enhanced
possesses
excellent
mechanical
toughness,
which
can
effectively
shield
anode
corrosive
reaction
ensure
good
+
transport.
Consequently,
LOBs
exhibit
long
life
990
cycles
(≈1980
h).
This
work
confers
concept
high‐performance
rationally
constructing
anodes.
Abstract
LiPF
6
‐based
carbonate
electrolytes
have
been
extensively
employed
in
commercial
Li‐ion
batteries,
but
they
face
numerous
interfacial
stability
challenges
while
applicating
high‐energy‐density
lithium‐metal
batteries
(LMBs).
Herein,
this
work
proposes
N‐succinimidyl
trifluoroacetate
(NST)
as
a
multifunctional
electrolyte
additive
to
address
these
challenges.
NST
could
optimize
Li
+
solvation
structure
and
eliminate
HF/H
2
O
the
electrolyte,
preferentially
be
decomposed
on
Ni‐rich
cathode
(LiNi
0.8
Co
0.1
Mn
,
NCM811)
generate
LiF/Li
3
N‐rich
cathode‐electrolyte
interphase
(CEI)
with
high
conductivity.
The
synergistic
effect
reduces
decomposition
inhibits
transition
metal
(TM)
dissolution.
Meanwhile,
promotes
creation
of
solid
(SEI)
rich
inorganics
anode
(LMA),
which
restrains
growth
dendrites,
minimizes
parasitic
reactions,
fosters
rapid
transport.
As
result,
compared
reference,
Li/LiNi
cell
1.0
wt.%
exhibits
higher
capacity
retention
after
200
cycles
at
1C
(86.4%
vs
.
64.8%)
better
rate
performance,
even
9C.
In
presence
NST,
Li/Li
symmetrical
shows
super‐stable
cyclic
performance
beyond
500
h
0.5
mA
cm
−2
/0.5
mAh
These
unique
features
are
promising
solution
for
addressing
deterioration
issue
high‐capacity
cathodes
paired
LMA.
Advanced Energy Materials,
Год журнала:
2024,
Номер
14(33)
Опубликована: Июль 3, 2024
Abstract
Abundant
and
economical
sodium
(Na)
metal
batteries
promise
superior
energy
densities
compared
to
lithium‐ion
batteries;
however,
they
face
commercialization
challenges
owing
problematic
interfacial
reactions
leading
dendrite
formation
during
cycling.
This
paper
reports
the
ultra‐long
rapid
operation
of
Na
enabled
by
introduction
a
vinylpyrrolidone
(VP)‐based
multifunctional
interface
stabilizer
in
electrolyte.
The
VP
electrolyte
additive
provides
benefits
such
as
surface
flattening,
durable
solid
interphase
layer
formation,
preservation
fresh
Na,
acceleration
horizontal
crystal
growth
along
(110)
plane.
Symmetric
Na–Na
cells
with
exhibit
notably
stable
for
over
5
000
cycles
at
high
current
density
mA
cm
−2
,
surpassing
previous
research.
Performance
improvement
is
also
demonstrated
full‐cell
configuration
an
3
V
2
(PO
4
)
O
F
cathode.
approach
offers
promising
solution
achieving
performance
levels
comparable
battery
technology.
Journal of Materials Chemistry A,
Год журнала:
2023,
Номер
11(19), С. 10155 - 10163
Опубликована: Янв. 1, 2023
A
stable
polythiourea-based
organic–inorganic
composite
film
was
constructed
to
form
Li
3
N,
2
S,
and
LiF
in
situ
at
the
LMA,
endowing
excellent
stability
Ni-rich
Li‖LiNi
0.88
Co
0.09
Mn
0.03
O
(NCM88)
cells.