Journal of the American Chemical Society,
Год журнала:
2025,
Номер
unknown
Опубликована: Фев. 26, 2025
Lithium-ion
batteries
(LIBs)
with
nonaqueous
liquid
electrolytes
are
prone
to
gas
generation
at
elevated
voltages
and
temperatures,
degrading
battery
performance
posing
serious
safety
risks.
Organosilicon
(OS)
additives
an
emerging
candidate
solution
for
gassing
problems
in
LIBs,
but
a
detailed
understanding
of
their
functional
mechanisms
remains
elusive.
In
this
work,
we
present
combined
computational
experimental
study
elucidate
the
gas-reducing
effects
OS
additives.
Cell
volume
measurements
chromatography–mass
spectrometry
reveal
that
can
substantially
reduce
evolution
particularly
CO2
regardless
source.
Through
density
theory
calculations,
identify
multiple
plausible
pathways
evolution,
including
(1)
nucleophile-induced
ring-opening
ethylene
carbonate
(EC)
subsequent
electro-oxidation
(2)
direct
lithium
(Li2CO3).
Correspondingly,
find
function
via
two
primary
mechanisms:
scavenging
nucleophiles
such
as
superoxide
(O2•–),
peroxide
(O22–),
ion
(CO32–);
oligomerization
oxide
dicarbonate
ion.
Moreover,
discover
possess
strong
coordination
affinity,
which
helps
further
nucleophilic
reaction
energies
hence
increases
nucleophile-scavenging
efficiency.
Finally,
provide
mechanistic
interpretation
enhanced
gas-reduction
observed
fluorinated
compounds,
corroborated
by
surface
analysis
results
from
X-ray
photoelectron
spectroscopy.
Our
offers
first
molecular-level
insights
into
how
contribute
reduced
formation
paving
way
improved
LIBs.
Chemical Reviews,
Год журнала:
2024,
Номер
unknown
Опубликована: Дек. 17, 2024
Electrochemical
batteries
play
a
crucial
role
for
powering
portable
electronics,
electric
vehicles,
large-scale
grids,
and
future
aircraft.
However,
key
performance
metrics
such
as
energy
density,
charging
speed,
lifespan,
safety
raise
significant
consumer
concerns.
Enhancing
battery
hinges
on
deep
understanding
of
their
operational
degradation
mechanisms,
from
material
composition
electrode
structure
to
pack
integration,
necessitating
advanced
characterization
methods.
These
methods
not
only
enable
improved
but
also
facilitate
early
detection
substandard
or
potentially
hazardous
before
they
cause
serious
incidents.
This
review
comprehensively
examines
the
principles,
applications,
challenges,
prospects
cutting-edge
techniques
commercial
batteries,
with
specific
focus
in
situ
operando
methodologies.
Furthermore,
it
explores
how
these
powerful
tools
have
elucidated
mechanisms
batteries.
By
bridging
gap
between
technologies,
this
aims
guide
design
more
sophisticated
experiments
models
studying
enhancement.
Advanced Science,
Год журнала:
2025,
Номер
unknown
Опубликована: Фев. 14, 2025
Proton
batteries
are
strong
contender
for
next-generation
energy
storage
due
to
their
high
safety
and
rapid
response.
However,
the
narrow
electrochemical
window
of
acidic
aqueous
electrolytes
limits
density
stability.
Here,
an
ionic
liquid
(IL)-based
electrolyte
(EMImOTf-H3PO4)
containing
H3PO4
in
polar
IL
solvent
1-ethyl-3-methylimidazolium
trifluoromethanesulfonate
(EMImOTf)
is
developed
stable
high-voltage
storage.
serving
as
a
proton
source
interacts
with
both
EMIm+
OTf-,
forming
intricate
hydrogen
bonding
network
that
effectively
prevents
decomposition
at
voltage.
The
half-cell
EMImOTf-H3PO4
pre-protonated
vanadium
hexacyanoferrate
(H-VHCF)
cathode
demonstrates
126%
improvement
Coulombic
efficiency
over
current
1
A
g-1.
fabricated
PTCDA/MXene//EMImOTf-H3PO4//H-VHCF
full
battery
achieves
operating
voltage
2
V
room
temperature,
surpassing
currently
reported
values
batteries.
After
30
000
cycles
5
g-1,
retains
86.1%
its
initial
capacity.
It
delivers
87.5
Wh
kg-1
power
30.6
kW
can
maintain
operation
across
temperature
range
110
°C
(-60
∼
50
°C).
These
findings
present
new
possibilities
all-weather
grid-scale
applications.
Journal of the American Chemical Society,
Год журнала:
2025,
Номер
unknown
Опубликована: Фев. 26, 2025
Lithium-ion
batteries
(LIBs)
with
nonaqueous
liquid
electrolytes
are
prone
to
gas
generation
at
elevated
voltages
and
temperatures,
degrading
battery
performance
posing
serious
safety
risks.
Organosilicon
(OS)
additives
an
emerging
candidate
solution
for
gassing
problems
in
LIBs,
but
a
detailed
understanding
of
their
functional
mechanisms
remains
elusive.
In
this
work,
we
present
combined
computational
experimental
study
elucidate
the
gas-reducing
effects
OS
additives.
Cell
volume
measurements
chromatography–mass
spectrometry
reveal
that
can
substantially
reduce
evolution
particularly
CO2
regardless
source.
Through
density
theory
calculations,
identify
multiple
plausible
pathways
evolution,
including
(1)
nucleophile-induced
ring-opening
ethylene
carbonate
(EC)
subsequent
electro-oxidation
(2)
direct
lithium
(Li2CO3).
Correspondingly,
find
function
via
two
primary
mechanisms:
scavenging
nucleophiles
such
as
superoxide
(O2•–),
peroxide
(O22–),
ion
(CO32–);
oligomerization
oxide
dicarbonate
ion.
Moreover,
discover
possess
strong
coordination
affinity,
which
helps
further
nucleophilic
reaction
energies
hence
increases
nucleophile-scavenging
efficiency.
Finally,
provide
mechanistic
interpretation
enhanced
gas-reduction
observed
fluorinated
compounds,
corroborated
by
surface
analysis
results
from
X-ray
photoelectron
spectroscopy.
Our
offers
first
molecular-level
insights
into
how
contribute
reduced
formation
paving
way
improved
LIBs.
