Abstract
A
promising
anode
material
for
Li‐ion
batteries,
silicon
(Si)
suffers
from
volume
expansion‐induced
pulverization
and
solid
electrolyte
interface
(SEI)
instability.
Microscale
Si
with
high
tap
density
initial
Coulombic
efficiency
(ICE)
has
become
a
more
anticipated
choice,
but
it
will
exacerbate
the
above
issues.
In
this
work,
polymer
polyhedral
oligomeric
silsesquioxane‐lithium
bis
(allylmalonato)
borate
(PSLB)
is
constructed
by
in
situ
chelation
on
microscale
surfaces
via
click
chemistry.
This
polymerized
nanolayer
an
“organic/inorganic
hybrid
flexible
cross‐linking”
structure
that
can
accommodate
change
of
Si.
Under
stable
framework
formed
PSLB,
large
number
oxide
anions
chain
segment
preferentially
adsorb
LiPF
6
further
induce
integration
inorganic‐rich,
dense
SEI,
which
improves
mechanical
stability
SEI
provides
accelerated
kinetics
Li
+
transfer.
Therefore,
Si4@PSLB
exhibits
significantly
enhanced
long‐cycle
performance.
After
300
cycles
at
1
g
−1
,
still
provide
specific
capacity
1083
mAh
.
Cathode‐coupled
LiNi
0.9
Co
0.05
Mn
O
2
(NCM90)
full
cell
retains
80.8%
its
after
150
0.5
C.
Angewandte Chemie International Edition,
Год журнала:
2024,
Номер
unknown
Опубликована: Окт. 12, 2024
Hydrometallurgy
remains
a
major
challenge
to
simplify
its
complex
separation
and
precipitation
processes
for
spent
lithium-ion
batteries
(LIBs).
Herein,
we
propose
Fischer-lactonization-driven
mechanism
the
cascade
reaction
of
leaching
chelation
LIBs.
Citric
acid
undergoes
two-step
dissociation
carboxylic
(-COOH)
complexes
with
leached
metal
ion,
while
residual
-COOH
is
attacked
by
H
protons
form
protonated
carboxyl
ion
(-COO
-).
Subsequently,
lone
pair
electrons
in
hydroxyl
same
molecule
attack
carbon
atom
-COO
-
facilitate
ester
bonding,
leading
formation
lactonized
gel.
The
rates
Li,
Ni,
Co
Mn
are
99.3,
99.1,
99.5
99.2
%,
respectively.
regenerated
monocrystalline
LiNi
Advanced Functional Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Апрель 1, 2025
Abstract
Direct
regeneration
of
spent
lithium
batteries
(LIBs)
cathodes
has
emerged
as
a
transformative
regimen
to
address
the
urgent
need
for
sustainable
recycling
methods
and
mitigate
critical
shortage
metal
resources
driven
by
escalating
LIB
demand.
Unlike
conventional
focused
on
extraction
separation,
direct
restores
functionality
cathode
in
situ,
streamlining
process
enhancing
efficiency.
Effective
necessitates
comprehensive
understanding
failure
mechanisms
pretreatment
processes.
Critical
strategies
include
reducing
(Li)
migration
barrier
enable
complete
reinsertion
into
structure
minimizing
Li‐transition
anti‐site
defects
reconstruct
lattice.
This
review
summarizes
advancements
mechanisms,
techniques,
cathode,
emphasizing
principles
innovations
regeneration.
By
evaluating
advantages
limitations
current
approaches,
opportunities
are
identified
innovation
overcome
existing
challenges.
Future
research
priorities
proposed
advance
technologies,
fostering
more
efficient
systems.
Abstract
A
promising
anode
material
for
Li‐ion
batteries,
silicon
(Si)
suffers
from
volume
expansion‐induced
pulverization
and
solid
electrolyte
interface
(SEI)
instability.
Microscale
Si
with
high
tap
density
initial
Coulombic
efficiency
(ICE)
has
become
a
more
anticipated
choice,
but
it
will
exacerbate
the
above
issues.
In
this
work,
polymer
polyhedral
oligomeric
silsesquioxane‐lithium
bis
(allylmalonato)
borate
(PSLB)
is
constructed
by
in
situ
chelation
on
microscale
surfaces
via
click
chemistry.
This
polymerized
nanolayer
an
“organic/inorganic
hybrid
flexible
cross‐linking”
structure
that
can
accommodate
change
of
Si.
Under
stable
framework
formed
PSLB,
large
number
oxide
anions
chain
segment
preferentially
adsorb
LiPF
6
further
induce
integration
inorganic‐rich,
dense
SEI,
which
improves
mechanical
stability
SEI
provides
accelerated
kinetics
Li
+
transfer.
Therefore,
Si4@PSLB
exhibits
significantly
enhanced
long‐cycle
performance.
After
300
cycles
at
1
g
−1
,
still
provide
specific
capacity
1083
mAh
.
Cathode‐coupled
LiNi
0.9
Co
0.05
Mn
O
2
(NCM90)
full
cell
retains
80.8%
its
after
150
0.5
C.