Lithium
(Li)-rich
Manganese
(Mn)-based
cathode
materials
are
considered
to
be
the
most
hopeful
for
next-generation
high-energy-density
Li
metal
batteries.
However,
rapid
capacity
fading
and
voltage
decaying
derived
from
phase
transformation
still
hinder
their
practical
application.
Herein,
we
developed
a
cation/anion
dual-doping
strategy
by
synchronically
incorporating
Zr4+
cation
F-
anion
boost
structural
stability
of
Li-rich
Mn-based
cathode.
The
strengthened
transition
metal-oxygen
bonds
raised
doping
effect
can
inhibit
release
oxygen
enhanced
electrochemical
reversibility
mitigate
anisotropic
lattice
distortion
stabilize
layered
structure.
Meanwhile,
dual
expands
distance
increases
vacancy
formation
energy,
thereby
improving
ion
diffusion
kinetics
stability.
As
result,
obtained
presents
an
excellent
initial
discharge
268.5
mAh
g-1
prolonged
cycle
lifespan
beyond
300
cycles.
A
stable
cycling
performance
under
high
areal
5.17
cm-2
with
low
negative/positive
electrode
ratio
1.93.
Our
provides
valuable
new
idea
properties
materials,
further
promoting
development
Solid-state
lithium-metal
batteries
(SSLMBs)
have
been
regarded
as
one
of
the
most
promising
battery
systems
due
to
their
high
energy
density
and
excellent
safety.
However,
low
ionic
conductivity
solid
electrolyte
(normally
<
1
mS
cm-1)
does
not
meet
practical
application
SSLMBs.
Herein,
we
propose
a
vertically-aligned
composite
electrolytes
(VA-CSE)
with
dual
Li+
transportation
paths:
dimensional
(1D)
Li+-transportation
highway
in
lithium
montmorillonite
(Li-MMT)
layer
along
aligned
poly
(vinylidene
fluoride-co-hexafluoropropylene)
(PVDF-HFP)
channels
unique
hopping
path
created
by
aggregated
ions
pairs
polymerized
vinyl
ethylene
carbonate-based
electrolyte.
This
Li-MMT/PVDF-HFP
(Li-MPSE)
exhibits
superionic
1.99
cm-1
transference
number
(0.73)
at
30
°C.
With
this
superior
Li-MPSE
electrolyte,
Li/LiFePO4
solid-state
stably
cycle
200
times
99.7%
capacity
retention
0.5
C
pouch
cell
also
presents
electrochemical
performance
Lithium
(Li)-rich
Manganese
(Mn)-based
cathode
materials
are
considered
to
be
the
most
hopeful
for
next-generation
high-energy-density
Li
metal
batteries.
However,
rapid
capacity
fading
and
voltage
decaying
derived
from
phase
transformation
still
hinder
their
practical
application.
Herein,
we
developed
a
cation/anion
dual-doping
strategy
by
synchronically
incorporating
Zr4+
cation
F-
anion
boost
structural
stability
of
Li-rich
Mn-based
cathode.
The
strengthened
transition
metal-oxygen
bonds
raised
doping
effect
can
inhibit
release
oxygen
enhanced
electrochemical
reversibility
mitigate
anisotropic
lattice
distortion
stabilize
layered
structure.
Meanwhile,
dual
expands
distance
increases
vacancy
formation
energy,
thereby
improving
ion
diffusion
kinetics
stability.
As
result,
obtained
presents
an
excellent
initial
discharge
268.5
mAh
g-1
prolonged
cycle
lifespan
beyond
300
cycles.
A
stable
cycling
performance
under
high
areal
5.17
cm-2
with
low
negative/positive
electrode
ratio
1.93.
Our
provides
valuable
new
idea
properties
materials,
further
promoting
development