Advanced Functional Materials,
Journal Year:
2023,
Volume and Issue:
33(15)
Published: Jan. 15, 2023
Abstract
The
theoretically
high‐energy‐density
lithium–sulfur
batteries
(LSBs)
are
seriously
limited
by
the
disadvantages
including
shuttle
effect
of
soluble
lithium
polysulfides
(LiPSs)
and
sluggish
sulfur
redox
kinetics,
especially
for
most
difficult
solid–solid
conversion
Li
2
S
to
S.
Herein,
a
multifunctional
catalytic
interlayer
improve
performance
LSBs
is
tried
introduce,
in
which
Fe
1–
x
S/Fe
3
C
nanoparticles
embedded
N/S
dual‐doped
carbon
network
(NSC)
composed
nanosheets
nanotubes
(the
final
product
named
as
FeSC@NSC).
well‐designed
3D
NSC
endows
with
satisfactory
LiPSs
capture‐catalytic
ability,
thus
ensuring
fast
reaction
kinetics
suppressing
shuttling.
density
functional
theory
calculations
disclose
mechanisms
that
FeSC@NSC
greatly
improves
liquid–solid
(LiPSs
)
unexpectedly
(Li
S)
one.
As
result,
based
on
can
achieve
high
specific
capacity
1118
mAh
g
−1
at
current
0.2
C,
relatively
stable
415
large
2.0
after
700
cycles
well
superior
rate
performance.
Advanced Materials,
Journal Year:
2022,
Volume and Issue:
35(10)
Published: Dec. 17, 2022
High-energy
and
long
cycle
lithium-sulfur
(Li-S)
pouch
cells
are
limited
by
the
insufficient
capacities
stabilities
of
their
cathodes
under
practical
electrolyte/sulfur
(E/S),
electrolyte/capacity
(E/C),
negative/positive
(N/P)
ratios.
Herein,
an
advanced
cathode
comprising
highly
active
Fe
single-atom
catalysts
(SACs)
is
reported
to
form
320.2
W
h
kg-1
multistacked
Li-S
with
total
capacity
≈1
A
level,
satisfying
low
E/S
(3.0),
E/C
(2.8),
N/P
(2.3)
ratios
high
sulfur
loadings
(8.4
mg
cm-2
).
The
high-activity
SAC
designed
manipulating
its
local
environments
using
electron-exchangeable
binding
(EEB)
sites.
Introducing
EEB
sites
two
different
types
S
species,
namely,
thiophene-like-S
(-S)
oxidized-S
(-SO2
),
adjacent
SACs
promotes
kinetics
Li2
redox
reaction
providing
additional
modulating
d-orbital
levels
via
electron
exchange
Fe.
-S
donates
electrons
SACs,
whereas
-SO2
withdraws
from
SACs.
Thus,
energy
level
can
be
modulated
/-S
site,
controlling
donating/withdrawing
characteristics.
This
desirable
electrocatalysis
maximized
intimate
contact
which
confined
together
in
porous
carbon.
Advanced Functional Materials,
Journal Year:
2023,
Volume and Issue:
33(42)
Published: Aug. 30, 2023
Abstract
The
serious
shuttle
effect
and
intrinsically
sluggish
oxidation–reduction
reaction
kinetics
of
polysulfides
severely
hinder
the
practical
commercialization
lithium–sulfur
(Li–S)
batteries.
Herein,
oxygen‐defect‐rich
WO
3−
x
–W
3
N
4
Mott–Schottky
heterojunctions
are
designed
as
efficient
catalysts.
Based
on
theoretical
calculations
comprehensive
experimental
characterization,
exhibits
a
lower
free
energy
change
(1.03
eV)
Li
2
S
decomposition
barrier
(0.92
than
W
,
which
significantly
enhances
sulfur
reduction
(SRR)
activity.
Furthermore,
relationship
between
catalytic
activity
gaps
in
d
p
bands
centers
(Δ
d–p
)
is
also
established,
with
low
Δ
heterojunction
leading
to
antibonding
state
energy,
promotes
electron
transfer
interfacial
redox
kinetics.
Oxygen
vacancies
can
improve
without
affecting
adsorption.
Hence,
Li–S
battery
using
@CC/S
exhibited
outstanding
rate
duration
performance
(913.9
mAh
g
–1
at
C,
stable
400
cycles
1
C).
Impressively,
achieves
high
areal
capacity
5.0
cm
−2
under
loading
4.98
mg
.
Advanced Functional Materials,
Journal Year:
2023,
Volume and Issue:
33(15)
Published: Jan. 15, 2023
Abstract
The
theoretically
high‐energy‐density
lithium–sulfur
batteries
(LSBs)
are
seriously
limited
by
the
disadvantages
including
shuttle
effect
of
soluble
lithium
polysulfides
(LiPSs)
and
sluggish
sulfur
redox
kinetics,
especially
for
most
difficult
solid–solid
conversion
Li
2
S
to
S.
Herein,
a
multifunctional
catalytic
interlayer
improve
performance
LSBs
is
tried
introduce,
in
which
Fe
1–
x
S/Fe
3
C
nanoparticles
embedded
N/S
dual‐doped
carbon
network
(NSC)
composed
nanosheets
nanotubes
(the
final
product
named
as
FeSC@NSC).
well‐designed
3D
NSC
endows
with
satisfactory
LiPSs
capture‐catalytic
ability,
thus
ensuring
fast
reaction
kinetics
suppressing
shuttling.
density
functional
theory
calculations
disclose
mechanisms
that
FeSC@NSC
greatly
improves
liquid–solid
(LiPSs
)
unexpectedly
(Li
S)
one.
As
result,
based
on
can
achieve
high
specific
capacity
1118
mAh
g
−1
at
current
0.2
C,
relatively
stable
415
large
2.0
after
700
cycles
well
superior
rate
performance.