Angewandte Chemie International Edition,
Journal Year:
2023,
Volume and Issue:
62(39)
Published: July 24, 2023
The
atom-cluster
interaction
has
recently
been
exploited
as
an
effective
way
to
increase
the
performance
of
metal-nitrogen-carbon
catalysts
for
oxygen
reduction
reaction
(ORR).
However,
rational
design
such
and
understanding
their
structure-property
correlations
remain
a
great
challenge.
Herein,
we
demonstrate
that
introduction
adjacent
metal
(M)-N4
single
atoms
(SAs)
could
significantly
improve
ORR
well-screened
Fe
atomic
cluster
(AC)
catalyst
by
combining
density
functional
theory
(DFT)
calculations
experimental
analysis.
DFT
studies
suggest
Cu-N4
SAs
act
modulator
assist
O2
adsorption
cleavage
O-O
bond
on
AC
active
center,
well
optimize
release
OH*
intermediates
accelerate
whole
kinetic.
depositing
with
nitrogen
doped
mesoporous
carbon
nanosheet
are
then
constructed
through
universal
interfacial
monomicelles
assembly
strategy.
Consistent
theoretical
predictions,
resultant
exhibits
outstanding
half-wave
potential
0.92
eV
in
alkali
0.80
acid,
high
power
214.8
mW
cm-2
zinc
air
battery.
This
work
provides
novel
strategy
precisely
tuning
atomically
dispersed
poly-metallic
centers
electrocatalysis.
ACS Nano,
Journal Year:
2022,
Volume and Issue:
16(10), P. 15734 - 15759
Published: Oct. 12, 2022
Because
of
their
high
energy
density,
low
cost,
and
environmental
friendliness,
lithium–sulfur
(Li–S)
batteries
are
one
the
potential
candidates
for
next-generation
energy-storage
devices.
However,
they
have
been
troubled
by
sluggish
reaction
kinetics
insoluble
Li2S
product
capacity
degradation
because
severe
shuttle
effect
polysulfides.
These
problems
overcome
introducing
transition
metal
compounds
(TMCs)
as
catalysts
into
interlayer
modified
separator
or
sulfur
host.
This
review
first
introduces
mechanism
redox
reactions.
The
methods
studying
TMC
in
Li–S
provided.
Then,
recent
advances
TMCs
(such
oxides,
sulfides,
selenides,
nitrides,
phosphides,
carbides,
borides,
heterostructures)
some
helpful
design
modulation
strategies
highlighted
summarized.
At
last,
future
opportunities
toward
presented.
Angewandte Chemie International Edition,
Journal Year:
2023,
Volume and Issue:
62(15)
Published: Feb. 18, 2023
Herein,
we
successfully
construct
bifunctional
electrocatalysts
by
synthesizing
atomically
dispersed
Fe-Se
atom
pairs
supported
on
N-doped
carbon
(Fe-Se/NC).
The
obtained
Fe-Se/NC
shows
a
noteworthy
oxygen
catalytic
performance
with
low
potential
difference
of
0.698
V,
far
superior
to
that
reported
Fe-based
single-atom
catalysts.
theoretical
calculations
reveal
p-d
orbital
hybridization
around
the
leads
remarkably
asymmetrical
polarized
charge
distributions.
based
solid-state
rechargeable
Zn-air
batteries
(ZABs-Fe-Se/NC)
present
stable
charge/discharge
200
h
(1090
cycles)
at
20
mA
cm-2
25
°C,
which
is
6.9
times
ZABs-Pt/C+Ir/C.
At
extremely
temperature
-40
ZABs-Fe-Se/NC
displays
an
ultra-robust
cycling
741
(4041
1
,
about
11.7
More
importantly,
could
be
operated
for
133
(725
even
5
°C.
Chemical Society Reviews,
Journal Year:
2023,
Volume and Issue:
52(17), P. 6139 - 6190
Published: Jan. 1, 2023
Sustainable
zinc-air
batteries
(ZABs)
are
considered
promising
energy
storage
devices
owing
to
their
inherent
safety,
high
density,
wide
operating
temperature
window,
environmental
friendliness,
etc.,
showing
great
prospect
for
future
large-scale
applications.
Thus,
tremendous
efforts
have
been
devoted
addressing
the
critical
challenges
associated
with
sustainable
ZABs,
aiming
significantly
improve
efficiency
and
prolong
operation
lifespan.
The
growing
interest
in
ZABs
requires
in-depth
research
on
oxygen
electrocatalysts,
electrolytes,
Zn
anodes,
which
not
systematically
reviewed
date.
In
this
review,
fundamentals
of
electrocatalysts
air
cathodes,
physicochemical
properties
ZAB
issues
strategies
stabilization
anodes
summarized
from
perspective
fundamental
characteristics
design
principles.
Meanwhile,
significant
advances
situ/operando
characterization
highlighted
provide
insights
into
reaction
mechanism
dynamic
evolution
electrolyte|electrode
interface.
Finally,
several
thoughts
perspectives
provided
regarding
opportunities
ZABs.
Therefore,
review
provides
a
thorough
understanding
advanced
chemistry,
hoping
that
timely
comprehensive
can
shed
light
upcoming
horizons
prosperous
area.
eScience,
Journal Year:
2022,
Volume and Issue:
2(5), P. 453 - 466
Published: Sept. 1, 2022
Zinc–air
batteries
(ZABs)
are
expected
to
be
some
of
the
most
promising
power
sources
for
wearable
and
portable
electronic
devices
have
received
widespread
research
interest.
As
an
ion
conductor
connecting
anodes
cathodes,
electrolyte
is
critical
overall
performance
ZABs
(e.g.,
energy
density,
rechargeability,
operating
voltage).
Compared
with
liquid
electrolytes,
polymer-based
electrolytes
superior
characteristics
ZABs,
such
as
negligible
leakage,
three-phase
interface
stabilization,
dendrite
suppression.
In
this
perspective,
we
focus
on
recent
progress
in
ZABs.
After
a
brief
introduction
emphasize
development
terms
their
intrinsic
properties
interfacial
chemistry.
Finally,
challenges
viable
strategies
proposed
We
hope
that
work
will
provide
useful
guidance
spur
high-performance
based
advanced
electrolytes.
Advanced Functional Materials,
Journal Year:
2023,
Volume and Issue:
34(4)
Published: Sept. 27, 2023
Abstract
The
large‐scale
deployment
of
aqueous
Zn‐ion
batteries
is
hindered
by
Zn
anode
instability
including
surface
corrosion,
hydrogen
gas
evolution,
and
irregular
deposition.
To
tackle
these
challenges,
a
polyhydroxylated
organic
molecular
additive,
trehalose,
incorporated
to
refine
the
solvation
structure
promote
planar
Within
regions
involving
hydroxy
groups
participate
in
reconstruction
bond
networks,
which
increases
overpotential
for
water
decomposition
reaction.
Moreover,
at
metal–molecule
interface,
chemisorption
trehalose
onto
zinc
enhances
corrosion
resistance
facilitates
deposition
manner.
optimized
electrolyte
significantly
improves
striping/plating
reversibility
maintains
stable
potentials
over
1600
h
5
mA
cm
−2
with
cutoff
capacity
1
symmetric
cells.
When
combined
MnO
2
cathode,
assembled
coin
cell
retains
≈89%
its
after
1000
cycles.
This
molecule
emphasizing
role
molecules
fine‐tuning
structures
anode/electrolyte
interfaces,
holds
promise
enhancing
various
metal
batteries.
Angewandte Chemie International Edition,
Journal Year:
2022,
Volume and Issue:
61(49)
Published: Oct. 14, 2022
Construction
of
catalytic
covalent
organic
frameworks
(COFs)
for
oxygen
reduction
reaction
(ORR)
and
evolution
(OER)
is
significant
but
rarely
demonstrated.
In
this
work,
we
have
first
constructed
bifunctional
COFs
towards
ORR
OER
by
integrating
diarylamine
derivatives
into
the
Co-porphyrin
based
frameworks.
Both
new
(CoTAPP-PATA-COF
CoTAPP-BDTA-COF)
good
ordered
structures,
high
surface
areas,
robust
chemical
stability.
The
units,
as
a
typical
electron
donor
redox-active
cores,
promote
intramolecular
transport
along
improve
electrochemically
active
areas.
Thus,
showed
higher
activities
than
that
COF
without
units.
CoTAPP-PATA-COF
had
halfwave
potential
0.80
V
ORR,
delieved
an
overpotential
420
mV
in
0.1
M
KOH.
theoretical
calculation
revealed
introducing
unites
improved
electrocatalysis.
Energy & Environmental Science,
Journal Year:
2023,
Volume and Issue:
16(6), P. 2629 - 2636
Published: Jan. 1, 2023
A
novel
N,O
symmetric
double-coordinated
configuration
of
unsaturated
Fe
single
atoms
confirmed
within
a
graphene
framework
(Fe–N,O/G)
is
demonstrated
experimentally
and
theoretically
for
highly
active
durable
ORR
catalyst
in
Zn-air
batteries.
Advanced Functional Materials,
Journal Year:
2022,
Volume and Issue:
33(8)
Published: Dec. 14, 2022
Abstract
High‐performance
rechargeable
Zn‐air
batteries
with
long‐life
stability
are
desirable
for
power
applications
in
electric
vehicles.
The
key
component
of
the
is
bifunctional
oxygen
electrocatalyst,
however,
designing
a
electrocatalyst
high
intrinsic
reversibility
and
durability
challenge.
Through
density
functional
theory
calculations,
it
found
that
catalytic
activity
originated
from
electronic
geometric
coordination
structures
synergistic
effect
Fe
Co
dual‐sites
metal‐N
4
environment,
assisting
stronger
hybridization
orbitals
between
(
dxz,
dz
2
)
OO*
px,
pz
),
thus
making
O
active
ability
site.
These
findings
enable
to
development
fancy
dual
single‐atom
catalyst
comprising
adjacent
FeN
CoN
sites
on
N‐doped
carbon
matrix
(FeCo‐NC).
FeCo‐NC
exhibits
extraordinary
activities
reduction
evolution
reaction
(ORR/OER),
which
displays
half‐wave
potential
(0.893
V)
ORR,
low
overpotential
(343
mV)
at
10
mA
cm
−2
OER.
assembled
air‐electrode
works
well
flexible
solid‐state
battery
specific
capacity
747.0
mAh
g
−1
,
long‐time
more
than
400
h
(30
°C),
also
superior
performance
extreme
temperatures
(−30
°C–60
°C).
Angewandte Chemie International Edition,
Journal Year:
2022,
Volume and Issue:
61(44)
Published: Sept. 12, 2022
As
a
key
component
of
batteries,
the
electrolyte
determines
ion
transport
and
interface
chemistry
cathode
anode.
In
this
work,
we
develop
dual-network
structured
hydrogel
composed
polyacrylamide
(PAM),
sodium
alginate
(SA)
potassium
iodide
(KI)
for
solid-state
zinc-air/iodide
hybrid
batteries.
The
assembled
battery
shows
excellent
renewability
long
cycling
life
110
h
with
high
energy
efficiency
80
%.
ion-crosslinked
structure
endows
material
improved
mechanical
strength
increased
ionic
conductivity.
More
importantly,
introduction
iodine
species
not
only
offers
more
favorable
cathodic
kinetics
iodide/iodate
redox
than
oxygen
electrocatalysis
but
also
regulates
solvation
zinc
ions
to
ensure
better
stability.
This
work
provides
significant
concepts
developing
novel
electrolytes
realize
high-performance
devices
technologies.