ACS Applied Energy Materials,
Journal Year:
2023,
Volume and Issue:
6(14), P. 7317 - 7322
Published: June 30, 2023
The
commercialization
of
rechargeable
Zn–air
batteries
(ZABs)
relies
heavily
on
the
development
cost-effective
and
highly
durable
bifunctional
electrocatalysts
that
can
promote
both
oxygen
reduction
reaction
(ORR)
evolution
(OER).
Transition-metal
phosphides-based
carbon
(TMPs/C)
composites
have
recently
been
acknowledged
as
efficient
catalysts,
yet
successful
construction
TMPs/C
still
remains
a
formidable
challenge.
Here,
we
report
dots
(CDs)-assisted
approach
to
efficiently
fabricate
CoP/C
nanocomposites
with
fine
microstructures
acting
active
electrocatalyst
for
ORR
OER.
CDs
act
stable
platform
adsorb
immobilize
Co
precursors,
obstructing
coalescence
small
CoP
particles
during
pyrolysis
eventually
ensuring
formation
microstructure,
where
carbon-encapsulated
dense
are
uniformly
distributed
nanosheets
(CoP@C/CNSs).
ZAB
assembled
using
CoP@C/CNSs
electrode
expresses
excellent
performance
high
power
density
180.1
mW
cm–2,
relatively
specific
capacity
(916
mA
h
g–1),
long
cycling
life
over
80
at
10
cm–2.
catalyst
such
configuration
is
anticipated
provide
practical
solution
production
storage
clean
energy.
Advanced Materials,
Journal Year:
2023,
Volume and Issue:
35(36)
Published: May 18, 2023
Abstract
The
electronic
structure
of
transition
metal
complexes
can
be
modulated
by
replacing
partial
ion
to
obtain
tuned
intrinsic
oxygen
reduction
reaction
(ORR)
or
evolution
(OER)
electrocatalytic
activity.
However,
the
anion‐modulated
ORR
activity
is
still
unsatisfactory,
and
construction
hetero‐anionic
remains
challenging.
Herein,
an
atomic
doping
strategy
presented
prepare
CuCo
2
O
4‐x
S
x
/NC‐2
(CCSO/NC‐2)
as
electrocatalysts,
structrual
characterization
results
favorably
demonstrate
substitution
atoms
for
in
CCSO/NC‐2,
which
shows
excellent
catalytic
performance
durability
OER
0.1
m
KOH.
In
addition,
catalyst
assembled
Zinc–air
battery
with
open
circuit
potential
1.43
V
maintains
after
300
h
cyclic
stability.
Theoretical
calculations
differential
charges
illustrate
that
optimizes
kinetics
promotes
electron
redistribution.
superior
CCSO/NC‐2
catalysis
mainly
due
its
unique
modulation
main
body.
introduction
CoO
covalency
constructs
a
fast
transport
channel,
thus
optimizing
adsorption
degree
active
site
Co
intermediates.
Angewandte Chemie International Edition,
Journal Year:
2023,
Volume and Issue:
62(28)
Published: May 4, 2023
Highly-active
and
low-cost
bifunctional
electrocatalysts
for
oxygen
reduction
evolution
are
essential
in
rechargeable
metal-air
batteries,
single
atom
catalysts
with
Fe-N-C
promising
candidates.
However,
the
activity
still
needs
to
be
boosted,
origination
of
spin-related
catalytic
performance
is
uncertain.
Herein,
an
effective
strategy
regulate
local
spin
state
through
manipulating
crystal
field
magnetic
proposed.
The
atomic
Fe
can
regulated
from
low
intermediate
high
spin.
cavitation
dxz
dyz
orbitals
FeIII
optimize
O2
adsorption
promote
rate-determining
step
(*O2
*OOH).
Benefiting
these
merits,
electrocatalyst
displays
highest
electrocatalytic
activities.
Furthermore,
Fe-N-C-based
zinc-air
battery
a
power
density
170
mW
cm-2
good
stability.
Journal of the American Chemical Society,
Journal Year:
2023,
Volume and Issue:
145(34), P. 18992 - 19004
Published: Aug. 21, 2023
An
AB2X4
spinel
structure,
with
tetrahedral
A
and
octahedral
B
sites,
is
a
paradigmatic
class
of
catalysts
several
possible
geometric
configurations
numerous
applications,
including
polysulfide
conversion
in
metal–sulfur
batteries.
Nonetheless,
the
influence
configuration
composition
on
mechanisms
catalysis
precise
manner
which
facilitate
polysulfides
remain
unknown.
To
enable
controlled
exposure
single
active
configurations,
herein,
Cotd2+
Cooh3+
Co3O4
for
sodium
are
large
part
replaced
by
Fetd2+
Feoh3+,
respectively,
generating
FeCo2O4
CoFe2O4.
Through
an
examination
electrochemical
activation
energies,
characterization
symmetric
cells,
theoretical
calculations,
we
determine
that
serves
as
site
breaking
S–S
bonds,
while
functions
formation
S–Na
bonds.
The
current
study
underlines
subtle
relationship
between
activity
catalysts,
providing
unique
insights
rational
development
improved
optimizing
their
atomic
configuration.
Angewandte Chemie International Edition,
Journal Year:
2024,
Volume and Issue:
63(33)
Published: May 27, 2024
Triggering
the
lattice
oxygen
oxidation
mechanism
is
crucial
for
improving
evolution
reaction
(OER)
performance,
because
it
could
bypass
scaling
relation
limitation
associated
with
conventional
adsorbate
through
direct
formation
of
oxygen-oxygen
bond.
High-valence
transition
metal
sites
are
favorable
activating
oxygen,
but
deep
pre-catalysts
suffers
from
a
high
thermodynamic
barrier.
Here,
taking
advantage
Jahn-Teller
(J-T)
distortion
induced
structural
instability,
we
incorporate
high-spin
Mn
Angewandte Chemie International Edition,
Journal Year:
2024,
Volume and Issue:
63(17)
Published: March 1, 2024
Abstract
Traditional
H
2
O
cleavage
mediated
by
macroscopic
electron
transfer
(MET)
not
only
has
low
utilization
of
,
but
also
sacrifices
the
stability
catalysts.
We
present
a
non‐redox
hydroxyl‐enriched
spinel
(CuFe
4
)
catalyst
with
dual
Lewis
acid
sites
to
realize
homolytic
.
The
results
systematic
experiments,
in
situ
characterizations,
and
theoretical
calculations
confirm
that
tetrahedral
Cu
optimal
acidity
strong
delocalization
can
synergistically
elongate
O−O
bonds
(1.47
Å
→
1.87
Å)
collaboration
adjacent
bridging
hydroxyl
(another
site).
As
result,
free
energy
is
decreased
(1.28
eV
0.98
eV).
be
efficiently
split
into
⋅OH
induced
CuFe
without
MET,
which
greatly
improves
(65.2
%,
nearly
times
than
traditional
catalysts).
system
assembled
affords
exceptional
performance
for
organic
pollutant
elimination.
scale‐up
experiment
using
continuous
flow
reactor
realizes
long‐term
(up
600
mL),
confirming
tremendous
potential
practical
applications.
Nature Communications,
Journal Year:
2024,
Volume and Issue:
15(1)
Published: Feb. 15, 2024
Abstract
As
inspired
by
the
Mn
4
CaO
5
oxygen
evolution
center
in
nature,
Mn-based
electrocatalysts
have
received
overwhelming
attention
for
water
oxidation.
However,
understanding
of
detailed
reaction
mechanism
has
been
a
long-standing
problem.
Herein,
homologous
KMnPO
and
•H
2
O
with
4-coordinated
6-coordinated
centers,
respectively,
are
prepared.
The
two
catalysts
constitute
an
ideal
platform
to
study
structure-performance
correlation.
presence
Mn(III),
Mn(IV),
Mn(V)
intermediate
species
identified
during
Mn(V)=O
is
demonstrated
be
substance
O−O
bond
formation.
In
O,
coordination
structure
did
not
change
significantly
,
changed
from
[MnO
]
5-coordinated
motif,
which
displays
triangular
biconical
configuration.
flexibility
thermodynamically
favored
retaining
Mn(III)−OH
generating
Mn(V)=O.
at
equilibrium
Mn(IV)=O,
concentration
determines
intrinsic
activity
This
provides
clear
picture
oxidation
on
systems.
Advanced Functional Materials,
Journal Year:
2024,
Volume and Issue:
34(36)
Published: March 10, 2024
Abstract
The
compositing
strategy
offers
great
potential
in
designing
bifunctional
oxygen
electrocatalysts
for
Zn–air
batteries.
Recent
reports
reveal
that
the
couple
of
RuO
2
,
serving
as
a
benchmark
evolution
reaction
(OER)
catalyst,
with
other
reduction
(ORR)
catalysts
is
wise
choice
to
build
highly
efficient
electrocatalysts.
However,
design
criteria
ORR
and
OER
activities
‐based
composite
are
still
unclear.
Herein,
series
transition
metal
(Fe,
Co,
Mn,
Ni)‐doped
spinel
oxides
designed
support
nanorods
exploring
mechanism.
Through
advanced
technology,
it
considered
increasing
content
binding
energy
Co
3+
enhancing
oxidation
state
Ru
4+
an
promote
/Co‐based
oxide
catalysts.
It
found
coupling
Mn‐doping
3
O
4
(CMO)
supports
can
induce
highest
catalytic
ORR/OER
excellent
performance
rechargeable
Operando
electrochemical
impedance
spectroscopy
theoretical
calculation
further
prove
synergistic
effect
between
CMO
originated
from
overflow
overcome
large
barrier
desorption
on
during
adsorption
ORR.
