Abstract
Rational
design
and
construction
of
oxygen
reduction
reaction
(ORR)
electrocatalysts
with
high
activity,
good
stability,
low
price
are
essential
for
the
practical
applications
renewable
energy
conversion
devices,
such
as
metal‐air
batteries.
Electronic
modification
through
constructing
metal/semiconductor
Schottky
heterointerface
represents
a
powerful
strategy
to
enhance
electrochemical
performance.
Herein,
we
demonstrate
concept
electrocatalyst
composed
uniform
Co
nanoparticles
in
situ
anchored
on
carbon
nanotubes
aligned
nanosheets
(denoted
Co@N‐CNTs/NSs
hereafter)
toward
ORR.
Both
experimental
findings
theoretical
simulation
testify
that
rectifying
contact
could
impel
voluntary
electron
flow
from
N‐CNTs/NSs
create
an
internal
electric
field,
thereby
boosting
transfer
rate
improving
intrinsic
activity.
As
consequence,
deliver
outstanding
ORR
impressive
long‐term
durability,
excellent
methanol
tolerance,
performance
air‐cathode
Zn‐air
The
may
provide
innovational
inspirations
synthesis
advanced
catalysts
sustainable
fields.
Advanced Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Авг. 27, 2024
Abstract
Due
to
the
slow
dynamics
of
mass
and
charge
transfer
at
Zn|electrolyte
interface,
stable
operation
Zn–air
batteries
(ZABs)
is
challenging,
especially
low
temperature.
Herein,
inspired
by
cell
membrane,
a
hydrophilic‐hydrophobic
dual
modulated
interface
constructed.
This
amphiphilic
design
enables
quasi‐solid‐state
(QSS)
ZABs
display
long‐term
cyclability
180
h@50
mA
cm
−2
25
°C.
Moreover,
record‐long
time
173
h@4
−60
°C
also
achieved,
which
almost
threefolds
untreated
QSS
ZABs.
Control
experiments
(in
situ)
characterization
reveal
that
growth
insulating
ZnO
passivation
layers
largely
inhibited
tuned
hydrophilic–hydrophobic
behavior.
Thus,
enhanced
dynamic
Zn
2+
from
attained.
As
an
extension,
Al‐air
(AABs)
with
bioinspired
show
unprecedented
discharge
stability
420
h@1
‐40
°C,
about
two
times
AABs.
bioinspired‐hydrophilic‐hydrophobic
modulation
strategy
may
provide
reference
for
energy
transform
storage
devices
broad
temperature
adaptability.
Advanced Functional Materials,
Год журнала:
2024,
Номер
34(28)
Опубликована: Фев. 24, 2024
Abstract
It
is
important
to
tune
the
coordination
configuration
of
dual‐atom
catalyst
(DAC),
especially
in
first
sphere,
render
high
intrinsic
catalytic
activities
for
oxygen
reduction/evolution
reactions
(ORR/OER).
Herein,
a
type
atomically
dispersed
and
boron‐coordinated
DAC
structure,
namely,
FeN
4
B‐NiN
B
dual
sites,
reported.
In
this
incorporation
boron
into
sphere
/NiN
atomic
sites
regulates
its
geometry
electronic
structure
by
forming
“Fe‐B‐N”
“Ni‐B‐N”
bridges.
The
exhibits
much
enhanced
ORR
OER
property
compared
‐NiN
counterparts.
Density
functional
theory
calculations
reveal
that
boron‐induced
charge
transfer
asymmetric
distributions
central
Fe/Ni
atoms
optimize
adsorption
desorption
behavior
ORR/OER
intermediates
reduce
activation
energy
potential‐determining
step.
Zinc‐air
batteries
employing
cathode
exhibit
maximum
power
density
(236.9
mW
cm
−2
)
stable
cyclability
up
1100
h.
result
illustrates
pivotal
role
first‐coordination
DACs
tuning
electrochemical
conversion
storage
activities.
Advanced Functional Materials,
Год журнала:
2024,
Номер
34(48)
Опубликована: Июль 5, 2024
Abstract
Cobalt
single
atom
catalysts
(SACs)
have
exhibited
promising
performance
in
both
the
oxygen
reduction
reaction
(ORR)
and
evolution
(OER),
positioning
them
as
potential
dual‐functional
for
Zn‐air
battery.
However,
long‐standing
challenge
lies
achieving
satisfactory
dual‐functionality
stability
of
these
SACs.
In
this
study,
to
optimize
4e
‒
ORR
performance,
boron
(B)
atoms
are
employed
with
low
electronegativity
regulate
structure
Co–N–C
catalytic
center.
This
resulted
formation
an
asymmetrically
coordinated
Co
metal
center
catalyst
(Co‐N
3
B).
Compared
Co‐N
4
,
B
lower
free
energy
stronger
adsorption
toward
*
O
species,
effectively
suppressing
2e
pathway
at
cobalt
site
preventing
corrosion
induced
by
hydrogen
peroxide
(H
2
)
reactions,
thereby
enhancing
stability.
situ
attenuated
total
reflectance
surface‐enhanced
infrared
absorption
spectroscopy
(ATR‐SEIRAS)
further
validated
excellent
interaction
between
active
centers
intermediates.
Furthermore,
self‐made
rechargeable
zinc‐air
battery
demonstrated
remarkable
discharge
peak
power
density
(≈253
mW
cm
‒2
),
(≈819
mAh
g
‒1
cyclic
exceeding
110
h.
study
provides
new
insights
into
constructing
atomic‐level
precision
offers
strong
references
practical
applications
storage
convension
electrocatalysts.
Advanced Energy Materials,
Год журнала:
2023,
Номер
13(38)
Опубликована: Авг. 7, 2023
Abstract
The
performance
optimization
of
single‐atom
catalysts
(SACs)
is
important
but
remains
challenging.
Taking
advantage
accompanying
in
situ
formation
atomic
clusters
(ACs)/nanoparticles
(NPs)
during
the
preparation
SACs
can
be
a
promising
solution.
coupled
ACs/NPs
and
single
atoms
(SAs)
highly
efficient
catalyzing
various
reactions
(e.g.,
oxygen
reduction
reaction
(ORR),
hydrogen
evolution
(HER),
CO
2
(CO
RR),
N
oxidation
(NOR),
etc),
showing
superior
activity,
selectivity,
stability.
mechanisms
mainly
categorized
as
intensified
SAs,
SAs
ACs/NPs,
proceeding
on
both
SAs.
proposed
may
applicable
to
rationalize
excellent
consisting
In
end,
existing
issues
further
development
directions
are
put
forward.
This
review
expected
simultaneously
contribute
application
in‐depth
understanding
catalysis
(SAC).
Energy & Environmental Science,
Год журнала:
2023,
Номер
16(12), С. 5663 - 5687
Опубликована: Янв. 1, 2023
This
review
summarizes
recent
progress
and
prospects
of
catalysts
containing
metal
single-atom
(M
1
)
nano-aggregates
(MNAs,
particles
or
clusters),
which
promise
to
combine
the
merits
SACs
MNA-based
for
efficient
electrocatalysis.
Abstract
Designing
cost‐efffective
electrocatalysts
for
the
oxygen
evolution
reaction
(OER)
holds
significant
importance
in
progression
of
clean
energy
generation
and
efficient
storage
technologies,
such
as
water
splitting
rechargeable
metal–air
batteries.
In
this
work,
an
OER
electrocatalyst
is
developed
using
Ni
Fe
precursors
combination
with
different
proportions
graphene
oxide.
The
catalyst
synthesis
involved
a
rapid
reduction
process,
facilitated
by
adding
sodium
borohydride,
which
successfully
formed
NiFe
nanoparticle
nests
on
support
(NiFe
NNG).
incorporation
enhances
catalytic
activity,
electron
transferability,
electrical
conductivity
NiFe‐based
catalyst.
NNG
exhibits
outstanding
performance,
characterized
low
overpotential
292.3
mV
Tafel
slope
48
dec
−1
,
achieved
at
current
density
10
mA
cm
−
2
.
Moreover,
remarkable
stability
over
extended
durations.
performance
par
that
commercial
IrO
alkaline
media.
Such
superb
can
be
attributed
to
synergistic
effect
between
graphene,
arises
from
their
large
surface
area
intrinsic
activity.
excellent
electrochemical
properties
hold
great
promise
further
applications
conversion
devices.