Advanced Functional Materials,
Год журнала:
2023,
Номер
34(3)
Опубликована: Окт. 5, 2023
Abstract
The
regulation
of
electronic
structure
is
intricately
linked
to
the
intrinsic
activity
oxygen
reduction.
Herein,
a
strategy
for
modulation
induced
by
bimetallic
push–pull
effects
in
dual‐atom
catalysts
(Fe,Ni/N‐C@NG)
developed.
Experiments
and
theoretical
analysis
reveal
that
Fe
sites
exhibit
favorable
bonding
behaviors
(Fe–O:
d
xz
‐p,
yz
z
2
‐p)
spin
configurations,
which
can
enable
rapid
desorption
*OH
thus
enhance
In
situ
monitoring
techniques
Gibbs
free
energy
diagram
further
demonstrate
adjacent
Ni
could
serve
as
second
active
center
participate
Fe,Ni/N‐C@NG
exhibits
enhanced
reduction
reaction
excellent
stability.
Meanwhile,
assembled
Zn–air
battery
maintains
stability
over
300
h
with
small
voltage
gap.
This
study
provides
multiple
insights
into
orbital
scale
laws
Advanced Materials,
Год журнала:
2024,
Номер
36(25)
Опубликована: Апрель 9, 2024
The
interaction
between
oxygen
species
and
metal
sites
of
various
orbitals
exhibits
intimate
correlation
with
the
reduction
reaction
(ORR)
kinetics.
Herein,
a
new
approach
for
boosting
inherent
ORR
activity
atomically
dispersed
Fe-N-C
matrix
is
represented
by
implanting
Fe
atomic
clusters
nearby.
as-prepared
catalyst
delivers
excellent
half-wave
potentials
0.78
0.90
V
in
acidic
alkaline
solutions,
respectively.
decent
can
also
be
validated
from
high-performance
rechargeable
Zn-air
battery.
experiments
density
functional
theory
calculations
reveal
that
electron
spin-state
monodispersed
active
transferred
low
spin
(LS,
t
Energy & Environmental Science,
Год журнала:
2023,
Номер
17(1), С. 249 - 259
Опубликована: Ноя. 16, 2023
Novel
Fe
single-atom
catalysts
with
highly
coordinated
Fe–N
4
SP
structures
were
designed
via
the
multi-coordination-shell
synergistic
effect.
The
optimization
of
enhances
their
ORR
activity
in
alkaline/acidic
media
towards
rechargeable
Zn–air
batteries.
Angewandte Chemie International Edition,
Год журнала:
2023,
Номер
62(28)
Опубликована: Май 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.
Nano-Micro Letters,
Год журнала:
2023,
Номер
15(1)
Опубликована: Окт. 13, 2023
Abstract
Single-atom
catalysts
(SACs)
have
garnered
increasingly
growing
attention
in
renewable
energy
scenarios,
especially
electrocatalysis
due
to
their
unique
high
efficiency
of
atom
utilization
and
flexible
electronic
structure
adjustability.
The
intensive
efforts
towards
the
rational
design
synthesis
SACs
with
versatile
local
configurations
significantly
accelerated
development
efficient
sustainable
electrocatalysts
for
a
wide
range
electrochemical
applications.
As
an
emergent
coordination
avenue,
intentionally
breaking
planar
symmetry
by
adding
ligands
axial
direction
metal
single
atoms
offers
novel
approach
tuning
both
geometric
structures,
thereby
enhancing
electrocatalytic
performance
at
active
sites.
In
this
review,
we
briefly
outline
burgeoning
research
topic
axially
coordinated
provide
comprehensive
summary
recent
advances
synthetic
strategies
Besides,
challenges
outlooks
field
also
been
emphasized.
present
review
provides
in-depth
understanding
SACs,
which
could
bring
new
perspectives
solutions
fine
regulation
structures
catering
high-performing
electrocatalysis.
Advanced Functional Materials,
Год журнала:
2023,
Номер
33(51)
Опубликована: Авг. 17, 2023
Abstract
Single‐atom
catalysts
(SACs)
have
been
widely
explored
as
additives
to
improve
the
performance
of
lithium–sulfur
(Li–S)
batteries,
however,
design
highly
catalytic
and
in‐depth
knowledge
structure–activity
relationship
SACs
remains
a
huge
challenge.
Herein,
electron
redistribution
Co
site
by
introducing
S
atom
replace
N
in
first
coordination
shell
is
theoretically
predicted
enhance
anchoring
capability
lithium
polysulfides
(LiPSs)
simultaneously
facilitate
redox
process
Li–S
due
strengthened
d‐p
orbital
hybridization
between
sulfur
species
compared
with
traditional
CoN
4
architecture.
Enlightened
theoretical
analysis,
asymmetric
(N,
S)
coordinated
single
atoms
embedded
on
N,
S‐doped
hierarchically
porous
carbon
(S‐Co‐SACs/NSC)
precisely
designed
constructed
high‐efficiency
fixity
catalyst
for
batteries.
Therefore,
battery
S@S‐Co‐SACs/NSC
cathode
exhibits
high
areal
capacity
cycling
stability.
This
work
highlights
vital
function
electronic
structures
promoting
practical
application
Angewandte Chemie International Edition,
Год журнала:
2023,
Номер
62(39)
Опубликована: Июль 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.
