Advanced Functional Materials,
Journal Year:
2023,
Volume and Issue:
34(9)
Published: Nov. 27, 2023
Abstract
Engineering
the
electronic
configuration
and
intermediates
adsorption
behaviors
of
high‐performance
non‐noble‐metal‐based
catalysts
for
sluggish
oxygen
reduction
reaction
(ORR)
kinetics
at
cathode
is
highly
imperative
development
anion
exchange
membrane
fuel
cells
(AEMFCs),
yet
remains
an
enormous
challenge.
Herein,
a
rare‐earth
metal
oxide
engineering
tactic
through
formation
Fe
3
O
4
/La
2
heterostructures
in
N,O‐doped
carbon
nanospheres
(Fe
@N,O‐CNSs)
efficient
electrocatalysis
reported.
The
theoretical
calculations
reveal
that
interfacial
bonds
formed
by
La─O─Fe
heterogeneous
interface
effectively
optimize
structure
d‐band
center
relative
to
Fermi
level,
which
results
significant
barriers
rate‐limiting
steps
during
ORR.
modulation
chemisorption
enables
@N,O‐CNSs
outstanding
ORR
performance
improved
stability,
with
significantly
higher
half‐wave
potential
value
(0.88
V).
More
impressively,
this
integrated
catalyst
delivers
remarkable
power
density
148.7
mW
cm
−2
practical
AEMFC
operating
conditions,
along
negligible
degradation
over
100
h
using
H
‐air
atmosphere,
than
commercial
Pt/C‐coupled
electrodes.
presented
here
are
believed
provide
guidelines
fabricating
AEMFCs
electrocatalysts
terms
heterointerface
strong
coupling
effect
induced
oxides.
Advanced Functional Materials,
Journal Year:
2024,
Volume and Issue:
34(36)
Published: March 18, 2024
Abstract
Recently,
a
diverse
array
of
novel
metal‐nitrogen‐carbon
(M‐N‐C)
single‐atom
catalysts
(SACs)
have
rapidly
evolve,
particularly
in
the
realm
oxygen
reduction
reaction
(ORR).
Despite
plethora
proposed
design
and
improvement
strategies
for
SACs,
comprehensive
review
systematically
compiling
components
M‐N‐C
from
unified
perspective
is
notably
absent.
For
first
time,
thorough
examination
each
component
conducted,
focusing
on
entropy
increase
active
sites
SACs.
single
M‐N
4
whole
system,
an
implies
elevated
degree
disorder
chaos.
Broadly,
entropy‐increasing
modification
M
(single
mental
sites)
guest
groups
entails
augmentation
chaos,
with
most
effective
co‐catalytic
synergy
achieved
by
establishing
multiple
through
“cocktail
effect”.
Concerning
N
(nitrogen
other
heteroatoms)
C
(carbon
supports),
induces
heightened
disorder,
symmetry
breaking
more
likely
to
drive
toward
adsorbing
molecules
attain
equilibrium
symmetric
structure.
All
these
innovative
led
remarkable
ORR
activity
stability
offer
guiding
criterion
future
preparation
Advanced Science,
Journal Year:
2024,
Volume and Issue:
11(12)
Published: Jan. 15, 2024
Abstract
Developing
efficient
metal‐nitrogen‐carbon
(M‐N‐C)
single‐atom
catalysts
for
oxygen
reduction
reaction
(ORR)
is
significant
the
widespread
implementation
of
Zn‐air
batteries,
while
synergic
design
matrix
microstructure
and
coordination
environment
metal
centers
remains
challenges.
Herein,
a
novel
salt
effect‐induced
strategy
proposed
to
engineer
N
P
coordinated
atomically
dispersed
Fe
atoms
with
extra‐axial
Cl
on
interlinked
porous
carbon
nanosheets,
achieving
superior
catalyst
(denoted
as
Fe‐NP‐Cl‐C)
ORR
batteries.
The
hierarchical
nanosheet
architecture
can
provide
rapid
mass/electron
transfer
channels
facilitate
exposure
active
sites.
Experiments
density
functional
theory
(DFT)
calculations
reveal
distinctive
Fe‐N
2
‐Cl
sites
afford
significantly
reduced
energy
barriers
promoted
kinetics
ORR.
Consequently,
Fe‐NP‐Cl‐C
exhibits
distinguished
performance
half‐wave
potential
(E
1/2
)
0.92
V
excellent
stability.
Remarkably,
assembled
battery
based
delivers
an
extremely
high
peak
power
260
mW
cm
−2
large
specific
capacity
812
mA
h
g
−1
,
outperforming
commercial
Pt/C
most
reported
congeneric
catalysts.
This
study
offers
new
perspective
structural
optimization
engineering
electrocatalysis
conversion
devices.
Advanced Functional Materials,
Journal Year:
2024,
Volume and Issue:
34(28)
Published: Feb. 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 Science,
Journal Year:
2024,
Volume and Issue:
11(33)
Published: July 1, 2024
Abstract
Modifying
the
coordination
or
local
environments
of
single‐,
di‐,
tri‐,
and
multi‐metal
atom
(SMA/DMA/TMA/MMA)‐based
materials
is
one
best
strategies
for
increasing
catalytic
activities,
selectivity,
long‐term
durability
these
materials.
Advanced
sheet
supported
by
metal
atom‐based
have
become
a
critical
topic
in
fields
renewable
energy
conversion
systems,
storage
devices,
sensors,
biomedicine
owing
to
maximum
utilization
efficiency,
precisely
located
centers,
specific
electron
configurations,
unique
reactivity,
precise
chemical
tunability.
Several
offer
excellent
support
are
attractive
applications
energy,
medical
research,
such
as
oxygen
reduction,
production,
hydrogen
generation,
fuel
selective
detection,
enzymatic
reactions.
The
strong
metal–metal
metal–carbon
with
metal–heteroatom
(i.e.,
N,
S,
P,
B,
O)
bonds
stabilize
optimize
electronic
structures
atoms
due
interfacial
interactions,
yielding
activities.
These
provide
models
understanding
fundamental
problems
multistep
This
review
summarizes
substrate
structure‐activity
relationship
different
active
sites
based
on
experimental
theoretical
data.
Additionally,
new
synthesis
procedures,
physicochemical
characterizations,
biomedical
discussed.
Finally,
remaining
challenges
developing
efficient
SMA/DMA/TMA/MMA‐based
presented.
Small,
Journal Year:
2024,
Volume and Issue:
20(33)
Published: April 9, 2024
Constructing
multiheteroatom
coordination
structure
in
carbonaceous
substrates
demonstrates
an
effective
method
to
accelerate
the
oxygen
reduction
reaction
(ORR)
of
supported
single-atom
catalyst.
Herein,
novel
etching
route
assisted
by
potassium
thiocyanate
(KCNS)
is
developed
convert
metal-organic
framework
2D
defect-rich
porous
N,S-co-doped
carbon
nanosheets
for
anchoring
atomically
dispersed
iron
sites
as
high-performance
ORR
catalysts
(Fe-SACs).
The
well-designed
KCNS-assisted
can
generate
spatial
confinement
template
direct
nanosheet
formation,
condition
form
structure,
and
additional
sulfur
atoms
coordinate
species.
Spectral
microscopy
analysis
reveals
that
element
Fe-SACs
highly
isolated
on
anchored
nitrogen
unsymmetrical
Fe-S
Energy & Environmental Science,
Journal Year:
2024,
Volume and Issue:
17(14), P. 4847 - 4870
Published: Jan. 1, 2024
Based
on
the
advancements
in
atomically
dispersed
multi-site
catalysts
for
FZABs,
this
review
discusses
design
methodologies
to
regulate
performance
of
bifunctional
oxygen
electrocatalysts
from
electronic
and
geometric
structures.
Journal of the American Chemical Society,
Journal Year:
2024,
Volume and Issue:
146(31), P. 21357 - 21366
Published: July 25, 2024
With
more
flexible
active
sites
and
intermetal
interaction,
dual-atom
catalysts
(DACs)
have
emerged
as
a
new
frontier
in
various
electrocatalytic
reactions.
Constructing
typical
p-d
orbital
hybridization
between
p-block
d-block
metal
atoms
may
bring
avenues
for
manipulating
the
electronic
properties
thus
boosting
activities.
Herein,
we
report
distinctive
heteronuclear
dual-metal
atom
catalyst
with
asymmetrical
FeSn
dual
embedded
on
two-dimensional
C2N
nanosheet
(FeSn–C2N),
which
displays
excellent
oxygen
reduction
reaction
(ORR)
performance
half-wave
potential
of
0.914
V
an
alkaline
electrolyte.
Theoretical
calculations
further
unveil
powerful
stannum
ferrum
sites,
triggers
electron
delocalization
lowers
energy
barrier
*OH
protonation,
consequently
enhancing
ORR
activity.
In
addition,
FeSn–C2N-based
Zn–air
battery
provides
high
maximum
power
density
(265.5
mW
cm–2)
specific
capacity
(754.6
mA
h
g–1).
Consequently,
this
work
validates
immense
along
perception
into
logical
design
DACs.
Advanced Energy Materials,
Journal Year:
2024,
Volume and Issue:
14(24)
Published: April 10, 2024
Abstract
Developing
seawater‐based
high‐performance
oxygen
reduction
reaction
(ORR)
electrocatalysts
is
meaningful
to
renewable
energy
storage
and
conversion,
the
Fe‐based
derivatives
encapsulated
by
nitrogen
(N)
doped
carbon
are
typical
representative.
Nevertheless,
unrevealing
mechanism
of
N
configuration
ORR
activity
chlorine
resistance
still
a
great
challenge.
In
this
work,
feasible
strategy
developed
prepare
controllable
pyridinic/pyrrolic‐N
carbon‐coated
(Fe
x
N‐NC).
Drawing
support
from
H
3
PO
4
blocking
based
in
situ
Fourier
transform
infrared
spectroscopy
(FTIR)
test
density‐functional
theory
(DFT)
calculation,
tandem
effect
pyridinic‐N
pyrrolic‐N
on
proved.
Additionally,
low
hydrogen
peroxide
(H
2
O
)
yield
4e
−
pathway
Fe
N‐NC
demonstrate
that
doping
effectively
reduces
adsorption
Cl
,
which
consistent
with
DFT.
The
half‐wave
potential
(E
1/2
for
reaches
0.874
V
alkaline
seawater,
ZABs
assembled
as
air
cathode
deliver
remarkable
power
density
(162
mW
cm
−2
),
along
excellent
long‐term
durability
(>400
h).
