Advanced Materials,
Journal Year:
2025,
Volume and Issue:
unknown
Published: Feb. 7, 2025
Abstract
Designing
single‐atom
catalysts
(SACs)
with
high
density
of
accessible
sites
by
improving
metal
loading
and
utilization
is
a
promising
strategy
to
boost
the
catalytic
activity,
but
remains
challenging.
Herein,
site
(SD)
iron
SAC
(D‐Fe‐N/C)
11.8
wt.%
Fe‐loading
reported.
The
in
situ
scanning
electrochemical
microscopy
technique
attests
that
active
SD
D‐Fe‐N/C
reach
as
1.01
×
10
21
g
−1
79.8%,
respectively.
Therefore,
demonstrates
superior
oxygen
reduction
reaction
(ORR)
activity
terms
half‐wave
potential
0.918
V
turnover
frequency
0.41
e
s
.
excellent
ORR
property
also
demonstrated
liquid
zinc‐air
batteries
(ZABs),
which
exhibit
peak
power
306.1
mW
cm
−2
an
ultra‐long
cycling
stability
over
1200
h.
Moreover,
solid‐state
laminated
ZABs
prepared
presetting
air
flow
layer
show
specific
capacity
818.8
mA
h
,
520
h,
wide
temperature‐adaptive
from
−40
60
°C.
This
work
not
only
offers
possibilities
metal‐loading
for
exploring
efficient
SACs,
provides
strategies
device
structure
design
toward
advanced
ZABs.
Angewandte Chemie International Edition,
Journal Year:
2023,
Volume and Issue:
62(22)
Published: March 30, 2023
Iron
phthalocyanine-based
polymers
(PFePc)
are
attractive
noble-metal-free
candidates
for
catalyzing
oxygen
reduction
reaction
(ORR).
However,
the
low
site-exposure
degree
and
poor
electrical
conductivity
of
bulk
PFePc
restricted
their
practical
applications.
Herein,
laminar
nanosheets
covalently
longitudinally
linked
to
graphene
(3D-G-PFePc)
was
prepared.
Such
structural
engineering
qualifies
3D-G-PFePc
with
high
site
utilization
rapid
mass
transfer.
Thence,
demonstrates
efficient
ORR
performance
a
specific
activity
69.31
μA
cm-2
,
81.88
A
g-1
turnover
frequency
0.93
e
s-1
site-1
at
0.90
V
vs.
reversible
hydrogen
electrode
in
O2
-saturated
0.1
M
KOH,
outperforming
lamellar
wrapped
counterpart.
Systematic
electrochemical
analyses
integrating
variable-frequency
square
wave
voltammetry
situ
scanning
microscopy
further
underline
kinetics
towards
ORR.
Advanced Functional Materials,
Journal Year:
2024,
Volume and Issue:
34(37)
Published: May 6, 2024
Abstract
The
exploitation
of
highly
activity
oxygen
evolution
reaction
(OER)
electrocatalysts
is
critical
for
the
application
electrocatalytic
water
splitting.
Triggering
lattice
mechanism
(LOM)
expected
to
provide
a
promising
pathway
overcome
sluggish
OER
kinetics,
however,
effectively
enhancing
involvement
remains
challenging.
In
this
study,
fabrication
B,
Fe
co‐doped
CoP
(B,
Fe─CoP)
nanofibers
reported,
which
serve
as
efficient
electrocatalyst
through
phosphorization
and
boronation
treatment
Fe‐doped
Co
3
O
4
nanofibers.
Experimental
results
combined
with
theoretical
calculations
reveal
that
simultaneous
incorporation
both
B
can
more
trigger
participation
in
CoFe
oxyhydroxides
reconstructed
from
Fe─CoP
compared
incorporating
only
or
Fe.
Therefore,
optimized
exhibit
superb
low
overpotentials
361
376
mV
at
1000
mA
cm
−2
alkaline
freshwater
natural
seawater,
respectively.
present
work
provides
significant
guidelines
innovative
design
concepts
development
following
LOM
pathway.
Advanced Energy Materials,
Journal Year:
2024,
Volume and Issue:
14(19)
Published: Feb. 21, 2024
Abstract
Designing
effective
electrocatalysts
tailored
for
targeted
reactions
requires
fundamental
insights
into
the
structure
dependence
of
reaction
microenvironment.
Herein,
inspired
by
finite
element
simulations,
N,O
co‐doped
carbon
nanosheets
featuring
a
hierarchical
micro/mesoporous
to
form
an
oxygen‐rich
and
local
alkaline‐like
microenvironment
two‐electron
oxygen
reduction
(2e
−
ORR)
in
neutral
medium
are
designed.
The
situ
ex
test
results
confirmed
that
architecture
can
elevate
pH
accelerate
generation
intermediates
(*O
2
,
*OOH),
leading
high‐efficiency
H
O
production.
Utilizing
this
favorable
microenvironment,
N,O‐CNS
0.5
demonstrated
exceptional
electrosynthesis
performance
media,
achieving
superior
yield
rate
(6705
mmol
g
catalyst
−1
h
flow
cell).
Additionally,
comparative
experiments
density‐functional
theory
calculations
provided
confirmation
bi‐doping
N
as
active
origin
responsible
electrochemical
2e
ORR.
This
study
synergistically
manipulates
sites,
providing
opportunity
efficient
electro‐production
medium.
Advanced Functional Materials,
Journal Year:
2024,
Volume and Issue:
34(29)
Published: March 17, 2024
Abstract
The
oxygen
reduction
reaction
(ORR)
plays
a
fundamental
role
in
sustainable
energy
technologies.
However,
the
creation
of
non‐precious
metal
electrocatalysts
with
high
ORR
activity
and
durability
under
all
pH
conditions
is
great
significance
but
remains
challenging.
Herein,
aim
to
overcome
this
challenge
by
creating
Fe
single
atom
catalyst
on
2D
defect‐containing
nitrogen‐doped
carbon
support
(Fe
1
/DNC)
via
microenvironment
engineering
strategy.
Microkinetic
modeling
reveals
that
FeN
4
(OH)
moieties
are
real
active
sites
conditions.
Due
synergistic
promotion
effect
denser
accessible
defect‐induced
electronic
properties,
/DNC
achieves
extraordinary
alkaline,
acidic,
neutral
conditions,
half‐wave
potentials
0.95,
0.82,
0.70
V,
respectively.
Moreover,
negligible
performance
decay
observed
stability
methanol
tolerance
tests.
Zn‐air
battery
employing
delivers
remarkable
peak
power
density
long‐term
operational
durability.
Theoretical
analysis
provides
compelling
evidence
defects
adjacent
can
endow
an
inductive
reshape
properties
balance
OOH*
formation
OH*
reduction.
This
work
offers
insight
into
regulation
asymmetric
coordination
structure
for
boosting
electrocatalytic
stability.
Angewandte Chemie International Edition,
Journal Year:
2024,
Volume and Issue:
63(28)
Published: May 9, 2024
The
single-atom
Fe-N-C
catalyst
has
shown
great
promise
for
the
oxygen
reduction
reaction
(ORR),
yet
intrinsic
activity
is
not
satisfactory.
There
a
pressing
need
to
gain
deeper
understanding
of
charge
configuration
and
develop
rational
modulation
strategies.
Herein,
we
have
prepared
Fe
with
co-coordination
N
O
(denoted
as
Fe-N/O-C)
adjacent
defect,
proposing
strategy
optimize
d-orbital
spin-electron
filling
sites
by
fine-tuning
first
coordination
shell.
Fe-N/O-C
exhibits
significantly
better
ORR
compared
its
counterpart
commercial
Pt/C,
much
more
positive
half-wave
potential
(0.927
V)
higher
kinetic
current
density.
Moreover,
using
catalyst,
Zn-air
battery
proton
exchange
membrane
fuel
cell
achieve
peak
power
densities
up
490
1179
mW
cm
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.
Chemical Science,
Journal Year:
2024,
Volume and Issue:
15(29), P. 11188 - 11228
Published: Jan. 1, 2024
The
oxygen
reduction
reaction
(ORR)
is
a
key
component
for
many
clean
energy
technologies
and
other
industrial
processes.
However,
the
low
selectivity
sluggish
kinetics
of
ORR
catalysts
have
hampered
conversion
efficiency
real
application
these
new
mentioned
before.
Recently,
tremendous
efforts
been
made
in
mechanism
understanding,
electrocatalyst
development
system
design.
Here,
comprehensive
critical
review
provided
to
present
recent
advances
field
electrocatalytic
ORR.
two-electron
four-electron
transfer
catalytic
mechanisms
evaluation
parameters
are
discussed
first.
Then,
up-to-date
synthetic
strategies
