Analytical Chemistry,
Journal Year:
2024,
Volume and Issue:
96(24), P. 10021 - 10027
Published: June 6, 2024
Although
oxygen
reduction
reaction
(ORR)
as
an
effective
signal
amplification
strategy
has
been
extensively
investigated
for
the
improvement
of
sensitivity
electrochemical
sensors,
their
activity
and
stability
are
still
a
great
challenge.
Herein,
single-atom
Fe
(FeSA)
nanoparticles
(FeNP)
on
nitrogen-doped
carbon
(FeSA/FeNP)
catalysts
demonstrate
highly
active
stable
ORR
performance,
thus
achieving
sensitive
sensing
organophosphorus
pesticides
(OPs).
Experimental
investigations
indicate
that
FeNP
in
FeSA/FeNP
can
improve
by
adjusting
electronic
structure
FeSA
sites.
Besides,
owing
to
excellent
catalase-like
activity,
rapidly
consume
situ
generated
H2O2
process
avoid
leakage
sites,
thereby
improving
ORR.
Utilizing
performance
FeSA/FeNP,
sensor
OPs
is
established
based
thiocholine-induced
poison
demonstrating
satisfactory
stability.
This
work
provides
new
insight
into
design
high
sensing.
Energy & Environmental Science,
Journal Year:
2023,
Volume and Issue:
17(2), P. 386 - 424
Published: Nov. 22, 2023
This
review
provides
an
in-depth
discussion
of
the
carbon-based
electrocatalysts
for
rechargeable
Zn–air
batteries
from
design
strategies,
research
progress,
and
future
perspectives.
Small,
Journal Year:
2024,
Volume and Issue:
20(43)
Published: July 2, 2024
Asymmetric
electronic
environments
based
on
microscopic-scale
perspective
have
injected
infinite
vitality
in
understanding
the
intrinsic
mechanism
of
polarization
loss
for
electromagnetic
(EM)
wave
absorption,
but
still
exists
a
significant
challenge.
Herein,
Zn
single-atoms
(SAs),
structural
defects,
and
Co
nanoclusters
are
simultaneously
implanted
into
bimetallic
metal-organic
framework
derivatives
via
two-step
dual
coordination-pyrolysis
process.
Theoretical
simulations
experimental
results
reveal
that
coupling
interactions
between
SAs
defects
delocalize
symmetric
generate
additional
dipole
without
sacrificing
conduction
owing
to
compensation
carbon
nanotubes.
Moreover,
with
large
nanocurvatures
induce
strong
interfacial
electric
field,
activate
superiority
heterointerfaces
promote
polarization.
Benefiting
from
aforementioned
merits,
resultant
deliver
an
optimal
reflection
-58.9
dB
effective
absorption
bandwidth
is
5.2
GHz.
These
findings
provide
innovative
insight
clarifying
microscopic
asymmetric
electron
viewpoint
inspire
generalized
modulation
engineering
optimizing
EM
absorption.
Advanced Functional Materials,
Journal Year:
2024,
Volume and Issue:
34(23)
Published: Jan. 15, 2024
Abstract
Fe–N–C
catalysts
are
emerging
as
promising
alternatives
to
Pt‐based
for
the
oxygen
reduction
reaction
(ORR),
while
they
still
suffer
from
sluggish
kinetics
due
discontented
binding
affinity
between
Fe‐N
4
sites
and
oxygen‐containing
intermediates,
unsatisfactory
stability.
Herein,
a
flexible
multichannel
carbon
fiber
membrane
immobilized
with
atomically
dispersed
neighboring
Fe
nanoclusters/nanoparticles
(FeN
‐Fe
NCP
@MCF)
is
synthesized.
The
optimized
geometric
electronic
structures
of
atomic
brought
by
adjacent
hierarchically
porous
structure
matrix
endow
FeN
@MCF
outstanding
ORR
activity
stability,
considerably
outperforming
its
counterpart
only
commercial
Pt/C
catalyst.
Liquid
solid‐state
zinc–air
batteries
employing
both
exhibit
durability.
Theoretical
calculation
reveals
that
nanoclusters
can
trigger
remarkable
electron
redistribution
modulate
hybridization
central
3
d
O
2
p
orbitals,
facilitating
activation
molecules
optimizing
adsorption
capacity
intermediates
on
sites,
thus
accelerating
kinetic.
This
work
offers
an
effective
approach
constructing
coupling
have
single
atoms
coexisting
efficient
catalysis.
Advanced Functional Materials,
Journal Year:
2024,
Volume and Issue:
34(33)
Published: April 18, 2024
Abstract
The
design
of
bifunctional
electrocatalysts
toward
reduction
reaction
carbon
dioxide
(ECO
2
RR)
and
oxygen
evolution
(OER)
in
aqueous
rechargeable
Zn─CO
batteries
(ZABs)
still
poses
a
significant
challenge.
Herein,
Ni
clusters
(Ni
x
)
0.5
0.8
nm
diameter
coupled
with
single
site
(Ni−N
4
−C),
denoted
as
Ni−N
/Ni
5
8
,
respectively,
are
synthesized
the
size
effect
nanoclusters
studied.
exhibits
an
≈100%
Faradaic
efficiency
(
FE
CO
ECO
RR
for
from
−0.4
to
−0.8
V
versus
reversible
hydrogen
electrode,
superior
that
−C
=
55.0%)
80.0%).
OER
performance
or
comparable
commercial
RuO
but
outperform
−C.
Theoretical
calculation
indicates
*
COOH
intermediates
bond
synergistically
atom
site,
promoting
activation
reducing
energy
barrier
potential
determining
step
RR.
Such
is
strongly
size‐dependent
larger
result
too
strong
binding
intermediates,
impede
formation
CO.
As
cathode
electrocatalyst
alkaline
ZABs,
peak
power
density
11.7
mW
cm
−2
cycling
durability
over
1200
cycles
420
h.
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
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 Functional Materials,
Journal Year:
2024,
Volume and Issue:
unknown
Published: May 3, 2024
Abstract
Single‐atom
nanozymes
(SAzymes)
have
made
significant
strides
in
antibacterial
treatment
but
fall
short
as
natural
enzyme
and
drug
replacements
due
to
limited
catalytic
performance.
Here,
a
rational
strategy
is
presented
for
incorporating
spatially
axial
boron
(B)
ligands
effectively
modulate
the
local
coordination
environment
of
planar
Fe─N
4
motifs
(Fe─B/N─C
SAzymes).
With
electronic
modulation,
Fe─B/N─C
SAzymes
exhibit
significantly
enhanced
oxidase‐,
peroxidase‐,
catalase‐like
activities.
Theoretical
calculations
highlight
that
B
adjust
charge
distribution
around
active
center,
which
facilitates
heterolysis
H
2
O
desorption
,
resulting
accelerated
decomposition.
Furthermore,
intrinsic
photothermal
effect
enhances
multienzyme‐like
activities,
rapidly
generating
abundant
reactive
oxygen
species
(ROS),
achieving
chemodynamic/photothermal
synergistic
therapy
impressive
disinfection
against
periodontal‐related
pathogenic
bacteria.
These
findings
offer
distinctive
viewpoint
optimizing
with
ligand
enhance
their
performance
effectiveness
periodontitis
therapy.
Advanced Energy Materials,
Journal Year:
2025,
Volume and Issue:
unknown
Published: Jan. 16, 2025
Abstract
Multi‐heteroatom‐doped
metal‐free
carbons
with
well‐tailored
electronic
structures
are
regarded
as
promising
oxygen
reduction
reaction
(ORR)
catalysts.
However,
their
active
sites
often
hindered
by
the
carbon
matrix,
resulting
in
reduced
catalytic
activity.
Herein,
nitrogen,
phosphorus,
and
sulfur
tri‐doped
hollow
hierarchical
porous
nanofibers
(NPS‐HPCNFs)
interpenetrated
pores
synthesized
using
a
facile
coaxial
electrospinning
method.
The
distinctive
steric
confinement
induced
created
positive
microenvironment
for
ORR.
As
result,
resultant
NPS‐HPCNF
catalyst
exhibits
half‐wave
potential
(
E
1/2
)
of
0.86
V
(vs.
RHE)
superb
long‐term
stability
0.1
m
KOH.
Furthermore,
zinc‐air
battery
(ZAB)
assembled
achieves
great
peak
power
density
210
mW
cm
−2
superior
specific
capacity
795
mAh
g
−1
,
outperforming
commercial
Pt/C
candidate.
In
addition,
functional
theory
(DFT)
calculations
reveal
that
synergistic
effect
N,
P,
S
tri‐doping
combined
defect
effectively
regulated
structure
significantly
enhanced
*
OOH
adsorption,
thus
accelerating
ORR
process.
Therefore,
abundant
represent
eco‐friendly
alternative
to
state‐of‐the‐art
electrocatalysts
various
electrochemical
energy
applications.