ACS Applied Nano Materials,
Journal Year:
2024,
Volume and Issue:
7(11), P. 13547 - 13556
Published: May 22, 2024
The
development
of
efficient
and
facile
nonprecious
metal
catalysts
for
the
oxygen
reduction
reaction
(ORR)
holds
great
significance.
Among
these,
single-atomic
metal–nitrogen–carbon
(M–N–C)
are
emerging
candidates
due
to
their
high
activity
prolonged
lifespan.
However,
traditional
preparation
M–N–C
suffers
from
thermal
aggregation
low
space–time
yield,
limiting
application
in
industry.
Inspired
by
"chainmail
protection"
carbonaceous
materials,
here
we
propose
an
"armor
strategy
large-scale
synthesis
a
highly
active
Fe
single-atom
ORR
catalyst
(Fe-8/8-CN)
pyrolyzing
well-designed
precursor
Fe-ZIF-8/ZIF-8.
In
this
precursor,
2-methylimidazole
zinc
MOF
(ZIF-8)
loaded
with
iron
(Fe-ZIF-8)
is
encased
additional
ZIF-8
armor
layer
(Fe-ZIF-8/ZIF-8)
that
effectively
shields
species
within
inner
during
pyrolysis
process,
ultimately
yielding
(Fe-8/8-CN).
Furthermore,
approaches
construction
Fe-ZIF-8/ZIF-8
make
it
efficiently
scale
up
yield
18.7
kg
m–3
day–1.
particular,
protection
preparing
universally
applicable
leaf-shaped
ZIF-L
other
ZIFs
diverse
morphologies.
Thanks
presence
outer
core
dispersing
catalytic
sites
porous
defect-rich
characteristics
volatilization
Zn
ZIF-8,
resulting
Fe-8/8-CN
demonstrates
superior
performance
alkaline
electrolyte
(E1/2
=
0.93
V,
JL
−5.89
mA
cm–2).
Finally,
Fe-8/8-CN,
as
cathode
material
flexible
zinc–air
batteries,
exhibits
peak
power
density
(97
mW
cm–2)
excellent
durability
Pt/C.
Environmental Science & Technology,
Journal Year:
2021,
Volume and Issue:
55(2), P. 1260 - 1269
Published: Jan. 8, 2021
Heterogeneous
electro-Fenton
(HEF)
reaction
has
been
considered
as
a
promising
process
for
real
effluent
treatments.
However,
the
design
of
effective
catalysts
simultaneous
H2O2
generation
and
activation
to
achieve
bifunctional
catalysis
O2
toward
•OH
production
remains
challenge.
Herein,
core-shell
structural
Fe-based
catalyst
(FeNC@C),
with
Fe3C
FeN
nanoparticles
encapsulated
by
porous
graphitic
layers,
was
synthesized
employed
in
HEF
system.
The
FeNC@C
presented
significant
performance
degradation
various
chlorophenols
at
conditions
an
extremely
low
level
leached
iron.
Electron
spin
resonance
radical
scavenging
revealed
that
key
reactive
species
FeIV
would
play
role
neutral
conditions.
Experimental
density
function
theory
calculation
dominated
positive
effect
FeNx
sites
on
form
•OH.
Meanwhile,
proved
be
less
pH
dependence,
high
stability,
well-recycled
materials
practical
application
wastewater
purification.
ACS Catalysis,
Journal Year:
2022,
Volume and Issue:
12(9), P. 5595 - 5604
Published: April 26, 2022
Tuning
the
geometric
and
electronic
structure
of
single-metal-atom
catalysts
via
simultaneous
presence
metal
nanoparticles
or
nanoclusters
(NCs)
offers
an
alternative
avenue
to
improving
their
catalytic
performance.
Herein,
we
demonstrate
that
coexistence
Fe
NCs
in
proximity
single
atoms
on
N-doped
porous
carbon
can
significantly
improve
performance
aerobic
oxidation
primary
amines
imines
using
air
as
oxidant.
A
broad
spectrum
aromatic,
heterocyclic,
aliphatic
was
efficiently
selectively
oxidized
into
corresponding
good
high
yields.
Experimental
measurements
theoretical
calculations
reveal
interacts
with
atoms,
which
not
only
benefits
adsorption
molecular
O2
amine
substrates
but
also
promotes
activation
generate
singlet
oxygen
(1O2)
then
facilitates
key
intermediate
imine
formation
H-atom
abstraction
a
lower
energy
barrier,
thereby
boosting
reaction
activity.
Nature Communications,
Journal Year:
2022,
Volume and Issue:
13(1)
Published: April 6, 2022
Zeolitic
imidazolate
frameworks
derived
Fe1-N-C
catalysts
with
isolated
single
iron
atoms
have
been
synthesized
and
applied
for
selective
ammoxidation
reactions.
For
the
preparation
of
different
Fe-based
materials,
benzylamine
as
an
additive
proved
to
be
essential
tune
morphology
size
ZIFs
resulting
in
uniform
smaller
particles,
which
allow
stable
atomically
dispersed
Fe-N4
active
sites.
The
optimal
catalyst
achieves
efficient
synthesis
various
aryl,
heterocyclic,
allylic,
aliphatic
nitriles
from
alcohols
water
under
very
mild
conditions.
With
its
chemoselectivity,
recyclability,
high
efficiency
conditions
this
new
system
complements
toolbox
nitrile
synthesis,
are
important
intermediates
many
applications
life
sciences
industry.
Advanced Functional Materials,
Journal Year:
2022,
Volume and Issue:
32(21)
Published: Feb. 20, 2022
Abstract
Single‐atom
catalysts
show
great
promise
as
non‐precious
electrocatalysts
for
CO
2
electroreduction
reaction
(CO
ER).
However,
it
is
still
challenging
to
gain
a
fundamental
understanding
of
the
complicated
dynamic
behavior
activation
achieve
high
product
selectivity.
Herein,
authors
report
an
unusual
iron
single‐atom
catalyst,
containing
atomically
dispersed
Fe–N
4
species
and
Fe
3
C
nanoparticles
(NPs)
(Fe
C|Fe
1
N
).
Having
fragmental‐rock‐shaped
nanocarbon
architecture,
isolated
sites
uniformly
disperse
with
adjacent
NPs
(<30
nm)
in
carbon
matrix.
Benefiting
from
strong
coupling
effect
between
unique
spatial
nanostructure,
displays
exceptional
ER
activity
low
onset
potential
−0.3
V
Faradaic
efficiency
94.6%
at
−0.5
production,
acting
one
most
active
Fe–N–C
even
exceeding
other
supported
metal
NPs.
Experimental
observations
discover
that
excellent
catalyst
attributable
presence
optimizes
J
coexisted
sites.
In
situ
attenuated
total
reflectance‐Fourier
transform
infrared
analysis
theoretical
calculations
reveal
strengthen
adsorption
on
accelerate
formation
*COOH
intermediate,
hence
enhance
whole
performance.
ChemistrySelect,
Journal Year:
2025,
Volume and Issue:
10(1)
Published: Jan. 1, 2025
Abstract
An
electrochemical
cyclization
strategy
is
employed
herewith
for
the
eco‐friendly
and
cost‐effective
synthesis
of
2‐substituted
quinazolines
by
using
2‐aminobenzylamines
aldehydes
or
alcohols
as
starting
substrates.
The
reactions
were
conducted
under
two
distinct
reaction
temperatures:
25
°C
60
alcohols.
Tetra‐
n
‐butylammonium
iodide
(TBAI)
participates
in
dual
roles
such
as,
an
electrolyte
a
mild
reagent
to
facilitate
formation
at
constant
current
30
mA
graphite
electrode
anode
platinum
cathode
dimethyl
sulfoxide
(DMSO)
solvent.
Under
devised
process,
accomplished
with
broad
substrate
scope
excellent
yields
(up
90%),
which
reduces
toxic
side
products.
plausible
mechanistic
pathways
have
been
formulated,
are
supported
control
experiments
cyclic
voltammetry
studies.
findings
demonstrate
that
conditions,
iodonium
ions
generated,
play
crucial
role
enhancing
efficacy
described
method.
Advanced Functional Materials,
Journal Year:
2020,
Volume and Issue:
31(10)
Published: Dec. 3, 2020
Abstract
The
rational
design
and
facile
synthesis
of
1D
hollow
tubular
carbon‐based
materials
with
highly
efficient
oxygen
reduction
reaction
(ORR)
performance
remains
a
challenge.
Herein,
simple
yet
robust
route
is
employed
to
simultaneously
craft
single‐atomic
Fe
sites
graphitic
layer‐wrapped
3
C
nanoparticles
(Fe
C@GL
NPs)
encapsulated
within
N‐doped
mesoporous
carbon
tubes
(denoted
Fe‐N‐HMCTs).
successional
compositional
structural
crafting
the
hydrothermally
self‐templated
polyimide
(PITs),
enabled
by
species
incorporation
acid
leaching
treatment,
respectively,
yields
Fe‐N‐HMCTs
that
are
subsequently
exploited
as
ORR
electrocatalyst.
Remarkably,
an
alkaline
electrolyte
capitalizing
on
achieves
excellent
activity
(onset
potential,
0.992
V;
half‐wave
0.872
V),
favorable
long‐term
stability,
strong
methanol
tolerance,
outperforming
state‐of‐the‐art
Pt/C
catalyst.
Such
impressive
performances
originate
from
configuration
active
(i.e.,
atomically
dispersed
Fe‐N
x
homogeneously
incorporated
in
conjunction
advantageous
architecture
containing
adequate
surface.
This
work
offers
new
view
fabricate
earth‐abundant
Fe‐N‐C
electrocatalysts
well‐designed
outstanding
for
electrochemical
energy
conversion
storage.
