Abstract
In
recent
years,
some
experiments
and
theoretical
work
have
pointed
out
that
diatomic
catalysts
not
only
retain
the
advantages
of
monoatomic
catalysts,
but
also
introduce
a
variety
interactions,
which
exceed
limit
catalytic
performance
can
be
applied
to
many
fields.
Here,
interaction
between
adjacent
metal
atoms
in
is
elaborated:
synergistic
effect,
spacing
enhancement
effect
(geometric
effect),
electronic
effect.
With
regard
classification
characterization
various
new
are
classified
into
four
categories:
heteronuclear/homonuclear,
with/without
carbon
carriers,
their
measures
introduced
explained
detail.
aspect
preparation
widely
used
atomic
layer
deposition
method,
metal–organic
framework
derivative
simple
ball
milling
method
introduced,
with
emphasis
on
formation
mechanism
catalysts.
Finally,
effective
control
strategies
key
applications
electrocatalysis,
photocatalysis,
thermal
catalysis,
other
fields
given.
ACS Catalysis,
Год журнала:
2023,
Номер
13(7), С. 5020 - 5032
Опубликована: Март 29, 2023
NOx
emission
is
a
major
environmental
issue,
and
selective
catalytic
reduction
(SCR)
the
most
effective
method
for
conversion
of
to
harmless
N2
H2O.
Manganese
oxide
has
excellent
low-temperature
(LT)
denitration
(de-NOx)
activity,
but
poor
SO2
tolerance
hinders
its
application.
Herein,
we
report
an
interesting
SCR
catalyst,
quasi-metal–organic-framework
(MOF)
nanorod
containing
manganese
(quasi-Mn-BTC)
with
abundant
oxygen
vacancies
(Vo),
unique
hierarchical
porous
structure,
half-metallic
property,
which
successfully
overcome
disadvantage
Mn-based
catalysts.
The
over
Mn-BTC-335
°C
only
drops
by
7%
until
gradually
increased
200
ppm
from
100
36
h.
Furthermore,
quasi-Mn-BTC
presents
LT
de-NOx
performance
above
90%
between
120
330
at
gas
hourly
space
velocity
36,000
h–1.
Experimental
theoretical
calculations
confirm
that
difficult
electron
transport
active
sites
can
prevent
it
competing
adsorption
NH3
NO.
low
degree
d–p
hybridization
unstable
p–p
on
make
oxidation;
thus,
weak
sulfation
sites,
ensuring
tolerance.
Additionally,
half-metallicity
extraordinary
d–sp
hybridization,
high
s–p
cause
strong
bonding
delocalization
electrons
promote
charge
transfer
adsorbed
ion
diffusion
NO
adsorption,
promoting
performance.
In
situ
diffuse
reflectance
infrared
Fourier
transform
spectra
density
functional
theory
calculation
further
reveal
reaction
follows
both
Eley–Rideal
(E-R)
Langmuir–Hinshelwood
(L-H)
mechanisms.
"standard
reaction"
more
likely
occur
in
E-R
reaction,
while
"fast
prone
L-H
pathway,
HNNOH
NH3NO2
are
two
key
intermediates.
This
work
provides
viable
strategy
augmenting
catalysts,
may
pave
new
way
application
MOFs
de-NOx,
complete
mechanism
solid
basis
future
improvements
NH3-SCR
reaction.
Energy storage materials,
Год журнала:
2023,
Номер
59, С. 102764 - 102764
Опубликована: Апрель 6, 2023
Atomically-dispersed
FeN4
moieties
are
emerging
as
low-cost
electrocatalysts
for
oxygen
reduction
reaction
(ORR),
which
can
be
applied
in
fuel
cells
and
metal-air
batteries.
Whereas,
the
unsatisfactory
position
of
d-band
center
from
metal
sites
offered
by
affects
adsorption-desorption
behaviors
oxygenated
intermediates,
further
impeding
improvement
their
ORR
performances.
Herein,
we
report
a
well-designed
diatomic
Fe/Zn-CNHC
catalyst
on
microporous
hollow
support.
This
strategy
drives
Fe
upward,
thus
making
active
more
favorable
stable
during
kinetic
processes.
The
material
exhibits
an
excellent
activity
with
half-wave
potential
0.91
V
stability
(insignificant
attenuation
after
5,000
cycles),
surpassing
commercial
Pt/C
many
other
single-atom
catalysts.
DFT
calculations
indicate
that
tuning
effect
Zn
d-orbital
electron
distribution
facilitates
stretching
cleavage
Fe-O,
accelerating
rate-determining
step.
work
presents
simple
to
fabricate
well-defined
coordination
inspires
future
research
developing
new
syntheses
control
electrocatalysts.
Abstract
Developing
cost‐efficient
trifunctional
catalysts
capable
of
facilitating
hydrogen
evolution
reaction
(HER),
oxygen
(OER),
and
reduction
(ORR)
activity
is
essential
for
the
progression
energy
devices.
Engineering
these
to
optimize
their
active
sites
integrate
them
into
a
cohesive
system
presents
significant
challenge.
This
study
introduces
nanoflower
(NFs)‐like
carbon‐encapsulated
FeNiPt
nanoalloy
catalyst
(FeNiPt@C
NFs),
synthesized
by
substituting
Co
2+
ions
with
high‐spin
Fe
in
Hofmann‐type
metal‐organic
framework,
followed
carbonization
pickling
processes.
The
FeNiPt@C
NFs
catalyst,
characterized
its
nitrogen‐doped
metal
alloy
structure
phase‐segregated
slight
surface
oxidization,
exhibits
excellent
catalytic
performance.
evidenced
activities
HER
(−25
mV
at
10
mA
cm
−2
),
ORR
(half‐wave
potential
0.93
V),
OER
(294
enhanced
water
oxidation
attributed
state
element.
Consequently,
Zn‐air
battery
anion
exchange
membrane
electrolyzer
assembled
demonstrate
remarkable
power
density
(168
mW
)
industrial‐scale
current
(698
1.85
respectively.
innovative
integration
multifunctional
paves
way
advancement
sustainable
systems.
ACS Nano,
Год журнала:
2023,
Номер
17(20), С. 19514 - 19525
Опубликована: Окт. 9, 2023
Single-atom
catalysts
(SACs)
are
regarded
as
promising
non-noble-metal
alternatives
for
the
oxygen
reduction
reaction
(ORR)
in
proton
exchange
membrane
fuel
cells
due
to
their
high
atom
utilization
efficiency
and
excellent
catalytic
properties.
However,
insufficient
long-term
stability
issues
of
SACs
under
working
conditions
seriously
hinder
practical
application.
In
this
perspective,
recent
progress
with
optimized
ORR
activity
is
first
reviewed.
Then,
possible
degradation
mechanisms
process
effective
strategies
improving
durability
summarized.
Finally,
some
challenges
opportunities
proposed
develop
stable
single-atom-based
electrocatalysts
future.
Journal of the American Chemical Society,
Год журнала:
2024,
Номер
146(13), С. 9124 - 9133
Опубликована: Март 22, 2024
Single-atom
catalysis
(SAC)
attracts
wide
interest
for
zinc–air
batteries
that
require
high-performance
bifunctional
electrocatalysts
oxygen
reactions.
However,
catalyst
design
is
still
highly
challenging
because
of
the
insufficient
driving
force
promoting
multiple-electron
transfer
kinetics.
Herein,
we
report
a
superstructure-assisted
SAC
on
tungsten
carbides
evolution
and
reduction
In
addition
to
usual
single
atomic
sites,
strikingly,
reveal
presence
ordered
Co
superstructures
in
interfacial
region
with
induce
internal
strain
promote
catalysis.
Theoretical
calculations
show
combined
effects
from
atoms
strongly
reduce
adsorption
energy
intermediates
overpotential
both
The
therefore
presented
impressive
activity
an
ultralow
potential
gap
0.623
V
delivered
high
power
density
188.5
mW
cm–2
assembled
batteries.
This
work
opens
up
new
opportunities
