Small,
Journal Year:
2024,
Volume and Issue:
unknown
Published: Dec. 26, 2024
In
the
era
of
atomic
manufacturing,
precise
manipulation
structures
to
engineer
highly
active
catalytic
sites
has
become
a
central
focus
in
catalysis
research.
Dual-atom
catalysts
(DACs)
have
garnered
significant
attention
for
their
superior
activity,
selectivity,
and
stability
compared
single-atom
(SACs).
However,
comprehensive
review
that
integrates
geometric
electronic
factors
influencing
DAC
performance
remains
limited.
This
systematically
explores
structure
DAC,
addressing
key
macroscopic
parameters,
such
as
spatial
arrangements
interatomic
distances,
well
microscopic
factors,
including
local
coordination
environments
structures.
Additionally,
metal-support
interactions
(MSI)
long-range
(LSI)
are
comprehensively
analyzed,
which
play
pivotal
yet
underexplored
role
governing
behavior.
integration
tailored
functional
groups
is
further
discussed
fine-tune
properties,
thereby
optimizing
intermediate
adsorption,
enhancing
reaction
kinetics,
expanding
multifunctionality
various
electrochemical
environments.
offers
novel
insights
into
rational
design
by
elucidating
intricate
mechanisms
underlying
DACs'
exceptional
performance.
Ultimately,
DACs
positioned
critical
players
precision
catalysis,
highlighting
potential
drive
breakthroughs
across
broad
spectrum
applications.
Journal of the American Chemical Society,
Journal Year:
2025,
Volume and Issue:
unknown
Published: Jan. 8, 2025
Diatomic
catalysts
featuring
a
tunable
structure
and
synergetic
effects
hold
great
promise
for
various
reactions.
However,
their
precise
construction
with
specific
configurations
diverse
metal
combinations
is
still
challenging.
Here,
selective
etching
ion
adsorption
strategy
proposed
to
accurately
assign
second
atom
(M2)
geminal
the
single
site
(M1–Nx)
constructing
diatomic
sites
(e.g.,
Fe–Pd,
Fe–Pt,
Fe–Ru,
Fe–Zn,
Co–Fe,
Co–Ni,
Co–Cu).
In
this
strategy,
hydrogen
peroxide
selectively
etches
positively
charged
carbon
atoms
near
M1–Nx
moiety
(denoted
as
α-C)
produces
vacancy,
which
could
trap
M2
at
subsequent
step.
These
show
optimized
electronic
enhanced
oxygen
reduction
activity
compared
single-site
counterparts,
representative
Fe–Pd–NC
Co–Fe–NC
stand
most
active
reaction
(half-wave
potential
of
0.92
0.91
V,
respectively).
The
α-C
in
single-atom
reported
here
represents
new
post-treatment
targeting
synthesis
sites.
ACS Catalysis,
Journal Year:
2025,
Volume and Issue:
15(3), P. 1477 - 1486
Published: Jan. 9, 2025
Electronic
perturbation
induced
by
the
microenvironment
regulation
adjacent
to
FeN4
sites
anchored
on
metal–N–C
materials
will
accelerate
its
oxygen
reduction
reaction
(ORR)
kinetics.
Herein,
we
report
a
fine-tuning
in
charge
configuration
of
through
defect-rich
N/S-doped
carbon
nest
derived
from
chemically
cross-linked
pyrrole/thiophene
copolymer
(CCPPT)
with
sp3-hybridized
cross-linker.
Compared
(PPT)
without
cross-linker,
CCPPT
knitted
three-dimensional
(3D)
network
delivers
higher
defect
density
and
∼2-fold
sulfur
retention
after
pyrolysis.
The
structural
characterizations
combined
theoretical
calculations
suggest
that
vacancy
defects
(Cvd)
FeN4/S2
moiety
together
induce
redistribution
resultant
CC-Fe1/NSC
CCPPT,
reducing
adsorption
strength
oxygen-containing
intermediates
energy
barrier
ORR.
As
expected,
shows
an
impressive
half-wave
potential
∼0.91
V
vs
reversible
hydrogen
electrode
(RHE),
surpassing
both
PPT-derived
Fe1/NSC
(0.88
V)
commercial
Pt/C
(0.86
V).
This
work
provides
distinctive
path
manipulate
single-atom
catalysts
toward
ORR
or
even
beyond.
Research Square (Research Square),
Journal Year:
2025,
Volume and Issue:
unknown
Published: Feb. 14, 2025
Abstract
Dual
atom
catalysts
(DACs),
characterized
by
high
activity
and
metal
utilization,
as
well
structural
diversity
with
a
large
variety
of
catalytic
sites,
hold
immense
promise
for
energy
conversion
technologies,
garnering
substantial
interest
from
both
academia
industry.
However,
achieving
precise
control
manipulation
atomic
dispersion,
pairing
ratios,
interatomic
distances
in
DACs,
which
significantly
affect
their
multifunctional
properties,
remains
significant
challenge.
Herein,
we
developed
ligand-restricted
strategy
the
synthesis
highly
DACs
tunable
distances.
This
was
accomplished
coordinating
diamine
ligands
dual
precursors,
restricting
relative
positions
two
atoms
on
two-dimensional
graphitic
carbon
nitride.
The
ratio
exceeded
82%,
chain
length
molecules
effectively
regulating
distance
between
paired
atoms.
As
demonstration,
Pt1-Au1
exhibited
almost
three
times
nitrate
reduction
to
ammonia
compared
unpaired
counterparts.
Furthermore,
shorter
distanced
DAC
reveals
four
photothermal
catalyzed
hydrogenation
reactions
than
longer
ones.
work
not
only
introduces
novel
design
atomic-scale
fabrication
complex
but
also
provides
valuable
insights
into
nanoscale
reaction
mechanisms
heterogeneous
catalysis.
ACS Nano,
Journal Year:
2025,
Volume and Issue:
unknown
Published: April 4, 2025
Dual-atom
catalysts
(DACs)
have
shown
significant
application
potential
in
Fenton-like
reactions.
However,
effectively
modulating
their
electronic
structure
and
fully
understanding
the
mechanisms
driving
high
catalytic
activity
remain
challenging.
Herein,
we
propose
a
coordination
anions
dimensionality
engineering
strategy
to
synthesize
biomass-derived
dual-atom
FeCo-N4O1C
catalysts,
which
Fe
Co
atoms
are
bridged
by
two-dimensional
planar
N
three-dimensional
(3D)
axial
O
atom.
Experimental
data
theoretical
calculations
reveal
that
3D
of
induces
spin
state
undergo
transition
from
low
an
intermediate
compared
with
single-atom
Fe-N4O1C,
resulting
moderate
adsorption
desorption
intermediates,
thus
reducing
energy
barriers
for
generating
more
singlet
oxygen
high-valent
cobalt-oxo
species
during
peroxymonosulfate
activation.
The
electron
transfer
neighboring
through
can
prevent
poisoning
active
species.
Benefiting
synergistic
effects
multiple
sites,
catalyst-dose
normalized
reaction
rate
constant
reaches
14.5
L
min-1
g-1
under
concentrations─an
improvement
1
∼
2
orders
magnitude
over
most
reported
catalysts.
practical
applicability
is
demonstrated
nearly
100%
pollutant
removal
7
days
continuous
operation
membrane
filtration
system.
This
study
provides
deep
insights
into
relationship
between
performance
spin-state
regulation
DACs,
introduces
promising
approach
large-scale
synthesis
low-cost,
highly
efficient
DACs