Advanced Science,
Год журнала:
2025,
Номер
unknown
Опубликована: Апрель 26, 2025
Abstract
Atomic‐level
catalysts
are
extensively
applied
in
heterogeneous
catalysis
fields.
However,
it
is
a
general
but
ineluctable
issue
that
active
metal
atoms
may
migrate,
aggregate,
deactivate,
or
leach
during
reaction
processes,
suppressing
their
catalytic
performances.
Designing
superior
intrinsic‐structural
stability
of
atomic‐level
with
high
activity
and
revealing
dynamic
structure
evolution
vital
for
wide
applications
complex
reactions
harsh
conditions.
Herein,
high‐stable
Pd─Cu
dual‐atom
PdN
3
─CuN
coordination
engineered
via
strong
chelation
Cu
2+
‐ions
electron
pairs
from
palladium‐source,
achieving
the
highest
turnover
frequency
under
lowest
overpotential
Cr(VI)
electrocatalytic
reduction
detection
strong‐acid
electrolytes.
In
situ
X‐ray
absorption
fine
spectra
reveal
“spring‐effect”
Cu─Pd
Cu─N
bonds
reversibly
stretched
potential
changes
can
be
recovered
at
0.6
V
regeneration.
The
modulated
electron‐orbit
coupling
effect
prevents
Cu‐atoms
aggregating
as
metallic
nanoparticles.
dual‐atoms
interact
two
O
H
2
CrO
4
,
forming
stable
bridge
configurations
transferring
electrons
to
promote
Cr─O
bond
dissociation,
which
prominently
decreases
energy
barriers.
This
work
provides
feasible
route
boost
robustness
single‐atoms
easily
affected
by
conditions
sustainable
applications.
Chemical Science,
Год журнала:
2024,
Номер
15(29), С. 11188 - 11228
Опубликована: Янв. 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
Chemical Science,
Год журнала:
2024,
Номер
15(36), С. 14585 - 14607
Опубликована: Янв. 1, 2024
The
development
of
high-efficiency
atomic-level
catalysts
for
energy-conversion
and
-storage
technologies
is
crucial
to
address
energy
shortages.
spin
states
diatomic
(DACs)
are
closely
tied
their
catalytic
activity.
Adjusting
the
DACs'
active
centers
can
directly
modify
occupancy
d-orbitals,
thereby
influencing
bonding
strength
between
metal
sites
intermediates
as
well
transfer
during
electro
reactions.
Herein,
we
discuss
various
techniques
characterizing
atomic
strategies
modulating
center
states.
Next,
outline
recent
progress
in
study
effects
DACs
oxygen
reduction
reaction
(ORR),
evolution
(OER),
hydrogen
(HER),
electrocatalytic
nitrogen/nitrate
(eNRR/NO
Angewandte Chemie International Edition,
Год журнала:
2024,
Номер
64(1)
Опубликована: Авг. 22, 2024
Single-atom
nanozymes
(SAzymes)
with
ultrahigh
atom
utilization
efficiency
have
been
extensively
applied
in
reactive
oxygen
species
(ROS)-mediated
cancer
therapy.
However,
the
high
energy
barriers
of
reaction
intermediates
on
single-atom
sites
and
overexpressed
antioxidants
tumor
microenvironment
restrict
amplification
oxidative
stress,
resulting
unsatisfactory
therapeutic
efficacy.
Herein,
we
report
a
multi-enzyme
mimetic
MoCu
dual-atom
nanozyme
(MoCu
DAzyme)
various
catalytic
active
sites,
which
exhibits
peroxidase,
oxidase,
glutathione
(GSH)
nicotinamide
adenine
dinucleotide
phosphate
(NADPH)
oxidase
mimicking
activities.
Compared
Mo
SAzyme,
introduction
Cu
atoms,
formation
synergetic
effects
among
enhance
substrate
adsorption
reduce
barrier,
thereby
endowing
DAzyme
stronger
Benefiting
from
above
enzyme-like
activities,
can
not
only
generate
multiple
ROS,
but
also
deplete
GSH
block
its
regeneration
to
trigger
cascade
stress.
Additionally,
strong
optical
absorption
near-infrared
II
bio-window
endows
remarkable
photothermal
conversion
performance.
Consequently,
achieves
high-efficiency
synergistic
treatment
incorporating
collaborative
therapy
This
work
will
advance
applications
DAzymes
provide
valuable
insights
for
nanocatalytic
Advanced Functional Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Март 3, 2025
Abstract
Fe
single‐atom
on
N‐doped
carbon
(FeN‐C)
catalysts
emerge
as
promising
alternatives
to
commercial
Pt/C
for
the
oxygen
reduction
reaction.
Heterogeneous
atom
doping
is
proposed
be
effective
modulating
catalyst
performance.
Despite
this,
relationship
between
fine
coordination
structure
of
doped
atoms
and
catalytic
activity
central
metal
site
remains
poorly
understood.
Herein,
with
S
in
either
first
shell
(FeSN–C)
or
second
(FeN–SC)
active
are
synthesized
compare
effects
different
structure.
FeN–SC
exhibits
prominent
performance
a
half‐wave
potential
0.92
V
rotating
disk
electrode
peak
power
density
251
mW
cm
−2
zinc–air
battery.
Theoretical
studies
reveal
that
effectively
modulates
electronic
charge
transfer
at
center.
Compared
directly
coordinated
within
shell,
located
more
optimizing
adsorption
desorption
energy
barriers
oxygen‐containing
intermediates
sites.
This
study
provides
new
strategy
adjust
by
engineering
multilayer
center
catalyst.
ACS Energy Letters,
Год журнала:
2024,
Номер
9(9), С. 4414 - 4440
Опубликована: Авг. 17, 2024
Electrochemical
reactions,
including
water
splitting,
oxygen
reduction,
hydrogen
oxidation,
carbon
dioxide
nitrogen
oxide
etc.,
are
critical
for
sustainable
energy
conversion
and
storage.
Achieving
high
efficiency
in
these
reactions
requires
catalysts
with
superior
activity,
selectivity,
stability,
often
realized
through
nanostructured
metal
catalysts.
However,
practical
challenges
such
as
low
selectivity
catalytic
degradation
persist.
In
situ
operando
characterization
techniques
offer
real-time
insights
into
catalyst
behavior
under
reaction
conditions,
enabling
a
deeper
understanding
of
structure–performance
relationships
and,
therefore,
guiding
the
design
optimization
electro-catalysts.
This
review
discusses
common
situ/operando
techniques,
highlights
their
applications
model
catalysts,
single-atom
single-crystal
further
explores
combinational
analysis
to
study
complex
nanocatalysts.
Finally,
we
provide
suggestions
perspectives
on
development
advance
field
electrochemical
catalysis.
Angewandte Chemie International Edition,
Год журнала:
2024,
Номер
63(49)
Опубликована: Сен. 13, 2024
Abstract
There
has
been
a
growing
interest
in
developing
catalysts
to
enable
the
reversible
iodine
conversion
reaction
for
high‐performance
aqueous
zinc‐iodine
batteries
(AZIBs).
While
diatomic
(DACs)
have
demonstrated
superior
performance
various
catalytic
reactions
due
their
ability
facilitate
synergistic
charge
interactions,
application
AZIBs
remains
unexplored.
Herein,
we
present,
first
time,
DAC
comprising
Mn−Zn
dual
atoms
anchored
on
nitrogen‐doped
carbon
matrix
(MnZn−NC)
loading,
resulting
AZIB
with
capacity
of
224
mAh
g
−1
at
1
A
and
remarkable
cycling
stability
over
320,000
cycles.
The
electron
hopping
along
Mn−N−Zn
bridge
is
stimulated
via
spin
exchange
mechanism.
This
process
broadens
Mn
3d
xy
band
width
enhances
metallic
character
catalyst,
thus
facilitating
transfer
between
intermediates.
Additionally,
increased
occupancy
within
d‐orbital
Zn
elevates
Zn's
d‐band
center,
thereby
enhancing
chemical
interactions
MnZn−NC
I‐based
species.
Furthermore,
our
mechanism
demonstrates
potential
applicability
other
Metal‐Zn−NC
DACs
spin‐polarized
atoms.
Our
work
elucidates
clear
mechanistic
understanding
provides
new
insights
into
catalyst
design
AZIBs.