Small,
Journal Year:
2024,
Volume and Issue:
unknown
Published: Dec. 9, 2024
Abstract
A
universal
method
is
demonstrated
for
the
fabrication
of
large‐area
highly
ordered
microporous
arrayed
metal
oxides
based
on
a
high‐quality
self‐assembly
opal
template
combined
with
sucrose‐assisted
sol‐gel
technique.
Sucrose
as
chelating
agent
optimizes
precursor
infiltration
and
regulates
both
oxide
formation
melting
process
polystyrene
templates,
thus
preventing
crack
during
calcination.
As
result,
over
20
element‐based
3DOM
arbitrary
compositions
are
successfully
prepared.
Therein,
champion
electrocatalyst
RuCoO
x
‐IO
exhibits
outstanding
bifunctional
oxygen
activity
an
ultra‐narrow
potential
gap
0.598
V,
Zn‐air
batteries
air
cathode
operates
1380
h
under
fast‐charging
cycling
(50
mA
cm
−2
),
reaches
high
energy
efficiency
69.5%
in
discharge‐charge
cycling.
In
situ
spectroscopy
characterizations
density
functional
theory
reveal
that
rational
construction
Ru─O─Co
heterointerface
decoupled
multi‐active
sites
mutual
coupling
RuO
2
Co
3
O
4
facilitate
interfacial
electron
transfer,
leading
to
optimized
d
‐band
centers
active
Ru/Co
weakened
spin
interaction
between
intermediates
sites,
so
enhance
adsorption
ability
*
OOH
fast
ORR
kinetics
while
favoring
desorption
Ru
OER.
Advanced Functional Materials,
Journal Year:
2024,
Volume and Issue:
unknown
Published: Sept. 27, 2024
Abstract
Integrating
active
sites
for
oxygen
reduction
and
evolution
reactions
(ORR
OER)
is
pivotal
advancing
bifunctional
electrodes.
Addressing
the
geometric/electronic
properties
of
these
essential
to
disrupt
linear
scaling
relationship
between
adsorption
desorption
complex
intermediates.
Herein,
a
proof‐of‐concept
presented
constructing
asymmetric
trinuclear
employing
both
composition‐
size‐based
coupling
strategies.
These
comprise
ORR‐active
Fe
single
atom
(Fe
SA
),
OER‐active
atomically
clustered
species
AC
Ni
as
modulators.
This
AC‐SA
‐Ni
@N‐doped
carbon
exhibits
excellent
catalytic
activities,
with
narrow
potential
gap
0.661
V
an
ORR
half‐wave
0.931
OER
1.592
at
10
mA
cm
−2
.
The
Zn‐air
battery
this
material
achieves
peak
power
density
293
mW
,
specific
capacity
748
mAh
g
Zn
−1
remarkable
stability.
Experimental
findings
theoretical
simulations
reveal
that
induced
strong
electronic
among
centers,
facilitating
charge
redistribution
optimizing
barriers
enhances
rapid
release
*
OH
during
efficient
transformation
from
O
OOH
OER.
study
presents
novel
strategy
developing
robust
Journal of Materials Chemistry A,
Journal Year:
2024,
Volume and Issue:
12(27), P. 16863 - 16876
Published: Jan. 1, 2024
The
symmetric
electronic
structure
of
an
Fe
single-atom
site
catalyst
was
effectively
regulated
by
incorporating
Co–N
x
sites
and
core–shell
Co
3
7
@C
nanoparticles,
resulting
in
high
performance
towards
the
ORR
Zn–air
batteries.
Journal of Materials Chemistry A,
Journal Year:
2024,
Volume and Issue:
12(39), P. 26316 - 26349
Published: Jan. 1, 2024
Dual-atom
catalysts
(DACs)
have
emerged
as
highly
promising
and
efficient
for
water
electrolysis,
primarily
due
to
their
distinct
dual-atom
site
effects.
ACS Nano,
Journal Year:
2025,
Volume and Issue:
unknown
Published: March 22, 2025
Rational
regulation
of
the
coordination
environment
single-atom
catalysts
(SACs)
is
a
promising
yet
challenging
strategy
to
enhance
their
activity.
Here,
we
introduce
an
O
atom
into
second
shell
Co–N4
sites
via
simple
thermal
treatment,
forming
Co–N4–ON
matrix
boost
photosynthetic
hydrogen
peroxide
(H2O2)
production.
This
modification
significantly
alters
electronic
structure
Co
site,
bringing
d-band
center
closer
Fermi
energy
and
elevating
conduction
band
Co–N4–CN
its
reducing
capacity.
Density
functional
theory
(DFT)
calculations
reveal
intensified
charge
redistribution
reduced
work
function
in
Co–N4–ON,
facilitating
O2
adsorption.
Notably,
exhibits
lowest
adsorption
energy,
indicating
stronger
interaction
between
Co–N4–O
O2,
which
further
strengthened
by
orbital
hybridization
transfer
at
interface,
leading
enhanced
activation.
The
optimized
catalyst
demonstrates
superior
reduction
capabilities
with
barrier
during
H2O2
desorption.
Consequently,
it
achieves
production
rate
3098.18
μmol
g–1
h–1
under
neutral
conditions,
2.6
times
higher
than
that
Co–N4–CN.
Moreover,
maintains
1967.79
over
10
h
continuous
flow
reactor
natural
sunlight
ambient
air,
highlighting
durability
practicality.
study
underscores
crucial
role
SACs
offers
valuable
insights
atomic-level
structure–activity
relationships,
thus
contributing
advancements
design
for
efficient