Photocatalytic
Fenton-coupled
oxygen
reduction
reaction
(ORR)
is
a
promising
strategy
for
•OH
production.
Single-atom
catalysts
(SACs),
featuring
high
atom
utilization,
exhibit
superior
catalytic
activity.
However,
it
remains
challenge
to
synchronously
achieve
efficient
catalysis
of
both
steps
on
one
active
site.
Herein,
novel
Co-Fe
hetero-atom
pair
tandem
photocatalyst
was
precisely
constructed
by
pre-designing
the
structure
covalent
organic
frameworks
(COFs)
and
introduction
strategies
sites.
Thanks
synergism
neighboring
atoms,
Co-Fe-COF
presents
highly
hydroxyl
radicals
production
following
process
O2+H2O→H2O2→•OH.
Additionally,
immobilization
pairs
pore
walls
COF
can
boost
enrichment
contaminants,
thus
increasing
utilization
•OH.
Theoretical
simulations
reveal
proximity
electronic
effect
O-bridged
not
only
thermodynamically
promotes
formation
OOH*,
but
also
dynamically
activates
self-healing
cycle
Fe(II)/Fe(III).
This
work
provides
routine
designing
high-performance
catalysts.
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:
2023,
Номер
63(6)
Опубликована: Дек. 16, 2023
Addressing
the
limitations
arising
from
consistent
catalytic
behavior
observed
for
various
intermediates
during
electrochemical
carbon
dioxide
reduction
reaction
(CO
