New Journal of Chemistry,
Journal Year:
2024,
Volume and Issue:
unknown
Published: Jan. 1, 2024
A
promising
catalyst
for
dispersing
CoPc
on
three-dimensional
porous
carbon
was
prepared
and
showed
impressive
performance
CO
2
electroreduction
to
CO.
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.
Angewandte Chemie,
Journal Year:
2023,
Volume and Issue:
136(6)
Published: Dec. 16, 2023
Abstract
Addressing
the
limitations
arising
from
consistent
catalytic
behavior
observed
for
various
intermediates
during
electrochemical
carbon
dioxide
reduction
reaction
(CO
2
RR)
poses
a
significant
challenge
in
optimization
of
activity.
In
this
study,
we
aimed
to
address
by
constructing
an
asymmetric
coordination
Fe
single
atom
catalyst
(SCA)
with
dynamically
evolved
structure.
Our
catalyst,
consisting
coordinated
one
S
and
three
N
atoms
(Fe−S
1
3
),
exhibited
exceptional
selectivity
Faradaic
efficiency
99.02
%)
demonstrated
high
intrinsic
activity
(TOF
7804.34
h
−1
remarkable
stability.
Using
operando
XAFS
spectra
Density
Functional
Theory
(DFT)
calculations,
elucidated
self‐relaxation
geometric
distortion
dynamic
evolution
bond
lengths
within
catalyst.
These
structure
changes
enabled
independent
regulation
*COOH
*CO
intermediate
adsorption
energies,
effectively
breaking
linear
scale
relationship
enhancing
CO
RR.
This
study
provides
valuable
insights
into
SACs
paves
way
targeted
designs
disrupt
scaling
relationships.
New Journal of Chemistry,
Journal Year:
2024,
Volume and Issue:
unknown
Published: Jan. 1, 2024
A
promising
catalyst
for
dispersing
CoPc
on
three-dimensional
porous
carbon
was
prepared
and
showed
impressive
performance
CO
2
electroreduction
to
CO.