Advanced Functional Materials,
Journal Year:
2023,
Volume and Issue:
33(16)
Published: Feb. 2, 2023
Abstract
Reverse
water‐gas
shift
(RWGS)
reaction
is
the
initial
and
necessary
step
of
CO
2
hydrogenation
to
high
value‐added
products,
regulating
selectivity
still
a
fundamental
challenge.
In
present
study,
an
efficient
catalyst
(CuZnN
x
@C‐N)
composed
by
Zn
single
atoms
Cu
clusters
stabilized
nitrogen
sites
reported.
It
contains
saturated
four‐coordinate
Zn‐N
4
low
valence
CuN
clusters.
Monodisperse
induces
aggregation
pyridinic
N
form
structures,
which
show
strong
Lewis
basicity
has
adsorption
for
*CO
*COOH
intermediates,
but
weak
*CO,
thus
greatly
improves
conversion
selectivity.
The
calcined
at
700
°C
exhibits
highest
43.6%
under
atmospheric
pressure,
18.33
times
Cu‐ZnO
close
thermodynamic
equilibrium
rate
(49.9%)
.
catalytic
process,
not
only
adsorbs
activates
H
,
also
cooperates
with
adjacent
structures
jointly
activate
molecules
further
promotes
This
synergistic
mechanism
will
provide
new
insights
developing
catalysts.
Advanced Energy Materials,
Journal Year:
2023,
Volume and Issue:
13(19)
Published: April 4, 2023
Abstract
Constructing
Cu
0
–Cu
+
double‐active
sites
is
significant
for
C–C
coupling
to
produce
multicarbon
products
during
the
CO
2
electrocatalytic
reduction
process.
However,
Cu‐based
precursors
(including
)
are
easily
reduced
,
especially
at
large
current
densities.
Thus,
developing
a
facile
stabilization
method
form
highly
desirable
but
challenging.
Herein,
fullerene
(C
60
used
as
an
electronic
buffer
stabilize
site.
Then,
composite
of
copper
oxide
and
C
precursor
designed
obtain
catalyst
consisting
in
situ
formed
sites.
The
not
only
delivers
up
61%
2+
Faraday
efficiency
partial
density
366
mA
cm
−2
also
exhibits
good
12
h
durability
site
−1.4
V
versus
reversible
hydrogen
electrode.
Moreover,
revealed
induce
preferential
*CO
*CHO
over
dimerization,
accounting
enhanced
selectivity.
Advanced Materials,
Journal Year:
2023,
Volume and Issue:
35(52)
Published: Aug. 20, 2023
Abstract
Electrochemical
carbon
dioxide
reduction
reaction
(CO
2
RR)
driven
by
renewable
energy
shows
great
promise
in
mitigating
and
potentially
reversing
the
devastating
effects
of
anthropogenic
climate
change
environmental
degradation.
The
simultaneous
synthesis
energy‐dense
chemicals
can
meet
global
demand
while
decoupling
emissions
from
economic
growth.
However,
development
CO
RR
technology
faces
challenges
catalyst
discovery
device
optimization
that
hinder
their
industrial
implementation.
In
this
contribution,
a
comprehensive
overview
current
state
research
is
provided,
starting
with
background
motivation
for
technology,
followed
fundamentals
evaluated
metrics.
Then
underlying
design
principles
electrocatalysts
are
discussed,
emphasizing
structure–performance
correlations
advanced
electrochemical
assembly
cells
increase
selectivity
throughput.
Finally,
review
looks
to
future
identifies
opportunities
innovation
mechanism
discovery,
material
screening
strategies,
assemblies
move
toward
carbon‐neutral
society.
Angewandte Chemie International Edition,
Journal Year:
2023,
Volume and Issue:
63(7)
Published: Dec. 29, 2023
Abstract
Photocatalytic
conversion
of
CO
2
and
H
O
into
fuels
oxygen
is
a
highly
promising
solution
for
carbon‐neutral
recycling.
Traditionally,
researchers
have
studied
reduction
oxidation
separately,
overlooking
potential
synergistic
interplay
between
these
processes.
This
study
introduces
an
innovative
approach,
spatial
synergy,
which
encourages
progress
by
bringing
the
two
half‐reactions
atomic
proximity.
To
facilitate
this,
we
developed
defective
ZnIn
S
4
‐supported
single‐atom
Cu
catalyst
(Cu−SA/D−ZIS),
demonstrates
remarkable
catalytic
performance
with
rates
112.5
μmol
g
−1
h
water
52.3
,
exhibiting
six‐fold
enhancement
over
D−ZIS.
The
structural
characterization
results
indicated
that
trapping
effect
vacancy
associates
on
copper
led
to
formation
unsaturated
coordination
structure,
Cu‐S
3
consequently
giving
rise
Zn
′
V
⋅⋅
“
defect
complexes.
FT‐IR
studies
coupled
theoretical
calculations
reveal
spatially
”,
where
breakage
O−H
in
synchronized
*COOH,
significantly
lowering
energy
barrier.
Notably,
this
and,
first
time,
substantiates
synergy
through
combination
experimental
analyses,
providing
fresh
insight
optimizing
photocatalytic
system.
Advanced Functional Materials,
Journal Year:
2023,
Volume and Issue:
33(16)
Published: Feb. 2, 2023
Abstract
Reverse
water‐gas
shift
(RWGS)
reaction
is
the
initial
and
necessary
step
of
CO
2
hydrogenation
to
high
value‐added
products,
regulating
selectivity
still
a
fundamental
challenge.
In
present
study,
an
efficient
catalyst
(CuZnN
x
@C‐N)
composed
by
Zn
single
atoms
Cu
clusters
stabilized
nitrogen
sites
reported.
It
contains
saturated
four‐coordinate
Zn‐N
4
low
valence
CuN
clusters.
Monodisperse
induces
aggregation
pyridinic
N
form
structures,
which
show
strong
Lewis
basicity
has
adsorption
for
*CO
*COOH
intermediates,
but
weak
*CO,
thus
greatly
improves
conversion
selectivity.
The
calcined
at
700
°C
exhibits
highest
43.6%
under
atmospheric
pressure,
18.33
times
Cu‐ZnO
close
thermodynamic
equilibrium
rate
(49.9%)
.
catalytic
process,
not
only
adsorbs
activates
H
,
also
cooperates
with
adjacent
structures
jointly
activate
molecules
further
promotes
This
synergistic
mechanism
will
provide
new
insights
developing
catalysts.
