Angewandte Chemie,
Год журнала:
2024,
Номер
unknown
Опубликована: Окт. 9, 2024
Abstract
Establishing
a
targeted
switch
for
CO
2
conversion
under
electric
drive
is
essential
achieving
carbon‐balance
by
enabling
selective
chemicals.
However,
engineering
the
topological
assembly
of
active
sites
to
precisely
regulate
competing
pathways
various
intermediates
has
been
plagued
unclear
structure‐function
relationships.
To
tailor
CO/formate
pathways,
herein
we
established
robust
nonlinear
with
tunable
Co
x
integrated
into
Pd
metallene,
which
involves
1
/Pd
single‐atom
alloy
(favoring
CO)
and
diatomic
formate).
Transitioning
from
atomic
bimetallenes
resulted
in
nonlinear,
high‐contrast
flip
selectivity,
surpassing
94
%
formate
productions
both
H‐cell
flow
cell.
Furthermore,
superior
selectivity
current
efficiency
(>80
%)
(>88
were
consistently
maintained
at
−150
mA
cm
−2
over
continuous
200
h.
Theoretical
simulations
situ
spectroscopy
analyses
unveiled
that
appropriate
adjacent
metal
site
combinations
(Pd−Pd,
Pd−Co
Co−Co)
lead
d
z
band
center
shift
preferred
adsorption
configurations
intermediates,
dictating
C
pathways.
Our
finding
reveals
desired
stability
within
system,
providing
new
perspective
fine‐tuning
energy
processes
through
specific
assembly.
Angewandte Chemie International Edition,
Год журнала:
2024,
Номер
unknown
Опубликована: Окт. 9, 2024
Abstract
Establishing
a
targeted
switch
for
CO
2
conversion
under
electric
drive
is
essential
achieving
carbon‐balance
by
enabling
selective
chemicals.
However,
engineering
the
topological
assembly
of
active
sites
to
precisely
regulate
competing
pathways
various
intermediates
has
been
plagued
unclear
structure‐function
relationships.
To
tailor
CO/formate
pathways,
herein
we
established
robust
nonlinear
with
tunable
Co
x
integrated
into
Pd
metallene,
which
involves
1
/Pd
single‐atom
alloy
(favoring
CO)
and
diatomic
formate).
Transitioning
from
atomic
bimetallenes
resulted
in
nonlinear,
high‐contrast
flip
selectivity,
surpassing
94
%
formate
productions
both
H‐cell
flow
cell.
Furthermore,
superior
selectivity
current
efficiency
(>80
%)
(>88
were
consistently
maintained
at
−150
mA
cm
−2
over
continuous
200
h.
Theoretical
simulations
situ
spectroscopy
analyses
unveiled
that
appropriate
adjacent
metal
site
combinations
(Pd−Pd,
Pd−Co
Co−Co)
lead
d
z
band
center
shift
preferred
adsorption
configurations
intermediates,
dictating
C
pathways.
Our
finding
reveals
desired
stability
within
system,
providing
new
perspective
fine‐tuning
energy
processes
through
specific
assembly.
Angewandte Chemie,
Год журнала:
2024,
Номер
unknown
Опубликована: Окт. 9, 2024
Abstract
Establishing
a
targeted
switch
for
CO
2
conversion
under
electric
drive
is
essential
achieving
carbon‐balance
by
enabling
selective
chemicals.
However,
engineering
the
topological
assembly
of
active
sites
to
precisely
regulate
competing
pathways
various
intermediates
has
been
plagued
unclear
structure‐function
relationships.
To
tailor
CO/formate
pathways,
herein
we
established
robust
nonlinear
with
tunable
Co
x
integrated
into
Pd
metallene,
which
involves
1
/Pd
single‐atom
alloy
(favoring
CO)
and
diatomic
formate).
Transitioning
from
atomic
bimetallenes
resulted
in
nonlinear,
high‐contrast
flip
selectivity,
surpassing
94
%
formate
productions
both
H‐cell
flow
cell.
Furthermore,
superior
selectivity
current
efficiency
(>80
%)
(>88
were
consistently
maintained
at
−150
mA
cm
−2
over
continuous
200
h.
Theoretical
simulations
situ
spectroscopy
analyses
unveiled
that
appropriate
adjacent
metal
site
combinations
(Pd−Pd,
Pd−Co
Co−Co)
lead
d
z
band
center
shift
preferred
adsorption
configurations
intermediates,
dictating
C
pathways.
Our
finding
reveals
desired
stability
within
system,
providing
new
perspective
fine‐tuning
energy
processes
through
specific
assembly.
