Angewandte Chemie International Edition,
Год журнала:
2022,
Номер
62(3)
Опубликована: Ноя. 18, 2022
Precise
design
and
tuning
of
the
micro-atomic
structure
single
atom
catalysts
(SACs)
can
help
efficiently
adapt
complex
catalytic
systems.
Herein,
we
inventively
found
that
when
active
center
main
group
element
gallium
(Ga)
is
downsized
to
atomic
level,
whose
characteristic
has
significant
differences
from
conventional
bulk
rigid
Ga
catalysts.
The
SACs
with
a
P,
S
coordination
environment
display
specific
flow
properties,
showing
CO
products
FE
≈92
%
at
-0.3
V
vs.
RHE
in
electrochemical
CO2
reduction
(CO2
RR).
Theoretical
simulations
demonstrate
adaptive
dynamic
transition
optimizes
adsorption
energy
*COOH
intermediate
renews
sites
time,
leading
excellent
RR
selectivity
stability.
This
liquid
system
interfaces
lays
foundation
for
future
exploration
synthesis
catalysis.
Angewandte Chemie International Edition,
Год журнала:
2022,
Номер
61(12)
Опубликована: Янв. 10, 2022
Constructing
monodispersed
metal
sites
in
heterocatalysis
is
an
efficient
strategy
to
boost
their
catalytic
performance.
Herein,
a
new
using
tailor
Pt-based
nanocatalysts
addressed
by
engineering
unconventional
p-d
orbital
hybridization.
Thus,
Ga
on
Pt3
Mn
nanocrystals
(Ga-O-Pt3
Mn)
with
high-indexed
facets
was
constructed
for
the
first
time
drive
ethanol
electrooxidation
reaction
(EOR).
Strikingly,
Ga-O-Pt3
nanocatalyst
shows
enhanced
EOR
performance
achieving
8.41
times
of
specific
activity
than
that
Pt/C.
The
electrochemical
situ
Fourier
transform
infrared
spectroscopy
results
and
theoretical
calculations
disclose
featuring
hybridization
not
only
promote
C-C
bond-breaking
rapid
oxidation
-OH
ethanol,
but
also
inhibit
generation
poisonous
CO
intermediate
species.
This
work
discloses
promising
construct
novel
tailored
site
as
fuel
cell
catalysts.
Advanced Materials,
Год журнала:
2023,
Номер
35(31)
Опубликована: Фев. 23, 2023
Single/dual-metal
atoms
supported
on
carbon
matrix
can
be
modulated
by
coordination
structure
and
neighboring
active
sites.
Precisely
designing
the
geometric
electronic
uncovering
structure-property
relationships
of
single/dual-metal
confront
with
grand
challenges.
Herein,
this
review
summarizes
latest
progress
in
microenvironment
engineering
single/dual-atom
sites
via
a
comprehensive
comparison
single-atom
catalyst
(SACs)
dual-atom
catalysts
(DACs)
term
design
principles,
modulation
strategy,
theoretical
understanding
structure-performance
correlations.
Subsequently,
recent
advances
several
typical
electrocatalysis
process
are
discussed
to
get
general
reaction
mechanisms
finely-tuned
SACs
DACs.
Finally,
full-scaled
summaries
challenges
prospects
given
for
This
will
provide
new
inspiration
development
atomically
dispersed
electrocatalytic
application.
Angewandte Chemie International Edition,
Год журнала:
2022,
Номер
61(34)
Опубликована: Июнь 18, 2022
Single-atom
active-site
catalysts
have
attracted
significant
attention
in
the
field
of
photocatalytic
CO2
conversion.
However,
designing
active
sites
for
reduction
and
H2
O
oxidation
simultaneously
on
a
photocatalyst
combining
corresponding
half-reaction
system
is
still
difficult.
Here,
we
synthesized
bimetallic
single-atom
with
two
compatible
centers
Mn
Co
carbon
nitride
(Mn1
Co1
/CN).
Our
experimental
results
density
functional
theory
calculations
showed
that
center
promotes
by
accumulating
photogenerated
holes.
In
addition,
activation
increasing
bond
length
angle
molecules.
Benefiting
from
synergistic
effect
atomic
centers,
Mn1
/CN
exhibited
CO
production
rate
47
μmol
g-1
h-1
,
which
significantly
higher
than
single-metal
photocatalyst.
Angewandte Chemie International Edition,
Год журнала:
2022,
Номер
62(3)
Опубликована: Ноя. 18, 2022
Precise
design
and
tuning
of
the
micro-atomic
structure
single
atom
catalysts
(SACs)
can
help
efficiently
adapt
complex
catalytic
systems.
Herein,
we
inventively
found
that
when
active
center
main
group
element
gallium
(Ga)
is
downsized
to
atomic
level,
whose
characteristic
has
significant
differences
from
conventional
bulk
rigid
Ga
catalysts.
The
SACs
with
a
P,
S
coordination
environment
display
specific
flow
properties,
showing
CO
products
FE
≈92
%
at
-0.3
V
vs.
RHE
in
electrochemical
CO2
reduction
(CO2
RR).
Theoretical
simulations
demonstrate
adaptive
dynamic
transition
optimizes
adsorption
energy
*COOH
intermediate
renews
sites
time,
leading
excellent
RR
selectivity
stability.
This
liquid
system
interfaces
lays
foundation
for
future
exploration
synthesis
catalysis.
