Angewandte Chemie International Edition,
Год журнала:
2023,
Номер
62(42)
Опубликована: Июнь 14, 2023
Dual-atom
catalysts
(DACs)
have
been
a
new
frontier
in
heterogeneous
catalysis
due
to
their
unique
intrinsic
properties.
The
synergy
between
dual
atoms
provides
flexible
active
sites,
promising
enhance
performance
and
even
catalyze
more
complex
reactions.
However,
precisely
regulating
site
structure
uncovering
dual-atom
metal
interaction
remain
grand
challenges.
In
this
review,
we
clarify
the
significance
of
inter-metal
DACs
based
on
understanding
center
structures.
Three
diatomic
configurations
are
elaborated,
including
isolated
single-atom,
N/O-bridged
dual-atom,
direct
dual-metal
bonding
interaction.
Subsequently,
up-to-date
progress
oxidation
reactions,
hydrogenation/dehydrogenation
electrocatalytic
photocatalytic
reactions
summarized.
structure-activity
relationship
catalytic
is
then
discussed
at
an
atomic
level.
Finally,
challenges
future
directions
engineer
discussed.
This
review
will
offer
prospects
for
rational
design
efficient
toward
catalysis.
ACS Nano,
Год журнала:
2023,
Номер
17(7), С. 6955 - 6965
Опубликована: Март 27, 2023
Controlling
atomic
adjustment
of
single-atom
catalysts
(SACs)
can
directly
change
its
local
configuration,
regulate
the
energy
barrier
intermediates,
and
further
optimize
reaction
pathways.
Herein,
we
report
an
atom
manipulating
process
to
synthesize
Ni
atoms
stabilized
on
vanadium
carbide
(NiSA-VC)
through
a
nanofiber-medium
thermodynamically
driven
migration
strategy.
Experimental
theoretical
results
systematically
reveal
tunable
pathway
from
nanoparticles
neighboring
N-doped
carbon
(NC)
finally
metal
that
was
obtained
by
regulating
competitive
adsorption
energies
between
VC
NC
for
capturing
atoms.
For
CO2-to-CO
electroreduction,
NiSA-VC
exhibits
industrial
current
density
-180
mA
cm-2
at
-1.0
V
vs
reversible
hydrogen
electrode
highest
Faradaic
efficiency
CO
production
(FECO)
96.8%
-0.4
RHE
in
flow
cell.
Significant
electron
transfers
occurring
structures
contribute
activation
CO2,
facilitate
free
energy,
*CO
desorption
as
rate-determining
step,
promote
activity
selectivity.
This
study
provides
understanding
how
design
powerful
SACs
electrocatalysis.
Nanoscale,
Год журнала:
2023,
Номер
15(28), С. 11759 - 11776
Опубликована: Янв. 1, 2023
Water
electro-splitting
driven
by
renewable
energy
is
significant
in
conversion
for
the
development
of
hydrogen
sources.
The
evolution
reaction
(HER)
directly
generating
products
occurs
cathode
catalysis.
Over
years,
progress
has
been
made
to
boost
HER
efficiency
exploratively
designing
highly
active
and
economical
Pt-based
electrocatalysts.
However,
there
are
still
some
urgent
problems
be
solved
catalysts
more
alkaline
electrolytes,
such
as
slow
kinetics
caused
additional
hydrolysis
dissociation
steps,
which
greatly
hinders
practical
application.
This
review
systematically
summarizes
several
strategies
optimizing
provides
direct
guidelines
design
Specifically,
intrinsic
activity
water
electrolysis
can
boosted
accelerating
dissociation,
binding
or
modulating
spatial
dimensions
electrocatalyst
based
on
mechanism.
Finally,
we
prospect
challenges
novel
electrocatalysts,
including
site
study,
mechanism
exploration
extensible
catalyst
preparation
technologies.
Angewandte Chemie International Edition,
Год журнала:
2023,
Номер
62(19)
Опубликована: Март 9, 2023
Developing
easily
accessible
descriptors
is
crucial
but
challenging
to
rationally
design
single-atom
catalysts
(SACs).
This
paper
describes
a
simple
and
interpretable
activity
descriptor,
which
obtained
from
the
atomic
databases.
The
defined
descriptor
proves
accelerate
high-throughput
screening
of
more
than
700
graphene-based
SACs
without
computations,
universal
for
3-5d
transition
metals
C/N/P/B/O-based
coordination
environments.
Meanwhile,
analytical
formula
this
reveals
structure-activity
relationship
at
molecular
orbital
level.
Using
electrochemical
nitrogen
reduction
as
an
example,
descriptor's
guidance
role
has
been
experimentally
validated
by
13
previous
reports
well
our
synthesized
4
SACs.
Orderly
combining
machine
learning
with
physical
insights,
work
provides
new
generalized
strategy
low-cost
while
comprehensive
understanding
structure-mechanism-activity
relationship.
Angewandte Chemie International Edition,
Год журнала:
2023,
Номер
62(42)
Опубликована: Июнь 14, 2023
Dual-atom
catalysts
(DACs)
have
been
a
new
frontier
in
heterogeneous
catalysis
due
to
their
unique
intrinsic
properties.
The
synergy
between
dual
atoms
provides
flexible
active
sites,
promising
enhance
performance
and
even
catalyze
more
complex
reactions.
However,
precisely
regulating
site
structure
uncovering
dual-atom
metal
interaction
remain
grand
challenges.
In
this
review,
we
clarify
the
significance
of
inter-metal
DACs
based
on
understanding
center
structures.
Three
diatomic
configurations
are
elaborated,
including
isolated
single-atom,
N/O-bridged
dual-atom,
direct
dual-metal
bonding
interaction.
Subsequently,
up-to-date
progress
oxidation
reactions,
hydrogenation/dehydrogenation
electrocatalytic
photocatalytic
reactions
summarized.
structure-activity
relationship
catalytic
is
then
discussed
at
an
atomic
level.
Finally,
challenges
future
directions
engineer
discussed.
This
review
will
offer
prospects
for
rational
design
efficient
toward
catalysis.
