Single-atom
catalysts
(SACs)
have
been
one
of
the
frontiers
in
field
catalysis
recent
years
owing
to
their
high
atomic
utilization
and
unique
electronic
structure.
To
facilitate
practical
application
single-atom,
it
is
vital
develop
a
sustainable,
facile
single-atom
preparation
method
with
mass
production
potential.
Herein,
universal
one-step
electrochemical
synthesis
strategy
proposed,
various
metal-organic
framework-supported
SACs
(including
Pt,
Au,
Ir,
Pd,
Ru,
Mo,
Rh,
W)
are
straightforwardly
obtained
by
simply
replacing
guest
metal
precursors.
As
proof-of-concept,
electrosynthetic
Pt-based
exhibit
outstanding
activity
stability
electrocatalytic
hydrogen
evolution
reaction
(HER).
This
study
not
only
enriches
methodology,
but
also
extends
scenario
synthesis,
opening
up
new
avenues
for
design
advanced
electro-synthesized
catalysts.
Chemical Reviews,
Год журнала:
2023,
Номер
123(9), С. 6257 - 6358
Опубликована: Март 21, 2023
The
oxygen
evolution
reaction
(OER)
and
reduction
(ORR)
are
core
steps
of
various
energy
conversion
storage
systems.
However,
their
sluggish
kinetics,
i.e.,
the
demanding
multielectron
transfer
processes,
still
render
OER/ORR
catalysts
less
efficient
for
practical
applications.
Moreover,
complexity
catalyst–electrolyte
interface
makes
a
comprehensive
understanding
intrinsic
mechanisms
challenging.
Fortunately,
recent
advances
in
situ/operando
characterization
techniques
have
facilitated
kinetic
monitoring
under
conditions.
Here
we
provide
selected
highlights
mechanistic
studies
with
main
emphasis
placed
on
heterogeneous
systems
(primarily
discussing
first-row
transition
metals
which
operate
basic
conditions),
followed
by
brief
outlook
molecular
catalysts.
Key
sections
this
review
focused
determination
true
active
species,
identification
sites,
reactive
intermediates.
For
in-depth
insights
into
above
factors,
short
overview
metrics
accurate
characterizations
is
provided.
A
combination
obtained
time-resolved
information
reliable
activity
data
will
then
guide
rational
design
new
Strategies
such
as
optimizing
restructuring
process
well
overcoming
adsorption-energy
scaling
relations
be
discussed.
Finally,
pending
current
challenges
prospects
toward
development
homogeneous
presented.
Advanced Materials,
Год журнала:
2023,
Номер
36(10)
Опубликована: Фев. 11, 2023
Nanozymes,
a
class
of
nanomaterials
mimicking
the
function
enzymes,
have
aroused
much
attention
as
candidate
in
diverse
fields
with
arbitrarily
tunable
features
owing
to
diversity
crystalline
nanostructures,
composition,
and
surface
configurations.
However,
uncertainty
their
active
sites
lower
intrinsic
deficiencies
nanomaterial-initiated
catalysis
compared
natural
enzymes
promote
pursuing
alternatives
by
imitating
biological
centers.
Single-atom
nanozymes
(SAzymes)
maximize
atom
utilization
well-defined
structure,
providing
an
important
bridge
investigate
mechanism
relationship
between
structure
catalytic
activity.
They
risen
new
burgeoning
alternative
enzyme
from
vitro
bioanalytical
tool
vivo
therapy
flexible
atomic
engineering
structure.
Here,
focus
is
mainly
on
three
parts.
First,
detailed
overview
single-atom
catalyst
synthesis
strategies
including
bottom-up
top-down
approaches
given.
Then,
according
structural
feature
nanocatalysts,
influence
factors
such
central
metal
atom,
coordination
number,
heteroatom
doping,
metal-support
interaction
are
discussed
representative
applications
(including
antibacterial/antiviral
performance,
cancer
therapy,
biosensing)
highlighted.
In
end,
future
perspective
challenge
facing
demonstrated.
Advanced Materials,
Год журнала:
2023,
Номер
36(2)
Опубликована: Июль 13, 2023
Single-atom
catalysts
(SACs)
have
attracted
considerable
attention
in
heterogeneous
catalysis
because
of
their
well-defined
active
sites,
maximum
atomic
utilization
efficiency,
and
unique
unsaturated
coordinated
structures.
However,
effectiveness
is
limited
to
reactions
requiring
sites
containing
multiple
metal
atoms.
Furthermore,
the
loading
amounts
single-atom
must
be
restricted
prevent
aggregation,
which
can
adversely
affect
catalytic
performance
despite
high
activity
individual
The
introduction
nanoscale
particles
(NMPs)
into
SACs
(NMP-SACs)
has
proven
an
efficient
approach
for
improving
performance.
A
comprehensive
review
urgently
needed
systematically
introduce
synthesis,
characterization,
application
NMP-SACs
mechanisms
behind
superior
This
first
presents
classifies
different
through
NMPs
enhance
SACs.
It
then
summarizes
currently
reported
synthetic
strategies
state-of-the-art
characterization
techniques
NMP-SACs.
Moreover,
electro/thermo/photocatalysis,
reasons
are
discussed.
Finally,
challenges
perspectives
future
design
advanced
addressed.
Nanoscale,
Год журнала:
2023,
Номер
15(7), С. 3550 - 3559
Опубликована: Янв. 1, 2023
Efficient
and
low-cost
transition
metal
single-atom
catalysts
(TMSACs)
for
hydrogen
evolution
reaction
(HER)
have
been
recognized
as
research
hotspots
recently
with
advances
in
delivering
good
catalytic
activity
without
noble
metals.
However,
the
high-cost
complex
preparation
of
TMSACs
insufficient
stability
limited
their
practical
applications.
Herein,
a
simple
top-down
pyrolysis
approach
to
obtain
P-modified
Co
SACs
loaded
on
crosslinked
defect-rich
carbon
nanosheets
was
introduced
alkaline
evolution,
where
atoms
are
locally
confined
before
prevent
aggregation.
Thereby,
abundant
defects
unsaturated
coordination
formed
during
significantly
improved
monatomic
structure
reduced
barrier.
Furthermore,
synergy
between
cobalt
phosphorus
established
optimize
decomposition
process
water
molecules,
which
delivers
key
promoting
slow
kinetics
HER.
As
result,
SAC
exhibited
excellent
HER,
overpotentials
70
mV
192
at
current
densities
-10
mA
cm-2
-100
cm-2,
respectively.
Advanced Functional Materials,
Год журнала:
2024,
Номер
34(29)
Опубликована: Март 17, 2024
Abstract
The
oxygen
reduction
reaction
(ORR)
plays
a
fundamental
role
in
sustainable
energy
technologies.
However,
the
creation
of
non‐precious
metal
electrocatalysts
with
high
ORR
activity
and
durability
under
all
pH
conditions
is
great
significance
but
remains
challenging.
Herein,
aim
to
overcome
this
challenge
by
creating
Fe
single
atom
catalyst
on
2D
defect‐containing
nitrogen‐doped
carbon
support
(Fe
1
/DNC)
via
microenvironment
engineering
strategy.
Microkinetic
modeling
reveals
that
FeN
4
(OH)
moieties
are
real
active
sites
conditions.
Due
synergistic
promotion
effect
denser
accessible
defect‐induced
electronic
properties,
/DNC
achieves
extraordinary
alkaline,
acidic,
neutral
conditions,
half‐wave
potentials
0.95,
0.82,
0.70
V,
respectively.
Moreover,
negligible
performance
decay
observed
stability
methanol
tolerance
tests.
Zn‐air
battery
employing
delivers
remarkable
peak
power
density
long‐term
operational
durability.
Theoretical
analysis
provides
compelling
evidence
defects
adjacent
can
endow
an
inductive
reshape
properties
balance
OOH*
formation
OH*
reduction.
This
work
offers
insight
into
regulation
asymmetric
coordination
structure
for
boosting
electrocatalytic
stability.
Abstract
Crystalline
perovskite
oxides
are
regarded
as
promising
electrocatalysts
for
water
electrolysis,
particularly
anodic
oxygen
evolution
reactions,
owing
to
their
low
cost
and
high
intrinsic
activity.
Perovskite
with
noncrystalline
or
amorphous
characteristics
also
exhibit
electrocatalytic
performance
toward
electrochemical
splitting.
In
this
review,
a
fundamental
understanding
of
the
advantages
crystalline,
noncrystalline,
is
presented.
Subsequently,
recent
progress
in
development
advanced
electrolysis
by
engineering
breaking
crystallinity
reviewed,
special
focus
on
underlying
structure–activity
relationships.
Finally,
remaining
challenges
unsolved
issues
presented,
an
outlook
briefly
proposed
future
exploration
next‐generation
water‐splitting
based
oxides.