Microstructures,
Journal Year:
2025,
Volume and Issue:
5(2)
Published: Feb. 25, 2025
Noble-metal
single-atom
catalysts
(SACs)
have
arisen
as
a
research
hotspot
in
heterogeneous
catalysis
resulting
from
superior
noble-metal-atom
utilization,
well-defined
catalytic
centers,
and
tunable
microenvironments.
Recently,
the
advent
rise
of
noble-metal
SACs
supported
by
layered
double
hydroxides
(LDHs)
injected
fresh
vitality
vigor
into
this
field.
LDHs
offer
distinct
advantages
support
SACs,
such
an
ordered
adjustable
crystal
structure,
two-dimensional
structure
possessing
large
specific
surface
area,
facile
synthesis
with
cost-effectiveness,
strong
co-catalytic
metal-support
interaction
between
single
atoms.
In
review,
we
classified
comprehensively
outlined
current
strategies
LDHs,
conducted
in-depth
analysis
mechanisms
underlying
each
strategy.
Subsequently,
considering
critical
role
microenvironment
affecting
their
catalytic-related
properties,
discussed
regulation
LDH-supported
SACs.
We
also
provide
introduction
to
characterization
techniques
for
singe-atom
sites
Furthermore,
diverse
applications
various
fields
roles
played
atoms
relevant
processes.
Finally,
delineated
challenges
future
directions
development
ACS ES&T Engineering,
Journal Year:
2022,
Volume and Issue:
2(10), P. 1776 - 1796
Published: Sept. 7, 2022
Single
atom
catalysts
(SACs)
have
emerged
as
a
promising
catalyst
material
architecture
for
energy,
chemical,
and
environmental
applications.
In
the
past
several
years,
SACs
been
increasingly
explored
persulfate-based
advanced
oxidation
processes
(AOPs)
due
to
their
superior
persulfate
activation
pollutant
degradation
performance
compared
benchmark
dissolved
ion
nanoparticle
catalysts.
However,
there
still
exist
uncertainties
on
mechanism
of
by
SACs,
which
involves
complex
interplay
sulfate
hydroxyl
radicals,
singlet
oxygen,
high-valent
metal
species,
and/or
mediated
electron
transfer.
Questions
also
remain
how
ions
molecularly
align
single
site,
are
converted
into
reactive
what
design
parameters
lead
higher
efficiency
degradation.
this
critical
review,
we
examine
SAC
materials
employed
AOPs
discuss
they
function
differently
counterparts.
We
further
our
discussion
current
limitations,
opportunities,
future
research
needs
in
(i)
filling
knowledge
gaps
mechanisms
persulfate-SAC
interactions;
(ii)
augmenting
fundamental
with
theoretical
simulation
situ
characterization
techniques;
(iii)
improving
tailored
applications;
(iv)
proactively
considering
challenges
associated
engineering
practices
water
matrixes.
Angewandte Chemie International Edition,
Journal Year:
2023,
Volume and Issue:
62(43)
Published: Sept. 5, 2023
Singlet
oxygen
(1
O2
)
is
an
excellent
reactive
species
(ROSs)
for
the
selective
conversion
of
organic
matter,
especially
in
advanced
oxidation
processes
(AOPs).
However,
due
to
huge
dilemma
synthesizing
single-site
type
catalysts,
control
and
regulation
1
generation
AOPs
still
challenging
underlying
mechanism
remains
largely
obscure.
Here,
taking
advantage
well-defined
flexibly
tunable
sites
covalent
frameworks
(COFs),
we
report
first
achievement
precisely
regulating
ROSs
peroxymonosulfate
(PMS)-based
by
site
engineering
COFs.
Remarkably,
COFs
with
bipyridine
units
(BPY-COFs)
facilitate
PMS
activation
via
a
nonradical
pathway
100
%
,
whereas
biphenyl-based
(BPD-COFs)
almost
identical
structures
activate
produce
radicals
(⋅OH
SO4.-
).
The
BPY-COFs/PMS
system
delivers
boosted
performance
degradation
target
pollutants
from
water,
which
ca.
9.4
times
that
its
BPD-COFs
counterpart,
surpassing
most
reported
PMS-based
systems.
Mechanism
analysis
indicated
highly
electronegative
pyridine-N
atoms
on
BPY-COFs
provide
extra
adsorb
terminal
H
PMS,
resulting
simultaneous
adsorption
O
one
pyridine
ring,
facilitates
cleavage
S-O
bond
generate
.
Advanced Materials,
Journal Year:
2024,
Volume and Issue:
36(38)
Published: July 23, 2024
Abstract
Atomically
dispersed
active
sites
in
a
photocatalyst
offer
unique
advantages
such
as
locally
tuned
electronic
structures,
quantum
size
effects,
and
maximum
utilization
of
atomic
species.
Among
these,
asymmetric
dual‐sites
are
particular
interest
because
their
charge
distribution
generates
local
built‐in
electric
potential
to
enhance
separation
transfer.
Moreover,
the
dual
provide
flexibility
for
tuning
complex
multielectron
multireaction
pathways,
CO
2
reduction
reactions.
The
coordination
opens
new
possibilities
engineering
structure–activity–selectivity
relationship.
This
comprehensive
overview
discusses
efficient
sustainable
photocatalysis
processes
photocatalytic
reduction,
focusing
on
strategic
active‐site
design
future
challenges.
It
serves
timely
reference
development
conversion
processes,
specifically
exploring
here
exemplified
by
into
valuable
chemicals.
Eco-Environment & Health,
Journal Year:
2023,
Volume and Issue:
2(2), P. 47 - 60
Published: April 26, 2023
Single-atom
catalysts
(SACs)
have
been
widely
recognized
as
state-of-the-art
in
environment
remediation
because
of
their
exceptional
performance,
100%
metal
atomic
utilization,
almost
no
secondary
pollution,
and
robust
structures.
Most
recently,
the
activation
persulfate
with
carbon-based
SACs
advanced
oxidation
processes
(AOPs)
raises
tremendous
interest
degradation
emerging
contaminants
wastewater,
owning
to
its
efficient
versatile
reactive
oxidant
species
(ROS)
generation.
However,
comprehensive
critical
review
unraveling
underlying
relationship
between
structures
corresponding
generated
ROS
is
still
rare.
Herein,
we
systematically
summarize
fundamental
understandings
intrinsic
mechanisms
single
atom
active
sites
produced
during
AOPs.
The
types
are
firstly
elaborated,
presenting
prior
pollutants
that
need
be
degraded.
Then,
preparation
characterization
methods
overviewed.
material
structure–ROS
type
persulfate-based
AOPs
discussed
depth
expound
catalytic
mechanisms.
Finally,
briefly
conclude
current
development
propose
prospects
for
rational
design
synthesis
on-demand
performances
future
research.
