Abstract
Single‐atom
catalysts
(SACs)
have
rapidly
become
a
hot
topic
in
photocatalytic
research
due
to
their
unique
physical
and
chemical
properties,
high
activity,
selectivity.
Among
many
semiconductor
carriers,
the
special
structure
of
carbon
nitride
(C
3
N
4
)
perfectly
meets
substrate
requirements
for
stabilizing
SACs;
they
can
also
compensate
defects
C
materials
by
modifying
energy
bands
electronic
structures.
Therefore,
developing
advanced
‐based
SACs
is
great
significance.
In
this
review,
we
focus
on
elucidating
efficient
preparation
strategies
burgeoning
applications
SACs.
We
outline
prospective
enhancing
performance
future.
A
comprehensive
array
methodologies
presented
identifying
characterizing
This
includes
an
exploration
potential
atomic
catalytic
mechanisms
through
simulation
regulation
behaviors
synergistic
effects
single
or
multiple
sites.
Subsequently,
forward‐looking
perspective
adopted
contemplate
future
prospects
challenges
associated
with
encompasses
considerations,
such
as
loading,
regulatory
design,
integration
machine
learning
techniques.
It
anticipated
that
review
will
stimulate
novel
insights
into
synthesis
high‐load
durable
SACs,
thereby
providing
theoretical
groundwork
scalable
controllable
field.
Advanced Functional Materials,
Год журнала:
2023,
Номер
33(44)
Опубликована: Июль 4, 2023
Abstract
Co
3
O
4
spinel
is
a
promising
transition
metal
oxide
(TMO)
catalyst
for
the
catalytic
ozonation
of
volatile
organic
compounds
(VOCs).
Herein,
metal–organic
frameworks
(MOFs)‐derived
Ni‐
and
Mg‐
substituted
catalysts
retain
similar
structures,
but
display
improved
reduced
performance
methyl
mercaptan
(CH
SH),
respectively.
Remarkably,
NiCo
2
can
still
≈90%
removal
CH
SH
after
running
20
h
at
room
temperature
under
an
initial
concentration
50
ppm
40
,
relative
humidity
60%,
space
velocity
300
000
mL
−1
g
exceeding
reported
values.
Experimental
characterizations
have
unveiled
that
substitution
Ni
Mg
into
altered
surface
acidity,
oxygen
species
mobility,
2+
/Co
3+
ratio.
The
in
situ
Raman
spectra
reveal
dynamic
formation
Co(III)‐O
ad
*
via
transformation
atomic
(O
*)
peroxide
*).
Theoretical
calculations
verify
Ni‐substitution
increases
nonuniform
charges
Fermi
density,
leading
to
moderate
increase
d‐band
center
energy
levels,
thereby
promoting
specific
adsorption/activation
convert
*/O
•OH/
1
/•O
−
which
contributes
eliminate
prevent
poisoning.
concept
tuning
provide
valuable
insights
design
other
ozonation.
Environmental Science & Technology,
Год журнала:
2023,
Номер
57(35), С. 13205 - 13216
Опубликована: Июль 24, 2023
The
design
of
a
micro-/nanoreactor
is
great
significance
for
catalytic
ozonation,
which
can
achieve
effective
mass
transfer
and
expose
powerful
reaction
species.
Herein,
the
mesoporous
carbon
with
atomic
Fe-N4
sites
embedded
in
ordered
nanochannels
(Fe-N4/CMK-3)
was
synthesized
by
hard-template
method.
Fe-N4/CMK-3
be
employed
as
nanoreactors
preferred
electronic
geometric
microenvironments
internal
ozonation
CH3SH.
During
CH3SH
oxidation
process,
coefficient
confined
system
sufficient
O3
featured
level
at
least
1.87
×
10-5,
34.6
times
that
Fe-N4/C-Si
unconfined
system.
Detailed
experimental
studies
theoretical
calculations
demonstrated
anchored
nanoconfinement
effects
regulated
local
structure
catalyst
promoted
activation
molecules
to
produce
oxygen
species
(AOS)
reactive
(ROS),
eventually
achieving
efficient
into
CO2/SO42-.
Benefiting
from
high
diffusion
rate
augmentation
AOS/ROS,
exhibited
an
excellent
poisoning
tolerance,
along
durability.
This
contribution
provides
proof-of-concept
strategy
accelerating
sulfur-containing
volatile
organic
compounds
(VOCs)
combining
catalysis
catalysts
extended
purification
other
gaseous
pollutants.
ACS Catalysis,
Год журнала:
2022,
Номер
13(1), С. 692 - 705
Опубликована: Дек. 23, 2022
High-performance
and
robust
catalysts
act
as
core
drivers
for
catalytic
ozonation
to
eliminate
gaseous
sulfur-containing
volatile
organic
compounds
(VOCs).
Herein,
nitrogen-doped
carbon
nanotubes
embedded
with
Co
species
(Co@NCNT)
are
synthesized
by
thermolysis
of
a
ZIF-67/melamine
mixture.
The
carbon-confinement
effects
in
Co@NCNT
not
only
improve
the
stability
but
also
regulate
electronic
structure
Co─C
bonds,
consequently
synergistically
improving
performance.
experimental
results
indicate
that
catalyst
could
still
remove
∼86%
odorous
methyl
mercaptan
(CH3SH)
after
running
60
h
at
25
°C
under
an
initial
concentration
50
ppm
CH3SH
40
ozone,
relative
humidity
60%,
space
velocity
600,000
mL
h–1
g–1,
outdistancing
reported
values
comparable
reaction
conditions.
Detailed
characterization
theoretical
simulations
reveal
metal–support
interaction
bonds
significantly
adjusts
species,
thereby
promoting
ozone-specific
adsorption/activation
convert
surface
atomic
oxygen
(*Oad)
·OH/1O2/·O2–.
Also,
electrons
obtained
from
electron-poor
center
transferred
through
C─Co
bond
bridge
maintain
redox
cycle
≡Co0/2+
→
≡Co3+
realize
efficient
stable
removal
into
CO2/SO42–/H2O.
This
work
demonstrates
MOF-derived
materials
tunable
structures
achieve
efficiency
VOCs
via
electron
transfer
trade-offs
provide
potential
candidate
application
air
purification.
