Advanced Functional Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Окт. 1, 2024
Abstract
Many
existing
research
focuses
on
the
differences
or
performance
comparisons
between
single‐atom
small‐sized
nanocluster
catalysts,
but
there
is
a
lack
of
comprehensive
coupling
relationship
structure
and
activity
mechanism
synergy.
This
study
investigates
combined
catalytic
potential
cobalt
single
atoms
(SAs)
nanoclusters
(NCs)
for
enhanced
peroxymonosulfate
(PMS)
activation
to
degrade
norfloxacin
(NFX).
A
novel
Co
SAs‐NCs
/CN/TiO
2
catalyst
synthesized,
featuring
SAs
NCs
uniformly
dispersed
carbon
film
wrapping
TiO
,
degradation
efficiency
NFX
solution
almost
completely
degraded,
with
mineralization
rate
76.35%.
Density
functional
theory
(DFT)
calculations
indicate
that
synergistic
interaction
promotes
more
efficient
PMS
adsorption
significantly
reduces
energy
barrier,
which
enhances
electron
transfer
increases
reactive
oxygen
species
(ROS)
generation.
highlights
robust
versatile
nature
this
system
in
addressing
various
contaminants.
elucidates
providing
new
ideas
advanced
oxidation
processes
(AOPs)
environmental
remediation,
linking
emphasizes
practicality
importance
effectively
long‐term
remediation
water
pollutants.
Environmental Science & Technology,
Год журнала:
2023,
Номер
57(33), С. 12153 - 12179
Опубликована: Авг. 3, 2023
Urbanization
and
industrialization
have
exerted
significant
adverse
effects
on
water
quality,
resulting
in
a
growing
need
for
reliable
eco-friendly
treatment
technologies.
Persulfate
(PS)-based
advanced
oxidation
processes
(AOPs)
are
emerging
as
viable
technologies
to
treat
challenging
industrial
wastewaters
or
remediate
groundwater
impacted
by
hazardous
wastes.
While
the
generated
reactive
species
can
degrade
variety
of
priority
organic
contaminants
through
radical
nonradical
pathways,
there
is
lack
systematic
in-depth
comparison
these
pathways
practical
implementation
different
scenarios.
Our
comparative
analysis
reaction
rate
constants
vs.
indicates
that
radical-based
AOPs
may
achieve
high
removal
efficiency
with
relatively
short
contact
time.
Nonradical
feature
advantages
minimal
matrix
interference
complex
wastewater
treatments.
(e.g.,
singlet
oxygen,
high-valent
metals,
surface
activated
PS)
preferentially
react
bearing
electron-donating
groups,
allowing
enhancement
degradation
known
target
contaminants.
For
byproduct
formation,
analytical
limitations
computational
chemistry
applications
also
considered.
Finally,
we
propose
holistically
estimated
electrical
energy
per
order
(EE/O)
parameter
show
significantly
higher
requirements
pathways.
Overall,
critical
comparisons
help
prioritize
basic
research
PS-based
inform
merits
system-specific
applications.
Proceedings of the National Academy of Sciences,
Год журнала:
2024,
Номер
121(4)
Опубликована: Янв. 17, 2024
Nonradicals
are
effective
in
selectively
degrading
electron-rich
organic
contaminants,
which
unfortunately
suffer
from
unsatisfactory
yield
and
uncontrollable
composition
due
to
the
competitive
generation
of
radicals.
Herein,
we
precisely
construct
a
local
microenvironment
carbon
nitride–supported
high-loading
(~9
wt.%)
Fe
single-atom
catalyst
(Fe
SAC)
with
sulfur
via
facile
supermolecular
self-assembly
strategy.
Short-distance
S
coordination
boosts
peroxymonosulfate
(PMS)
activation
generates
high-valent
iron–oxo
species
IV
=O)
along
singlet
oxygen
(
1
O
2
),
significantly
increasing
yield,
PMS
utilization,
p
-chlorophenol
reactivity
by
6.0,
3.0,
8.4
times,
respectively.
The
nonradicals
is
controllable
simply
changing
content.
In
contrast,
long-distance
both
radicals
nonradicals,
could
not
promote
reactivity.
Experimental
theoretical
analyses
suggest
that
short-distance
upshifts
d
-band
center
atom,
i.e.,
being
close
Fermi
level,
changes
binding
mode
between
atom
site
generate
=O
high
yield.
S-coordinated
SAC
exhibits
excellent
application
potential
various
water
matrices.
These
findings
can
guide
rational
design
robust
SACs
toward
selective
utilization.
Abstract
With
maximum
utilization
of
active
metal
sites,
more
and
researchers
have
reported
using
single
atom
catalysts
(SACs)
to
activate
persulfate
(PS)
for
organic
pollutants
removal.
In
SACs,
atoms
(Fe,
Co,
Cu,
Mn,
etc.)
different
substrates
(porous
carbon,
biochar,
graphene
oxide,
carbon
nitride,
MOF,
MoS
2
,
others)
are
the
basic
structural.
Metal
atoms,
substances,
connected
chemical
bonds
all
a
great
influence
on
electronic
structures
that
directly
affect
activation
process
PS
degradation
efficiency
pollutants.
However,
there
few
relevant
reviews
about
interaction
between
substances
during
process.
this
review,
SACs
with
species
summarized
investigate
metal−support
evaluate
their
effects
oxidation
reaction
Furthermore,
how
reactive
pathways
also
discussed.
Finally,
challenges
prospects
in
PS‐AOPs
proposed.
