Recently,
photocatalysis
combined
peroxydisulfate
activation
under
visible
light
(PC-PDS/Vis)
was
developed
as
a
promising
technology
for
removing
antibiotics
in
water.
Herein,
Mn-FeOOH
nanoclusters
were
grown
in-situ
on
the
surface
of
graphitic
carbon
nitride
nanosheets
(CNNS)
using
wet
chemical
method,
which
served
catalyst
to
drive
(PDS)
activation.
Photovoltaic
property
characterizations
revealed
that
Mn-FeOOH/CNNS
demonstrated
superior
capture
ability
and
carrier
separation
efficiency.
Through
DFT
calculations,
it
determined
synergistic
effect
between
Mn
Fe
species
could
enhance
adsorption
PDS.
Thus,
acquired
high
removal
efficiency
99.7%
50
min
tetracycline
(TC)
constructed
PC-PDS/Vis
system.
In
addition,
exhibited
recycling
stability
with
low
iron
leaching,
attributed
interaction
clusters
species.
Lastly,
quenching
experiments
ESR
tests
unveiled
•O2-
played
significant
part
TC
removal,
while
•OH
SO4•-
acted
additional
parameters
contributing
overall
process.
These
discoveries
provide
fresh
outlook
PC-PDS
degradation,
offering
deeper
insights
advancement
sustainable
cutting-edge
wastewater
treatment
technologies.
Inorganic Chemistry,
Journal Year:
2024,
Volume and Issue:
63(44), P. 21260 - 21274
Published: Oct. 24, 2024
Atomically
dispersed
catalysts
anchored
on
nitrogen-rich
substrates
present
promising
application
potential
for
the
persulfate-based
advanced
oxidation
process.
Nevertheless,
efficient
activation
efficiency
and
a
clear
activated
mechanism
of
persulfate
remain
challenging
in
carbon
nitride-based
single-atom
(SACs).
To
these,
combined
with
regulation
strategy
metal–ligand
section
carrier's
architecture,
an
atomically
Co
catalyst
regular
hollow
tubular
nitride
(Co/TCN
SAC)
herein
was
devised
utilized
to
activate
permonosulfate.
As
result,
Co/TCN
SACs
show
excellent
catalytic
performance
degradation
common
antibiotics.
Combined
X-ray
absorption
fine
structure
theory
calculation,
it
is
confirmed
that
superficially
CoO3
sites
Co2N2O2–CoO3
unit
are
active
center
peroxymonosulfate
(PMS)
activation.
The
electrochemical
test
situ
electron
paramagnetic
resonance
results
demonstrate
radical
(SO4•–
•OH)
nonradical
(electron
transfer
process
1O2)
paths
contributing
superior
performance.
In
addition,
exhibits
high
reaction
structural
stability
considering
water
quality
parameters.
Finally,
continuous
device
operated
laboratory
scale,
which
exhibited
satisfactory
continuously
removing
electron-rich
antibiotics
such
as
tetracycline.
This
work
reveals
atomic-level
modulation
cobalt
atomic
their
structure–activity
relationship
Tetrabromobisphenol
A
(TBBPA)
tends
to
desorb
from
contaminated
soil
into
underground
water
in
alkaline
environments,
threatening
ecology
and
human
health.
The
peroxymonosulfate-based
advanced
oxidation
process
offers
a
solution
decompose
TBBPA,
but
its
performance
declines
under
high
pH
values.
To
tackle
the
problem,
series
of
oxygen
vacancy
(Vo)
enriched
Co
Ni
bimetallic
hydrotalcite
materials
were
developed
this
study
by
ion
exchange
activate
PMS
for
TBBPA
degradation
values
efficiently.
Experimental
results
indicated
that
Vo-rich
Ni2Co1-LDH-Vo
catalyst
significantly
boosted
kinetics
with
rate
constant
(kobs)
0.2423
min–1
at
11,
1O2
identified
as
dominant
reactive
species.
Characterization
correlation
analysis
jointly
suggested
Vo
effectively
enhanced
activation
selectivity
towards
promoting
redox
cycles
Co2+⇋Co3+
Ni2+⇋Ni3+
simultaneously
activating
dissolved
oxygen.
Density
functional
theory
(DFT)
calculations
revealed
appropriate
Ni/Co
ratio
(2)
lowered
formation
energy
vacancies,
which
favored
generation
Vo.
Besides,
adsorption
configurations
on
both
atoms
optimized
Vo,
facilitating
subsequent
generate
selectively.
Notably,
Fukui
index
excluded
central
carbon
cleavage
pathway,
proposing
novel
sequential
opening
ring
pathway.
This
strategy
designing
catalysts
efficiently
degrade
values,
provides
theoretical
backing
Vo-engineered
synergistic
systems
optimize
activation.
