ACS ES&T Engineering,
Год журнала:
2023,
Номер
3(11), С. 1975 - 1985
Опубликована: Окт. 17, 2023
Molybdenum
disulfide
(MoS2)
is
a
prevalent
cocatalyst
for
peroxymonosulfate
(PMS)
activation
with
iron-based
materials.
The
contribution
of
molybdenum
atoms
in
MoS2
to
iron
regeneration
during
PMS
has
been
broadly
known,
though
the
role
sulfur
remains
explored.
Here,
we
applied
one-step,
facile
means
prepare
particulate
Fe3O4
supported
by
wrinkled
discernible
vacancies
(SV),
forming
flower-like
Fe3O4–MoS2
composite
catalyst.
We
demonstrated,
first
time,
strong
affinity
SV
PMS,
facilitating
formation
an
intermediate
FeIII–PMS*
while
modulating
generation
pivotal
nonradical
species.
Using
extensive
characterization,
confirmed
simultaneous
high-valent
iron-oxo
species
(≡FeIV═O)
and
singlet
oxygen
(1O2)
catalysts.
In
addition,
proposed
that
≡FeIV═O
stemmed
from
precursor,
which
underwent
heterolytic
cleavage
O–O
bonds
concomitant
rearrangement
atoms.
Meanwhile,
1O2
excited
formed
active
(O*)
liberated
oxides.
Consequently,
catalysts
showed
impressive
performance
removing
typical
micropollutants
real
water
sources,
such
as
secondary
effluent
wastewater
treatment
plants,
tap
water,
surface
stream.
Our
study
provides
new
insights
into
pathway
Sv-containing
MoS2,
clearing
way
developing
high-performance
decontamination.
Fully
understanding
the
periodate
(PI)
activation
system
is
still
a
great
challenge,
which
calls
for
efficient
heterogeneous
catalysts
with
sophisticated
structure.
Herein,
we
developed
"MOF-on-MXene"
heterostructures.
By
constructing
S-scheme
heterostructures
MXene/Z67450,
internal
electric
field
generated
via
Ti-O-Co
bonds
at
interface,
favoring
excitation
of
photogenerated
electrons,
providing
driving
force
accelerating
charge
transfer,
and
enhancing
redox
performances.
Further
contributed
by
synergy
Co-N4
bonds,
MXene/Z67450
composites
exhibit
enhanced
ability
activating
to
degrade
organic
pollutants
building
donor-catalyst-acceptor
system.
In
presence
light,
degraded
∼100%
tetracycline
hydrochloride
(TCH)
in
only
10
min.
The
active
sites
can
react
give
intermediate
MXene/Z67450-PI
(*PI).
As
result,
it
efficiently
reduced
PI
adsorption
energy
promoted
decomposition
formation
holes/electrons,
singlet
oxygen
(1O2)
as
well
hydroxyl
radical
(•OH).
addition,
high
stability,
reusability,
selectivity,
environmental
robustness.
Our
study
provides
research
direction
rationally
designing
MXene-based
heterojunctions
applying
them
