Environmental Science & Technology,
Journal Year:
2022,
Volume and Issue:
56(12), P. 7924 - 7934
Published: May 19, 2022
Oxygen
vacancies
play
a
vital
role
in
the
catalytic
activity
of
layered
double
hydroxide
(LDH)
catalysts
wastewater
treatment.
However,
mechanism
oxygen
vacancy-mediated
LDH-activated
to
produce
reactive
species
(ROS)
still
lacks
reasonable
explanation.
In
this
work,
tartrate-modified
CuCoFe-LDH
(CuCoFe/Tar-LDH)
with
abundant
was
designed,
which
can
efficiently
degrade
nitrobenzene
(NB)
under
room
conditions.
The
technical
energy
consumption
is
0.011
kW
h
L–1.
According
characterization
and
calculation
results,
it
proposed
that
are
formed
because
deficiency
caused
by
reduction
between
metal
ion
oxygen,
transitions
lower
state.
Compared
CuCoFe-LDH,
vacancy
formation
CuCoFe/Tar-LDH
decreased
from
1.98
1.13
eV.
O2
bond
length
adsorbed
on
1.27
Å,
close
theoretical
superoxide
radicals
(•O2–)
(1.26
Å).
Radical
trapping
experiments
electron
spin-resonance
spectroscopy
spectrum
prove
•O2–
an
important
precursor
•OH.
This
work
dedicated
in-depth
exploration
catalyst
activation
for
molecular
conversion
relationship
ROS.
Advanced Functional Materials,
Journal Year:
2023,
Volume and Issue:
33(12)
Published: Jan. 6, 2023
Abstract
Composites‐based
photocatalysis
relies
on
the
interfacial
electron
transfer
between
metallic
cocatalyst
and
photosensitizer
(the
semiconductor)
to
realize
spatial
separation
of
charge
carriers.
Herein,
an
ingenious
heterojunction
Co‐CN
single
atom
catalysts
(SACs)
g‐C
3
N
4
is
constructed
for
heterogeneous
photo‐Fenton‐like
reactions.
Driven
by
built‐in
electric
field
across
heterojunctions,
migration
photogenerated
carriers
promoted,
leading
fast
from
SACs.
Theoretical
calculations
transient
absorption
spectroscopy
reveal
modulated
trapping
in
SA‐Co‐CN/g‐C
heterostructure,
resulting
remarkably
enhanced
generation
reactive
oxygen
species
via
peroxymonosulfate
activation
under
light
irradiation.
This
/PMS/vis
system
efficient
oxidation
various
antibiotics
with
high
removal
efficiency
(>98%),
a
wide
operating
pH
range
(pH
3–11)
excellent
stability
long‐term
operation.
study
provides
new
tactic
rational
design
SACs‐based
heterojunctions
bridge
catalysis,
attaining
superior
photoredox
activity
coupling.
Environmental Science & Technology,
Journal Year:
2022,
Volume and Issue:
56(12), P. 8765 - 8775
Published: May 12, 2022
As
an
efficient
active
oxidant
for
the
selective
degradation
of
pollutants
in
wastewater,
high-valent
copper
species
Cu(III)
with
persulfate
activation
has
attracted
substantial
attention
some
Cu-based
catalysts.
However,
systematic
study
a
catalyst
structure
and
mechanism
about
peroxydisulfate
(PDS)
is
challenging
owing
to
coexistence
multiple
Cu
structural
symmetry
PDS.
Herein,
we
anchored
atom
two
pyridinic
N
atoms
synthesize
single-atom
(CuSA-NC).
Experimental
characterizations
theoretical
calculations
complemented
each
other
well
because
uniform
atomic
sites.
The
was
identified
as
site,
unsaturated
Cu-N2
configuration
more
conductive
PDS
than
saturated
Cu-N4
configuration.
Benefiting
from
generation
Cu(III),
CuSA-NC
exhibited
obvious
anti-interference
performance
pollutant
complex
matrix.
superior
catalytic
activity
compared
that
reported
catalysts
good
durability
continuous-flow
experiment
further
revealed
potential
practical
applications.
This
work
strongly
deepens
understanding
sites
under
develops
approach
actual
water
purification.
Environmental Science & Technology,
Journal Year:
2022,
Volume and Issue:
56(4), P. 2637 - 2646
Published: Jan. 28, 2022
The
redox
behavior
of
metal
active
sites
determines
the
rate
heterogeneous
catalysis
in
peroxymonosulfate
activation.
Previous
reports
focused
on
construction
catalysts
for
accelerating
interfacial
electron
transfer.
In
this
work,
a
new
strategy
was
proposed
facilitating
valence
cycles
Cu+/Cu2+
by
using
pollutants.
2.5Cu/CeO2/PMS
system
capable
achieving
efficient
removal
pollutants,
including
tetracycline,
oxytetracycline,
and
rhodamine
B,
wide
pH
working
range.
presence
Cu-N
bond
formed
between
-NH2
group
tetracycline
Cu
site
catalyst,
showing
that
coordination
changed
to
CuO4N1.
charge
CuO4N1
rearranged,
making
it
easier
obtain
electrons
promote
PMS
oxidation,
thereby
reduction
Cu2+
Cu+
activation
showed
excellent
sustainability
selectivity
organic
This
study
provides
novel
routine
utilizing
pollutants
accelerate
species.