Proceedings of the National Academy of Sciences,
Journal Year:
2023,
Volume and Issue:
120(26)
Published: June 20, 2023
Hydrogen
peroxide
(H
2
O
)
is
an
important
green
oxidant
in
the
field
of
sewage
treatment,
and
how
to
improve
its
activation
efficiency
generate
free
radicals
with
stronger
oxidation
performance
a
key
issue
current
research.
Herein,
we
synthesized
Cu-doped
α-Fe
3
catalyst
(7%
Cu–Fe
for
H
under
visible
light
degradation
organic
pollutants.
The
introduction
Cu
dopant
changed
d-band
center
Fe
closer
Fermi
level,
which
enhanced
adsorption
site
,
cleavage
pathway
from
heterolytic
homolytic
cleavage,
thereby
improving
selectivity
•OH
generation.
In
addition,
doping
also
promoted
absorption
ability
separation
hole–electron
pairs,
photocatalytic
activities.
Benefiting
high
•OH,
7%
exhibited
efficient
activities
against
ciprofloxacin,
rate
was
3.6
times
as
much
that
it
had
good
variety
Environmental Science & Technology,
Journal Year:
2023,
Volume and Issue:
57(47), P. 19012 - 19022
Published: Aug. 21, 2023
A
carbon-based
advanced
oxidation
process
is
featured
for
the
nonradical
electron-transfer
pathway
(ETP)
from
electron-donating
organic
compounds
to
activated
persulfate
complexes,
enabling
it
as
a
green
technology
selective
of
pollutants
in
complex
water
environments.
However,
thermodynamic
and
kinetic
behaviors
regime
had
been
ambiguous
due
neglect
influence
pH
on
mechanisms.
In
this
study,
three
kinds
were
divided
ETP
regime:
(i)
physio-adsorption,
(ii)
adsorption-dominated
(oxidation
rate
slightly
surpasses
adsorption
rate),
(iii)
oxidation-dominated
outpaces
rate).
The
differential
attributed
physicochemical
properties
pollutants.
For
example,
hydrophobicity,
molecular
radius,
positive
electrostatic
potential
controlled
mass-transfer
stage
reactants
(peroxydisulfate
(PDS)
organics).
Meanwhile,
other
descriptors,
including
Fukui
index,
potential,
electron
cloud
density
regulated
processes
thus
kinetics
oxidation.
Most
importantly,
pathways
these
could
be
altered
by
adjusting
chemistry.
This
study
reveals
principles
developing
efficient
systems
selectively
remove
recycle
wastewater.
Environmental Science & Technology,
Journal Year:
2024,
Volume and Issue:
58(11), P. 4844 - 4851
Published: Feb. 22, 2024
This
perspective
presents
the
latest
advancements
in
selective
polymerization
pathways
advanced
oxidation
processes
(AOPs)
for
removal
of
featured
organic
pollutants
wastewater.
In
radical-based
homogeneous
reactions,
SO4•
–-based
systems
exhibit
superior
oxidative
activity
toward
aromatics
with
electron-donating
substituents
via
single
electron
transfer
and
radical
adduct
formation
(RAF).
The
produced
cations
subsequently
undergo
coupling
reactions
to
produce
polymers.
For
•OH-based
oxidation,
metal
ions
facilitate
production
monomer
radicals
RAF.
Additionally,
heterogeneous
catalysts
can
mediate
both
persulfate
activation
without
generating
inorganic
radicals.
Metal-based
will
a
direct
pathway
polymerization.
contrast,
carbon-based
induce
low-molecular-weight
oligomers
(≤4
units)
an
process.
comparison
mineralization,
remarkably
reduce
peroxide
usage,
quickly
separate
from
aqueous
phase,
generate
polymeric
byproducts.
Thus,
AOP-driven
hold
significant
promise
reducing
carbon
emission
realizing
recycling
water
treatment
processes.
Environmental Science and Ecotechnology,
Journal Year:
2024,
Volume and Issue:
20, P. 100405 - 100405
Published: Feb. 28, 2024
The
ubiquity
of
refractory
organic
matter
in
aquatic
environments
necessitates
innovative
removal
strategies.
Sulfate
radical-based
advanced
oxidation
has
emerged
as
an
attractive
solution,
offering
high
selectivity,
enduring
efficacy,
and
anti-interference
ability.
Among
many
technologies,
sulfite
activation,
leveraging
its
cost-effectiveness
lower
toxicity
compared
to
conventional
persulfates,
stands
out.
Yet,
the
activation
process
often
relies
on
transition
metals,
suffering
from
low
atom
utilization.
Here
we
introduce
a
series
single-atom
catalysts
(SACs)
employing
metals
g-C3N4
substrates,
effectively
activating
for
acetaminophen
degradation.
We
highlight
superior
performance
Fe/CN,
which
demonstrates
degradation
rate
constant
significantly
surpassing
those
Ni/CN
Cu/CN.
Our
investigation
into
electronic
spin
polarization
characteristics
these
reveals
their
critical
role
catalytic
efficiency,
with
oxysulfur
radical-mediated
reactions
predominating.
Notably,
under
visible
light,
activity
is
enhanced,
attributed
increased
generation
radicals
strengthened
electron
donation-back
donation
dynamic.
proximity
Fe/CN's
d-band
center
Fermi
level,
alongside
polarization,
shown
improve
adsorption
reduce
HOMO-LUMO
gap,
thereby
accelerating
photo-assisted
activation.
This
work
advances
understanding
SACs
environmental
applications
lays
groundwork
future
water
treatment
technologies.
