Environmental Science & Technology,
Journal Year:
2023,
Volume and Issue:
57(48), P. 20206 - 20218
Published: Nov. 15, 2023
In
the
realm
of
wastewater
treatment,
power
ferrate
(Fe(VI))
and
peracetic
acid
(PAA)
as
oxidants
stands
out.
But
their
combined
might
is
where
enhancement
truly
lies.
Their
collaborative
effect
intensifies,
but
underlying
mechanics,
especially
across
varying
pH
levels
pollutant
types,
still
lurks
in
obscurity.
Our
study
delved
into
sophisticated
oxidation
interplay
among
Fe(VI)-PAA,
Fe(VI)-H2O2,
standalone
Fe(VI)
systems.
Notably,
at
a
9.0,
boasting
kinetic
constant
∼0.127
M-1·s-1,
Fe(VI)-PAA
system
annihilated
sulfamethoxazole,
outpacing
its
counterparts
by
staggering
48.73-fold
when
compared
to
Fe(VI)-H2O2
105.58-fold
using
individually.
The
behavior
active
species─such
dynamic
•OH
radicals
high-valent
iron
species
(Fe(IV)/Fe(V))─shifted
with
variations,
leading
distinct
degradation
pathways.
detailed
exploration
pinpoints
behaviors
certain
from
3.0
9.0.
more
acidic
environments,
proved
indispensable
for
system's
reactivity.
Conversely,
inclined,
was
increasingly
steered
species.
This
intensive
probe
demystifies
interactions,
deepening
our
understanding
capabilities
Fe(VI)-centered
guiding
us
toward
cleaner
water
solutions.
Importantly,
value,
often
underappreciated,
holds
reins
organic
decontamination.
Embracing
this
key
player
vital
we
strategize
expansive
systems
upcoming
ventures.
Environmental Science & Technology,
Journal Year:
2021,
Volume and Issue:
55(22), P. 15400 - 15411
Published: Nov. 5, 2021
Ubiquitous
oxygen
vacancies
(Vo)
existing
in
metallic
compounds
can
activate
peroxymonosulfate
(PMS)
for
water
treatment.
However,
under
environmental
conditions,
especially
oxygenated
surroundings,
the
interactions
between
Vo
and
PMS
as
well
organics
degradation
mechanism
are
still
ambiguous.
In
this
study,
we
provide
a
novel
insight
into
activation
over
Vo-containing
Fe–Co
layered
double
hydroxide
(LDH).
Experimental
results
show
that
Vo/PMS
is
capable
of
selective
via
single-electron-transfer
nonradical
pathway.
Moreover,
O2
firstly
demonstrated
most
critical
trigger
system.
Mechanistic
studies
reveal
that,
with
abundant
electrons
confined
vacant
electron
orbitals
Vo,
thermodynamically
enabled
to
capture
from
form
O2•–
imprinting
effect
start
process.
Simultaneously,
becomes
electron-deficient
withdraws
sustain
electrostatic
balance
achieve
(32%
Bisphenol
A
without
PMS).
Different
conventional
activation,
collaboration
kinetics
thermodynamics,
endowed
ability
donate
reductant
other
than
an
oxidant
1O2.
case,
1O2
act
indispensable
intermediate
species
accelerate
circulation
(as
high
14.3
mg/L)
micro
area
around
promote
nano-confinement
electron-recycling
process
67%
improvement
degradation.
This
study
provides
brand-new
perspective
natural
environments.
ACS Catalysis,
Journal Year:
2021,
Volume and Issue:
11(17), P. 11129 - 11159
Published: Aug. 23, 2021
Advanced
oxidation
processes
(AOPs)
based
on
persulfates
such
as
peroxymonosulfate
and
peroxydisulfate
via
heterogeneous
catalysts
have
been
a
research
hotspot
due
to
their
outstanding
performances
in
removing
emerging
organic
contaminants
(OCs).
In
this
Review,
we
highlight
the
recent
advances
theoretical
simulations
for
persulfate-based
AOPs
(PS-AOPs)
using
density
functional
theory
(DFT),
with
emphasis
catalyst
properties
mechanism
of
persulfate
activation
over
variety
(including
nanocarbons,
metals,
metal
oxides).
Moreover,
OCs
degradation
by
diverse
reactive
oxygen
species
investigated
computations
are
also
summarized.
The
descriptors
computational
studies
related
structure–performance
relationships
discussed.
Finally,
challenges
future
focuses
DFT
PS-AOPs
proposed,
including
evaluation
properties,
elucidation
mechanism,
especially
nonradical
pathway,
rational
design
on-demand
catalysts.
