Poly-
and
per-fluoroalkyl
substances
(PFAS)
are
synthetic
chemicals
with
global
health
concerns
due
to
their
stability
environmental
persistence.
Pristine
boron
nitride
(h-BN)
has
been
reported
as
an
efficient
photocatalyst
for
PFAS
degradation.
We
have
assessed
the
electrochemical
properties
of
h-BN
electrochemically
degrade
perfluorooctanoic
acid
(PFOA).
electrocatalytically
oxidizes
100
mg/L
PFOA
shorter
chains
a
70%
removal
efficiency
in
3
h
at
pH
4.5.
Modifying
surface
UiO-66
enhances
degradation
by
facilitating
proximal
adsorption
catalytic
sites,
93%
49%
defluorination.
Computational
results
show
that
∆G
oxidation
is
151
kcal/mol
(E0
≈
1.89
V),
agreement
experiments.
electrocatalyst
degradation,
decoration
its
activity
through
trap-n-zap
strategy.
The
electrical
energy
per
order
(EE/O)
UiO-66@BN
6.1
Kwh/m3
indicating
promising
potential
remediation
applications.
Environmental Science & Technology,
Год журнала:
2024,
Номер
58(18), С. 8065 - 8075
Опубликована: Апрель 10, 2024
We
report
a
previously
unrecognized
but
efficient
reductive
degradation
pathway
in
peroxydisulfate
(PDS)-driven
soil
remediation.
With
supplements
of
naturally
occurring
low-molecular-weight
organic
acids
(LMWOAs)
anaerobic
biochar-activated
PDS
systems,
rates
12
γ-hexachlorocyclohexanes
(HCH)-spiked
soils
boosted
from
40%
without
LMWOAs
to
maximum
99%
with
1
mM
malic
acid.
Structural
analysis
revealed
that
an
increase
α-hydroxyl
groups
and
diminution
pKa1
values
facilitated
the
formation
carboxyl
anion
radicals
(COO•–)
via
electrophilic
attack
by
SO4•–/•OH.
Furthermore,
kinetics
were
strongly
correlated
matter
(SOM)
contents
than
iron
minerals.
Combining
newly
developed
situ
fluorescence
detector
quenching
experiments,
we
showed
for
high,
medium,
low
SOM
contents,
dominant
reactive
species
switched
singlet
oxygen/semiquinone
SO4•–/•OH
then
COO•–
(contribution
increased
30.8
66.7%),
yielding
superior
HCH
degradation.
Validation
experiments
using
model
compounds
highlighted
critical
roles
redox-active
moieties,
such
as
phenolic
–
OH
quinones,
radical
conversion.
Our
study
provides
insights
into
environmental
behaviors
related
activation
persulfate
broader
horizon
inspiration
more
advanced
reduction
technologies.
Journal of the American Chemical Society,
Год журнала:
2024,
Номер
unknown
Опубликована: Сен. 11, 2024
We
have
discovered
a
strategy
to
synthesize
reactive
radical
salts,
effectively
bottling
up
radicals
in
space
and
time
for
future
use.
apply
this
new
principle
electrochemiluminescence
(ECL)
through
the
simultaneous
electro-reduction
of
peroxydisulfate,
S
Environmental Science & Technology,
Год журнала:
2024,
Номер
58(14), С. 6415 - 6424
Опубликована: Март 26, 2024
The
total
oxidizable
precursor
(TOP)
assay
has
been
extensively
used
for
detecting
PFAS
pollutants
that
do
not
have
analytical
standards.
It
uses
hydroxyl
radicals
(HO•)
from
the
heat
activation
of
persulfate
under
alkaline
pH
to
convert
H-containing
precursors
perfluoroalkyl
carboxylates
(PFCAs)
target
analysis.
However,
current
TOP
oxidation
method
does
apply
emerging
because
(i)
many
structures
contain
C–H
bonds
HO•
attack
and
(ii)
transformation
products
are
necessarily
PFCAs.
In
this
study,
we
explored
use
classic
acidic
digestion,
which
generates
sulfate
(SO4–•),
extend
capability
assay.
We
examined
Nafion-related
ether
sulfonates
or
−COO–,
characterized
products,
quantified
F
atom
balance.
SO4–•
greatly
expanded
scope
precursors.
was
initiated
by
decarboxylation,
followed
various
spontaneous
steps,
such
as
HF
elimination
ester
hydrolysis.
further
compared
legacy
fluorotelomers
using
versus
HO•.
results
suggest
novel
product
distribution
patterns,
depending
on
functional
group
oxidant
dose.
general
trends
strategies
were
also
validated
analyzing
a
mixture
100000-
10000-fold
diluted
aqueous
film-forming
foam
(containing
fluorotelomer
surfactants
organics)
spiked
Nafion
precursor.
Therefore,
(1)
combined
oxidation,
(2)
list
standard
chemicals,
(3)
elucidation
mechanisms
will
provide
more
critical
information
probe
pollutants.
Environmental Science & Technology,
Год журнала:
2025,
Номер
unknown
Опубликована: Апрель 17, 2025
The
UV/sulfite
advanced
reduction
process
(ARP)
holds
promise
for
the
removal
of
per-
and
polyfluoroalkyl
substances
(PFASs)
by
a
hydrated
electron
(eaq-)-induced
H/F
exchange
under
anoxic
conditions.
Traditionally,
presence
coexisting
nitrate
in
water
has
always
been
regarded
as
major
inhibitory
factor
PFASs
defluorination.
However,
this
study
observed
an
unexpected
promotive
effect
on
defluorination,
challenging
previous
phenomenon.
Notably,
addition
100
μM
resulted
remarkable
54%
enhancement
PFOA
A
novel
mechanism
was
discovered
that
nitrate-derived
reactive
nitrogen
species
(RNS)
activated
decarboxylation-hydroxylation-elimination-hydrolysis
(DHEH)
process,
important
degradation
pathway
ARP.
Induced
eaq-,
PFAS
molecule
first
became
perfluorinated
radical
then
transformed
into
unstable
alcohol
reacting
with
water.
Due
to
high
reactivity
driven
unpaired
electrons
RNS,
molecules
were
destabilized
H-O
bond
stretched
from
0.98
1.04
Å.
This
effectively
enhanced
spontaneity
reaction
between
consequently
made
whole
DHEH
more
thermodynamic
favorable
(ΔG,
-23.53
→
-376.28
kJ/mol).
Such
breaks
through
view
directly
reacts
eaq-
affect
defluorination
ARP
systems.
finding
offers
innovative
perspective
optimizing
strategically
regulating
levels
bodies.
