Environmental Science & Technology,
Год журнала:
2019,
Номер
53(15), С. 8553 - 8562
Опубликована: Июль 15, 2019
Organic
aerosols
are
subjected
to
atmospheric
processes
driven
by
sunlight,
including
the
production
of
reactive
oxygen
species
(ROS)
capable
transforming
their
physicochemical
properties.
In
this
study,
secondary
organic
(SOA)
generated
from
aromatic
precursors
were
found
sensitize
singlet
(1O2),
an
arguably
underappreciated
ROS.
Specifically,
we
quantified
1O2,
OH
radical,
and
H2O2
quantum
yields
within
photoirradiated
solutions
laboratory-generated
SOA
toluene,
biphenyl,
naphthalene,
1,8-dimethylnaphthalene.
At
5
mgC
L-1
extracts,
average
steady-state
concentrations
1O2
radicals
in
irradiated
3
±
1
×
10-14
M
3.6
0.9
10-17
M,
respectively.
Furthermore,
ROS
ambient
PM10
extracts
comparable
those
SOA,
suggesting
a
similarity
both
types
samples.
Finally,
using
our
measured
concentrations,
predict
that
certain
compounds
aerosols,
such
as
amino
acids,
organo-nitrogen
compounds,
phenolic
have
shortened
lifetimes
more
than
factor
2
when
is
considered
additional
sink.
Overall,
findings
highlight
importance
source
its
potential
competitive
photooxidation
processes.
Chemical Reviews,
Год журнала:
2021,
Номер
121(7), С. 4100 - 4146
Опубликована: Март 8, 2021
Singlet
oxygen
(1O2)
is
a
reactive
species
produced
in
sunlit
waters
via
energy
transfer
from
the
triplet
states
of
natural
sensitizers.
There
has
been
an
increasing
interest
measuring
apparent
1O2
quantum
yields
(ΦΔ)
aquatic
and
atmospheric
organic
matter
samples,
driven
part
by
fact
that
this
parameter
can
be
used
for
environmental
fate
modeling
contaminants
to
advance
our
understanding
dissolved
photophysics.
However,
lack
reproducibility
across
research
groups
publications
remains
challenge
significantly
limits
usability
literature
data.
In
first
review,
we
critically
evaluate
experimental
techniques
have
determine
ΦΔ
values
matter,
identify
quantify
sources
errors
potentially
explain
large
variability
literature,
provide
general
recommendations
future
studies.
second
part,
qualitative
overview
known
trends
as
function
type,
isolation
extraction
procedures,
bulk
water
chemistry
parameters,
molecular
spectroscopic
features,
chemical
treatments,
wavelength,
season,
location.
This
review
supplemented
with
comprehensive
database
samples.
Environmental Science & Technology,
Год журнала:
2022,
Номер
56(14), С. 10149 - 10160
Опубликована: Июль 6, 2022
Microplastics
(MPs)
interact
frequently
with
dissolved
organic
matter
(DOM)
commonly
found
in
the
environment,
but
information
on
aging
behavior
of
MPs
under
participation
DOM
is
still
lacking.
Thus,
polystyrene
microplastic
(PSMP)
process
was
systematically
studied
by
electron
paramagnetic
resonance
spectroscopy,
high-performance
liquid
chromatography,
Fourier
transform
infrared
(FTIR)
and
two-dimensional
correlation
spectroscopy
analyses
dark
ultraviolet
(UV)
light
conditions.
to
promote
transfer
generate
reactive
oxygen
species
(ROS)
conditions
PSMPs,
while
generating
ROS
UV
more
susceptible
photoelectrons
accelerated
PSMPs.
However,
among
four
types,
fulvic
acid
(FA)
has
a
significant
promoting
effect
PSMPs
than
humic
acid,
which
can
be
attributed
stronger
conversion
ability
FA
semiquinone
radicals.
Density
functional
theory
calculations
are
used
describe
difference
different
structures
plastics
DOM.
This
study
provides
necessary
theoretical
basis
for
migration
groundwater
deep
surface
water.
Environmental Science & Technology,
Год журнала:
2019,
Номер
53(20), С. 11725 - 11734
Опубликована: Сен. 11, 2019
Dissolved
organic
matter
(DOM)
composition
influences
its
ability
to
form
photochemically
produced
reactive
intermediates
(PPRI).
While
relationships
have
been
established
between
bulk
DOM
properties
and
triplet
(3DOM)
singlet
oxygen
(1O2)
quantum
yields,
contradictory
evidence
exists
for
hydroxyl
radical
(•OH)
hydroxylating
species.
Furthermore,
little
is
known
about
these
at
the
molecular
level.
We
evaluated
photochemical
reactivity
of
water
samples
from
a
wastewater
treatment
plant
St.
Louis
River
in
Minnesota
Wisconsin,
U.S.A.
Bulk
characterization
using
ultraviolet-visible
spectroscopy
demonstrates
that
color
apparent
size
decrease
downstream,
while
analysis
Fourier-transform
ion
cyclotron
resonance
mass
spectrometry
reveals
saturation
chemodiversity
highest
near
Lake
Superior.
3DOM
yield
coefficients
1O2
yields
increase
downstream
correlate
strongly
with
saturated
formulas.
Similar
results
are
observed
carbon-normalized
photodegradation
rate
constants
atorvastatin,
carbamazepine,
venlafaxine,
which
react
primarily
1O2.
In
contrast,
•OH
lowest
less
saturated,
more
oxygenated
DOM,
suggesting
not
major
precursor.
Mixed
DEET,
reacts
multiple
PPRI.
Molecular-level
compositional
data
reveal
insights
into
differing
formation
pathways
individual
PPRI,
but
information
specific
contaminants
needed
predict
their
fate.
Environmental Science & Technology,
Год журнала:
2019,
Номер
53(5), С. 2482 - 2490
Опубликована: Фев. 13, 2019
Excited
triplet
states
of
chromophoric
dissolved
organic
matter
(3CDOM*)
are
highly
reactive
species
in
sunlit
surface
waters
and
play
a
critical
role
oxygen
(ROS)
formation
pollutant
attenuation.
In
the
present
study,
series
chemical
probes,
including
sorbic
acid,
alcohol,
amine,
trimethylphenol,
furfuryl
were
employed
to
quantitatively
determine
3CDOM*
1O2
various
matters.
Using
high
concentration
alcohol
as
high-energy
quencher,
can
be
first
distinguished
(>250
kJ
mol–1)
low-energy
(<250
mol–1).
The
terrestrial-origin
natural
(NOM)
was
found
mainly
consist
states,
while
predominant
autochthonous-origin
NOM
effluent/wastewater
(EfOM/WWOM).
quantum
yields
electron
transfer
yield
coefficients
(fTMP)
generated
from
remained
constant
all
tested
External
phenolic
compound
showed
quenching
effects
on
triplet-state
tended
have
higher
efficiency
for
aromatic
ketone
which
main
states.
comparison
with
NOM,
EfOM/WWOM
presented
lower
reaction
rate
constants
amines
these
differences
likely
due
dissimilar
electric
charge
conditions.
Understanding
photochemistry
CDOM
is
essential
providing
useful
insights
into
their
photochemical
aquatic
systems.
Environmental Science & Technology,
Год журнала:
2021,
Номер
55(23), С. 15810 - 15820
Опубликована: Ноя. 10, 2021
We
investigated
the
photoaging
of
polypropylene
(PP)
microplastics
(MPs)
in
lake
water.
The
results
showed
that
PP
MPs
was
significantly
inhibited
water
compared
with
ultrapure
after
12
d
ultraviolet
(UV)
irradiation,
and
humic
acid
fulvic
acid,
rather
than
carbonate
(CO32–),
nitrate
(NO3–),
or
chloride
(Cl–)
ions,
were
identified
as
primary
contributors
to
observed
inhibition.
Mechanisms
for
roles
(Suwannee
River
acid)
(Pony
Lake
reducing
rates
photodegradation
acted
both
reactive
oxygen
species
(ROS)
scavengers
(e.g.,
•OH)
(dominant
contribution)
optical
light
filters.
As
ROS
scavengers,
decreased
capacity
formation
•OH
O2•–
by
under
irradiation.
In
addition,
chromophores
competed
photons
through
light-shielding
effect,
thereby
causing
less
fragmentation
particles
changes
other
properties
(melting
temperature,
contact
angle,
surface
zeta
potential).
proposed
mechanisms
inhibition
will
aid
our
efforts
assess
duration
aging
alterations
MP
during
long-term
weathering
natural
waters.
Environmental Science & Technology,
Год журнала:
2022,
Номер
56(4), С. 2803 - 2815
Опубликована: Янв. 28, 2022
Here,
we
systematically
compared
the
photoactivity
and
photobleaching
behavior
between
dissolved
black
carbon
(DBC)
from
rice
straw
biochar
leached
organic
(LDOC)
compost
using
complementary
techniques.
The
Fourier
transform-ion
cyclotron
resonance
mass
spectrometry
(FT-ICR
MS)
analysis
showed
that
DBC
was
dominated
by
polycyclic
aromatic
(55.1%)
tannin-like
molecules
(24.1%),
while
LDOC
lignin-like
(58.9%)
(19.7%).
Under
simulated
sunlight
conditions,
had
much
higher
apparent
quantum
yields
for
3DOM*
1O2
but
lower
•OH
than
LDOC.
After
a
168
h
irradiation,
total
number
of
formulas
identified
FT-ICR
MS
decreased
40.1%
with
concurrent
increases
in
O/C
H/C
ratios
also
decreases
double
bond
equivalence
minus
oxygen
(DBE
–
O)
average
molecular
weight
gel
permeation
chromatography.
However,
despite
large
UVA254
DOC,
only
12.0%
nearly
unchanged
ratio,
DBE
O
values,
distribution,
benzenepolycarboxylic
condensation
(BACon)
index
regardless
percentage
condensed
(ConAC
%).
Compared
LDOC,
photolysis
less
oxidative
destructive
mainly
via
breakup
small
portion
highly
rings,
probably
accompanied
photodecarboxylation.
Environmental Science & Technology,
Год журнала:
2023,
Номер
57(16), С. 6703 - 6711
Опубликована: Апрель 11, 2023
Predicting
the
formation
of
photochemically
produced
reactive
intermediates
(PPRI)
during
irradiation
dissolved
organic
matter
(DOM)
has
remained
challenging
given
complex
nature
this
material
and
differences
in
PPRI
mechanisms.
We
investigate
role
DOM
composition
photoreactivity
using
48
samples
that
span
range
freshwater
systems
wastewater.
relate
quantum
yields
for
excited
triplet-state
(fTMP),
singlet
oxygen
(Φ1O2),
hydroxylating
species
(Φ•OH)
to
determined
spectroscopy,
Fourier-transform
ion
cyclotron
resonance
mass
spectrometry,
electron-donating
capacity
(EDC).
fTMP
Φ1O2
follow
similar
trends
are
correlated
with
bulk
properties
derived
from
UV–vis
spectra
EDC.
In
contrast,
no
individual
property
can
be
used
predict
Φ•OH.
At
molecular
level,
subset
is
positively
both
Φ•OH
EDC
distinct
formulas
related
Φ1O2,
demonstrating
•OH
1O2
formed
different
fractions.
Multiple
linear
regressions
each
parameters
multiple
techniques,
complementary
methods
ideal
characterizing
because
technique
only
a
DOM.