Analytical Chemistry,
Journal Year:
2025,
Volume and Issue:
unknown
Published: May 6, 2025
Fourier
transform
ion
cyclotron
resonance
mass
spectrometry
(FT-ICR
MS)
has
become
a
cutting-edge
technique
for
molecular
characterization
of
dissolved
organic
matter
(DOM)
and
trace
contaminants.
Nevertheless,
FT-ICR
MS
is
rarely
applied
to
simultaneously
elucidate
DOM
chemodiversity
quantify
the
concentrations
Compared
conventional
solid-phase
extraction
(SPE),
pH-dependent
fractionation
molecules
using
sequential
SPE
strategy
significantly
enhanced
recovery
carbon
yielded
more
chemical
formulas
from
environmental
samples
(p
<
0.05).
The
at
circumneutral
pH
provided
exclusive
isolation
some
hydrogen-rich
oxygen-poor
molecules,
caused
5-fold
reduction
in
matrix
effects,
improved
detection
limits
structure
typical
wastewater
indicator,
sucralose,
was
successfully
validated
analysis
with
tandem
hydrogen/deuterium
exchange
measurements.
With
standard
addition
method,
quantitation
sucralose
extracts
isolated
were
estimated
be
0.26
0.87
μg/L,
respectively.
representative
urban
lake
measured
by
(e.g.,
0.9-4.1
μg/L)
comparable
those
determined
liquid
chromatography
coupled
an
Orbitrap
analyzer.
findings
this
study
expand
application
research
highlighting
its
potential
identifying
contaminants,
quantifying
their
concentrations,
elucidating
inform
contaminant
sources
aquatic
systems.
Water Research,
Journal Year:
2024,
Volume and Issue:
253, P. 121148 - 121148
Published: Jan. 16, 2024
This
publication
summarizes
my
journey
in
the
field
of
chemical
oxidation
processes
for
water
treatment
over
last
30+
years.
Initially,
efficiency
application
oxidants
micropollutant
abatement
was
assessed
by
target
compounds
only.
is
controlled
reaction
kinetics
and
therefore,
second-order
rate
constant
these
reactions
are
pre-requisite
to
assess
feasibility
such
processes.
Due
tremendous
efforts
this
area,
we
currently
have
a
good
experimental
data
base
constants
many
oxidants,
including
radicals.
Based
on
this,
predictions
can
be
made
without
with
Quantitative
Structure
Activity
Relationships
Hammet/Taft
or
energies
highest
occupied
molecular
orbitals
from
quantum
computations.
Chemical
has
economically
feasible
extent
transformation
micropollutants
often
limited
mineralization
cannot
achieved
under
realistic
conditions.
The
formation
products
oxidant
inherent
following
questions
evolved
years:
Are
formed
biologically
less
active
than
compounds?
Is
there
new
toxicity
associated
products?
more
biodegradable
corresponding
In
addition
positive
effects
quality
related
micropollutants,
react
mainly
matrix
components
as
dissolved
organic
matter
(DOM),
bromide
iodide.
As
fact,
fraction
consumed
DOM
typically
>
99%,
which
makes
inherently
inefficient.
consequences
loss
capacity
inorganic
disinfection
byproducts
also
involving
iodide,
oxidized
reactive
bromine
iodine
their
ensuing
DOM.
Overall,
it
turned
out
three
decades,
that
complex
understand
manage.
However,
research
led
understanding
underlying
allow
widespread
optimized
practice
drinking
water,
municipal
industrial
wastewater
reuse
systems.
Dissolved
organic
matter
(DOM)
is
the
primary
precursor
of
disinfection
products
(DBPs)
during
chlorination.
However,
compositional
characteristics
DOM
transformation
chlorination
process
in
different
source
waters
and
its
relationship
to
cytotoxicity
remain
understudied.
Here,
we
used
high-resolution
mass
spectrometry
evaluate
chlorination-induced
molecular-level
changes
derived
from
surface
water
sources.
We
correlated
components
with
profiles
selected
DBPs
using
new
alternative
methods
predictive
toxicological
assessments.
Our
findings
indicate
a
selective
natural
tendency
for
lignin
protein
conversion
manual
process.
The
reactivity
bioactive
compounds
decreased
order
>
tannin
or
ConAC.
mainly
attributed
lignin-
protein-like
within
CHO
CHNO
groups.
Additionally,
mitochondrial
damage
highly
sensitive
indicator
DOM-induced
cytotoxicity.
toxicity
revealed
37
common
toxicity-driving
characterized
by
low
mass,
medium
H/C
ratio,
O/C
reduction
state,
hydrophobicity.
highlight
need
exploit
health
effects
provide
substantial
experimental
evidence
necessity
remove
potential
toxicants.
Iodinated
disinfection
byproducts
(I-DBPs)
pose
significant
health
concerns
due
to
their
high
toxicity.
Current
approaches
recognize
unknown
I-DBPs
in
mass
spectrometry
(MS)
analysis
rely
on
negative
ionization
mode,
which
the
characteristic
I–
fragment
can
be
observed
tandem
spectra
(MS/MS).
Still,
many
ionize
exclusively
positive
where
is
absent.
To
address
this
gap,
work
developed
a
machine
learning-based
strategy
iodinated
compounds
(I-compounds)
from
MS/MS
both
electrospray
(ESI+)
and
(ESI−)
modes.
Investigating
over
6000
of
381
I-compounds,
we
first
identified
five
I-containing
neutral
losses
one
diagnostic
ESI+
ESI–
modes,
respectively.
We
then
trained
Random
Forest
models
integrated
them
into
IodoFinder,
Python
program,
streamline
recognition
I-compounds
raw
LC-MS
data.
IodoFinder
accurately
recognized
96%
161
I-compound
standards
In
its
application
DBP
mixtures,
discovered
19
with
annotated
structures
an
additional
17
assigned
formulas,
including
12
novel
3
confirmed
I-DBPs.
envision
that
will
advance
identification
known
exposome
studies.
