Environmental Science & Technology,
Год журнала:
2024,
Номер
58(43), С. 19289 - 19304
Опубликована: Окт. 16, 2024
Dissolved
organic
matter
(DOM)
is
an
ultracomplex
mixture
that
plays
a
central
role
in
global
biogeochemical
cycles.
Despite
its
importance,
DOM
remains
poorly
understood
at
the
molecular
level.
Over
last
decades,
significant
efforts
have
been
made
to
decipher
chemical
composition
of
by
high-resolution
mass
spectrometry
(HR-MS)
and
liquid
chromatography
(LC)
coupled
with
tandem
(MS/MS).
Yet,
complexity
high
degree
nonresolved
isomers
still
hamper
full
structural
analysis
DOM.
To
address
this
challenge,
we
developed
offline
two-dimensional
(2D)
LC
approach
using
two
reversed-phase
dimensions
orthogonal
pH
levels,
followed
MS/MS
data
acquisition
networking.
2D-LC-MS/MS
reduced
DOM,
enhancing
quality
spectra
increasing
spectral
annotation
rates.
Applying
our
analyze
coastal-surface
from
Southern
California
(USA)
open-ocean
North
Pacific
(Hawaii),
annotated
total
more
than
600
structures
via
spectrum
matching,
which
was
up
90%
iterative
1D
LC-MS/MS
same
run
time.
Our
offer
unprecedented
insights
into
marine
highlight
potential
approaches
samples.
Environmental Science & Technology,
Год журнала:
2024,
Номер
58(10), С. 4637 - 4647
Опубликована: Март 1, 2024
Marine
dissolved
organic
matter
(DOM)
is
an
important
component
of
the
global
carbon
cycle,
yet
its
intricate
composition
and
sea
salt
matrix
pose
major
challenges
for
chemical
analysis.
We
introduce
a
direct
injection,
reversed-phase
liquid
chromatography
ultrahigh
resolution
mass
spectrometry
approach
to
analyze
marine
DOM
without
need
solid-phase
extraction.
Effective
separation
achieved
with
large
chromatographic
column
extended
isocratic
aqueous
step.
Postcolumn
dilution
sample
flow
buffer-free
solvents
implementing
counter
gradient
reduced
buildup
in
ion
source
resulted
excellent
repeatability.
With
this
method,
over
5,500
unique
molecular
formulas
were
detected
from
just
5.5
nmol
100
μL
filtered
Arctic
Ocean
seawater.
observed
highly
linear
detector
response
variable
concentrations
high
robustness
against
matrix.
Compared
extracted
DOM,
our
injection
method
demonstrated
superior
sensitivity
heteroatom-containing
DOM.
The
analysis
seawater
offers
fast
simple
preparation
avoids
fractionation
introduced
by
facilitates
studies
environments,
where
only
minimal
volume
available
e.g.
sediment
pore
water,
ice
cores,
or
permafrost
soil
solution.
small
requirement
also
supports
higher
spatial
(e.g.,
soils)
temporal
culture
experiments).
Chromatographic
adds
further
information
formulas,
enhancing
understanding
biogeochemistry,
chemodiversity,
ecological
processes.
Environmental Science & Technology,
Год журнала:
2023,
Номер
57(7), С. 2981 - 2991
Опубликована: Фев. 7, 2023
The
interactions
between
dissolved
organic
matter
(DOM)
and
iron
(Fe)
oxyhydroxide
are
crucial
in
regulating
the
biogeochemical
cycling
of
nutrients
elements,
including
preservation
carbon
soils.
mechanisms
DOM
molecular
assembly
on
mineral
surfaces
have
been
extensively
studied
at
mesoscale
with
equilibrium
experiments,
yet
molecular-level
evolution
DOM-mineral
interface
under
dynamic
interaction
conditions
is
not
fully
understood.
Here,
we
designed
a
microfluidic
reactor
coupled
an
online
solid
phase
extraction
(SPE)-LC-QTOF
MS
system
to
continually
monitor
changes
composition
during
flowing
contact
Fe
circumneutral
pH,
which
simulates
soil
minerals
interacting
constant
input.
Time-series
UV-visible
absorption
spectra
mass
spectrometry
data
showed
that
after
aromatic
moieties
were
first
preferentially
sequestered
by
pristine
surface,
adsorption
nonaromatic
molecules
greater
hydrophobicity,
lower
acidity,
weights
(<400)
from
new
solutions
was
favored.
This
accompanied
transition
surface
chemistry-dominated
organic-organic
interaction-dominated
adsorption.
These
findings
provide
direct
evidence
zonal
model
taking
dynamics
interfacial
into
consideration.
study
also
shows
microfluidics
high-resolution
(HRMS)
promising
experimental
platform
for
probing
microscale
environmental
integrating
situ
reactions,
sample
pretreatment,
automatic
analysis.
Environmental Science & Technology,
Год журнала:
2022,
Номер
56(3), С. 1894 - 1904
Опубликована: Янв. 10, 2022
Effluent
organic
matter
(EfOM),
a
major
ozone
consumer
during
wastewater
ozonation,
is
complex
mixture
of
natural
and
anthropogenic
molecules.
Ozonation
EfOM
adds
to
molecular
complexity
by
introducing
polar
potentially
mobile
ozonation
byproducts
(OBPs).
Currently,
nontargeted
direct
infusion
(DI)
ultrahigh
resolution
mass
spectrometry
(e.g.
FT-ICR-MS)
used
study
OBPs
but
requires
sample
extraction,
limiting
the
accessible
polarity
range
OBPs.
To
better
understand
impact
on
formation
OBPs,
nonextracted
effluent
was
analyzed
injection
onto
reversed-phase
liquid
chromatography
system
(RP-LC)
online
hyphenated
with
an
FT-ICR-MS.
Over
four
times
more
were
detected
in
compared
extracted
solid
phase
extraction
measured
DI-FT-ICR-MS
(13817
vs
3075).
1500
highly
oxygenated
exclusively
early
eluting
fractions
EfOM,
indicating
Oxygenation
these
newly
discovered
higher
than
previously
found,
average
DBE-O
value
-3.3
O/C
ratio
0.84
earliest
OBP
fractions.
These
are
consistently
lost
may
play
important
role
understanding
environmental
ozonated
EfOM.
Moreover,
316
formulas
classified
as
nonreactive
can
be
identified
LC-FT-ICR-MS
isomers
varying
degrees
reactivity,
providing
for
first
time
experimental
evidence
differential
reactivity
ozone.
Environmental Science and Ecotechnology,
Год журнала:
2024,
Номер
21, С. 100392 - 100392
Опубликована: Янв. 27, 2024
Activated
carbon
is
employed
for
the
adsorption
of
organic
micropollutants
(OMPs)
from
water,
typically
present
in
concentrations
ranging
ng
L−1
to
μg
L−1.
However,
efficacy
OMP
removal
considerably
deteriorated
due
competitive
background
dissolved
matter
(DOM),
at
substantially
higher
mg
Interpreting
characteristics
DOM
crucial
predicting
efficiencies
across
diverse
natural
waters.
Molecular
weight
(MW),
aromaticity,
and
polarity
influence
competitiveness.
Although
aromaticity-related
metrics,
such
as
UV254,
low
MW
were
proposed
correlate
with
competitiveness,
method
suffers
limitations
understanding
interplay
aromaticity
determining
Here,
we
elucidate
intricate
competition,
spanning
a
fraction
level
compound
level,
by
employing
direct
sample
injection
liquid
chromatography
coupled
ultrahigh-resolution
Fourier-transform
ion
cyclotron
resonance
mass
spectrometry.
Anion
exchange
resin
pre-treatment
eliminated
93
%
UV254-active
DOM,
predominantly
aromatic
polar
only
minimally
alleviated
competition.
characterization
revealed
that
nonpolar
molecular
formulas
(constituting
26
PAC-adsorbable
DOM)
medium
contributed
more
Isomer-level
analysis
indicated
competitiveness
highly
LMW
compounds
was
strongly
counterbalanced
increased
polarity.
Strong
aromaticity-derived
π-π
interaction
cannot
facilitate
hydrophilic
compounds.
Our
results
underscore
constraints
depending
solely
on
aromaticity-based
approaches
exclusive
interpretive
measure
In
broader
context,
this
study
demonstrates
an
effect-oriented
analysis,
elucidating
counterbalancing
interactions
properties
level.
The Analyst,
Год журнала:
2024,
Номер
149(12), С. 3468 - 3478
Опубликована: Янв. 1, 2024
We
show
how
ultrahigh
resolution
mass
spectrometry
hyphenated
with
liquid
chromatography
and
a
post-column
infused
internal
standard
can
be
used
for
semi-quantitative
analysis
of
dissolved
organic
matter
injected
at
native
concentrations.
ACS ES&T Water,
Год журнала:
2021,
Номер
1(8), С. 1975 - 1982
Опубликована: Июль 27, 2021
Dissolved
organic
matter
(DOM)
is
an
ultracomplex
mixture
of
compounds
in
the
land/ocean–atmosphere
interface.
Normally,
polar
from
DOM
are
hardly
retained
by
liquid
chromatography
(LC)
columns
for
further
analytical
purposes.
Here,
we
utilized
Fourier
transform
ion
cyclotron
resonance
mass
spectrometry
with
LC
online
analysis
river
water
and
rainwater.
With
sophisticated
instrumental
optimization,
different
portions
metal
salts,
carboxyl-rich
alicyclic
molecules,
organosulfates
(OSs),
lignin-like
could
be
fully
fractionated
within
one
cycle
(20
min).
The
complexity
analyte
was
greatly
reduced
separation,
which
therefore
allows
much
better
MS
performance.
Moreover,
compounds'
structures
were
characterized
tandem
(MSn).
protocol
presented
herein
offers
a
novel
insight
into
conventional
LC-MS
method,
that
it
has
potential
to
investigate
OSs
other
components
according
specific
functional
groups
heteroatoms
explore
their
sources
reaction
mechanisms.
