Journal of Geophysical Research Atmospheres,
Год журнала:
2024,
Номер
129(23)
Опубликована: Ноя. 28, 2024
Abstract
The
key
problems
with
Positive
Matrix
Factorization
(PMF)
model
for
PM
2.5
source
apportionment
were
inconsistent
results
different
species
selections
and
a
lack
of
evaluation
criteria
accuracy.
Moreover,
high
proportions
secondary
inorganic
aerosols
sources
(SNA)
identified
by
PMF
without
corresponding
primary
sources.
This
study
develops
new
method
that
combines
multi‐isotopes
(
34
S,
15
N,
18
O
14
C)
to
optimize
apportionment.
Data
sets
A–F,
constructed
from
components,
input
into
obtain
optimal
(3–9
factors),
which
changed
the
selection
species.
Specifically,
contributions
coal
combustion
(CC,
3%–36%),
biomass
burning
(BB,
11%–38%),
vehicle
(VS,
4%–15%)
showed
significant
differences
in
data
sets,
indicating
conventional
methods
cannot
accurate
results.
Then,
introduced
restrict
reallocate
SNA
sources,
overcoming
influence
on
Additionally,
C
was
used
evaluate
results,
combination
more
markers
(data
set
F,
9‐factor)
techniques
obtained
optimized
aligned
Compared
initial
CC,
VS,
BB
allocated
9‐factor
increased
26.4%,
5%,
19.5%,
respectively,
becoming
main
.
represents
first
time
achieves
reapportionment
evaluation,
improving
methods.
Environment International,
Год журнала:
2025,
Номер
196, С. 109317 - 109317
Опубликована: Фев. 1, 2025
Stable
nitrogen
isotopic
composition
(δ15N)
has
proven
to
be
a
valuable
tool
for
identifying
sources
of
nitrates
(NO3-)
in
PM2.5.
However,
the
absence
systematic
study
on
δ15N
values
domestic
NOx
hinders
accurate
identification
NO3-
China.
Here,
we
systematically
determined
and
refined
six
categories
Tianjin
using
an
active
sampling
method.
Moreover,
PM2.5
were
measured
during
pre-heating,
mid-heating
late-heating
periods,
which
are
most
heavily
polluted
Tianjin.
The
results
indicate
that
fingerprints
types
indicative
regional
characteristics
China,
particularly
North
China
Plain.
Bayesian
isotope
mixing
(MixSIAR)
model
demonstrated
coal
combustion,
biomass
burning,
vehicle
exhaust
collectively
contributed
more
than
60
%,
dominating
periods
failure
consider
signatures
local
could
result
overestimation
contribution
from
natural
gas
combustion.
Additionally,
industrial
sources,
uncharacterized
source
previous
studies,
may
directly
fraction
other
being
overestimated
by
10
%.
Notably,
as
number
input
increased,
various
was
becoming
stable,
inter-influence
between
significantly
reduced.
This
fingerprint
effectively
distinguish
NO3-,
thereby
providing
insights
controlling
pollution.
Journal of Geophysical Research Atmospheres,
Год журнала:
2024,
Номер
129(9)
Опубликована: Апрель 29, 2024
Abstract
The
stable
nitrogen
isotopic
composition
(δ
15
N)
has
been
widely
used
to
quantify
sources
of
ammonium
(NH
4
+
)
in
PM
2.5
.
However,
the
overlap
and
uncertainty
δ
N
values
from
different
NH
3
sources,
coupled
with
their
seasonal
variability,
hinder
accurate
identification
source.
Here,
various
source
samples
collected
by
active
sampler
were
determined.
Subsequently,
we
measured
,
which
seasonally
Tianjin.
We
found
that
combustion‐related
(c‐NH
exhibiting
higher
compared
volatile
(v‐NH
),
but
all
was
fell
within
range
reported
previous
studies.
Furthermore,
inconsistent
variations
observed
N‐NH
originating
emissions
agricultural
soil
human
excreta.
application
Bayesian
isotope
mixing
model
(MixSIAR
model)
revealed
a
significant
increase
contribution
v‐NH
when
incorporating
current
data,
as
opposed
for
Notably,
(53.1%)
almost
equivalent
c‐NH
(46.9%)
considering
signatures
Additionally,
estimated
exhibited
is
more
reasonable
than
non‐seasonal
scenario.
This
study
demonstrated
contributed
Tianjin
equally,
it
highlighted
should
be
considered
estimating
contributions
MixSIAR
model.
Journal of Geophysical Research Atmospheres,
Год журнала:
2025,
Номер
130(2)
Опубликована: Янв. 13, 2025
Abstract
δ
15
N‐NO
3
−
is
widely
used
to
trace
the
NO
x
/NO
emission
sources
without
unique
source
tracers.
However,
there
still
controversy
regarding
N
fractionation
effects
during
formation,
leading
uncertain
apportionment.
To
address
this,
this
study
introduces
dual
oxygen
isotopes
(∆
17
O
and
18
O)
constrain
N‐∆
O/∆
N‐δ
of
formation
compare
impact
(δ
on
Results
found
significant
differences
in
∆
(−3.7
∼
+16.1‰)
(+8.5
+16.2‰)
haze,
reflecting
from
three
pathways
(NO
2
+
OH,
HC,
5
hydrolysis)
two
OH
hydrolysis),
respectively.
The
value
obtained
by
increases
with
increase
HC
contribution
(0.02–0.65).
Additionally,
different
results
apportionment
were
(
HC‐induced
haze.
For
example,
identified
coal
combustion
(46
±
8%)
biomass
burning
(32
3%)
as
major
Zibo
Conversely,
revealed
mobile
(55
(22
5%)
main
contributors.
Evidence
diurnal
variation
characteristics
tracers
show
that
analysis
more
sensitive
accurate
than
O).
These
highlight
non‐negligible
role
provide
insight
into
improving
tracing
techniques
for
identification
through
constraint
isotopes.
Journal of Geophysical Research Atmospheres,
Год журнала:
2023,
Номер
128(8)
Опубликована: Апрель 19, 2023
Abstract
Sulfate
(SO
4
2−
)
sources
are
unclear
leading
to
the
underestimation
of
its
concentration
in
model.
Hourly
resolution
δ
34
S‐SO
2
and
values
three
haze
episodes
(EP1‐EP3)
were
synchronously
collected
for
first
time
quantify
influence
S
fractionation
from
emission
(e.g.,
coal
combustion)
SO
atmospheric
oxidation
on
/SO
source
apportionment.
After
considering
combustion
oxidation,
reasonable
logical
contributions
obtained,
showing
highly
consistent
with
that
Positive
Matrix
Factorization
model
results.
Considering
fraction
apportionment
obtained
by
hourly
can
more
accurately
reflect
dynamic
changes
sources.
Traffic
emissions
(49%)
(46%–65%)
major
contributors
EP1
EP2‐EP3,
respectively.
However,
obvious
deviations
contribution
found
without
combustion.
Especially
northwest
transmission
channels
deviation
accounted
17.1%–38.5%
secondary
.
Moreover,
was
considered
as
a
sensitive
indicator
than
results
comparison
technique
air
quality
(Nested
Air
Quality
Prediction
Model
System),
which
provide
reliable
evidence
control.
Environmental Science & Technology,
Год журнала:
2023,
Номер
57(49), С. 20726 - 20735
Опубликована: Ноя. 30, 2023
δ18O
is
widely
used
to
track
nitrate
(NO3-)
formation
but
overlooks
NO3
radical
reactions
with
hydrocarbons
(HCs),
particularly
in
heavily
emitting
hazes.
This
study
introduces
high-time
resolution
Δ17O-NO3-
as
a
powerful
tool
quantify
NO3-
during
five
hazes
three
cities.
Results
show
significant
differences
between
and
δ18O-NO3-
identifying
formation.
results
suggested
N2O5
hydrolysis
(62.0-88.4%)
the
major
pathway
of
formation,
while
shows
contributions
NO2
+
OH
(17.7-66.3%),
HC
(10.8-49.6%),
(22.9-33.3%),
revealing
contribution
(41.7-56%)
under
severe
pollution.
Furthermore,
varies
temperatures,
NOx
oxidation
rate
(NOR),
pollution
levels.
Higher
lower
were
observed
at
higher
except
for
low
NOR
haze
where
temperatures
(T
←
10
°C).
emphasizes
significance
emission-dominated
haze.
Contributions
relate
positive
(fP1
=
3.0*NOR2
-
2.4*NOR
0.8)
negative
(fP2
-2.3*NOR2
1.8*NOR)
quadratic
functions,
respectively,
min/max
values
0.4.
At
mild
pollution,
(58.1
±
22.2%)
dominated
shifting
(35.5
16.3%)
Additionally,
reveals
that
morning-evening
rush
hours
high
noon
promote
OH,
respectively.
Our
are
attributed
NOR,
vital
quantifying