Atmospheric chemistry and physics,
Год журнала:
2024,
Номер
24(24), С. 14177 - 14190
Опубликована: Дек. 19, 2024
Abstract.
Secondary
organic
aerosols
(SOAs)
from
highly
volatile
compounds
(VOCs)
are
currently
not
well
represented
in
numerical
models
as
their
heterogeneous
formation
mechanisms
the
atmosphere
remain
unclear.
Based
on
smog
chamber
experiments,
here
we
investigated
yield
and
pathway
of
SOA
acetone
photochemical
reactions
under
low-NOx
conditions
presence
preexisting
haze
particles
((NH4)2SO4
NH4HSO4)
saline
mineral
(Na2SO4)
ammonia-rich
conditions.
Our
results
showed
that
acetone-derived
is
remarkably
enhanced
via
multiphase
these
seeds,
especially
for
particles.
We
found
aerosol
acidity
a
key
factor
controlling
pathways
SOA,
which
acids,
alcohol,
carbonyls
produced
dissolve
into
aqueous
phase
seeds
subsequently
esterify
and/or
oligomerize
SOAs
consist
larger
molecules
acidic
but
smaller
neutral
aerosols.
Moreover,
light
absorption
ability
formed
(NH4)2SO4
stronger
than
Na2SO4
particles,
ammonia,
due
to
N-containing
organics.
Through
comparison
with
methylglyoxal
(MGly),
total
2.8–8.2
times
irreversible
uptake
MGly,
suggesting
only
considering
MGly
precursor
will
probably
underestimate
role
global
production
since
abundantly
exists
troposphere.
Atmospheric chemistry and physics,
Год журнала:
2024,
Номер
24(16), С. 9263 - 9275
Опубликована: Авг. 26, 2024
Abstract.
An
enhanced
formation
of
brown
carbon
(BrC)
with
a
non-negligible
warming
effect
at
the
tropopause
has
recently
been
found.
However,
its
mechanism
is
unclear.
Here,
we
report
on
BrC
process
that
happens
during
air
mass
upward
transport
by
conducting
simultaneous
measurements
atmospheric
4
h
time
resolution
mountain
foot
(MF,
400
m
a.s.l.)
and
mountainside
(MS,
1120
Mt.
Hua,
China,
in
2016
summer.
Our
results
showed
daytime
light
absorption
(abs365
nm)
MS
approximately
60
%
lower
than
MF
due
to
dilution
caused
planetary
boundary
layer
expansion,
but
relative
black
about
30
higher
MF,
suggesting
significant
secondary
lifting
from
MS.
Such
accounted
for
>
50
only
27
MF.
Moreover,
N:C
elemental
ratio
was
15
mainly
an
aerosol
aqueous-phase
water-soluble
organic
nitrogen
(WSON)
compounds.
Stable
isotope
composition
further
indicated
such
light-absorbing
WSON
compounds
were
produced
reaction
carbonyls
NH4+.
work
revealed,
first
time,
ammonia-induced
aqueous
reactions
can
significantly
promote
process,
which
probably
responsible
upper
layer.
Abstract.
To
understand
the
spatial
variation
of
optical
and
structural
properties
water-soluble
brown
carbon
its
influencing
factors
in
China,
light
absorption,
fluorescence,
Fourier
transform
infrared
(FTIR)
spectrum
organic
(WSOC)
different
regions
China
are
measured
following
same
analytical
methods.
The
average
absorption
coefficients
mass
efficiencies
WSOC
at
365
nm
(Abs365
MAE365)
rank
from
high
to
low
as
northwest
>
southwest
north
east
regional
site,
with
higher
values
Northern
than
Southern
sites,
inland
areas
coastal
areas.
resolved
by
positive
matrix
factorization
model
combined
spectra
abundant
aromatic
O-H
C=C
functional
groups
determined
FTIR
both
indicate
that
compounds
important
light-absorbing
substances
WSOC,
which
also
have
a
significant
impact
on
fluorophores.
Multiple
linear
regression
analysis
shows
identified
fluorophores
fluorescence
parallel
factor
contribute
about
62–93
%
all
humic-like
substance
(HULIS)
contributes
most,
especially
highly‑oxygenated
HULIS
(29
%–50
%)
long
emission
wavelengths.
Combustion
source
emissions
atmospheric
chemical
processes
impacts
some
sites.
Moreover,
relative
humidity
(RH)
can
affect
MAE365
decreasing
increase
RH
when
<
60
remaining
relatively
unchanged
%.
Taken
together,
this
study
promotes
better
understanding
heterogeneity
their
China.
Atmosphere,
Год журнала:
2024,
Номер
15(11), С. 1294 - 1294
Опубликована: Окт. 28, 2024
Brown
carbon
aerosols
(BrC),
a
subfraction
of
organic
aerosols,
significantly
influence
the
atmospheric
environment,
climate
and
human
health.
The
North
China
Plain
(NCP)
is
hotspot
for
BrC
research
in
China,
yet
our
understanding
optical
properties
rural
regions
still
very
limited.
In
this
study,
we
characterize
chemical
components
light
absorption
at
site
during
winter
NCP.
average
mass
concentration
PM1
135.1
±
82.3
μg/m3;
organics
nitrate
are
main
PM1.
coefficient
(babs,BrC)
53.6
45.7
Mm−1,
accounting
39.5
10.2%
total
370
nm.
Diurnal
variations
reveal
that
babs,BrC
lower
afternoon,
attributed
to
evolution
planetary
boundary
layers.
mainly
emitted
locally,
both
aqueous
phase
photooxidation
reactions
can
increase
babs,BrC.
Notably,
reduced
when
RH
>
65%.
During
foggy
conditions,
facilitate
formation
secondary
contribute
bleaching
BrC.
This
process
ultimately
causes
decrease
Ångström
exponent
(AAE)
efficiency
(MAE).
contrast,
babs,BrC,
along
with
AAE
MAE,
rise
due
substantial
primary
emissions.
study
enhances
polluted
Atmospheric chemistry and physics,
Год журнала:
2024,
Номер
24(24), С. 14177 - 14190
Опубликована: Дек. 19, 2024
Abstract.
Secondary
organic
aerosols
(SOAs)
from
highly
volatile
compounds
(VOCs)
are
currently
not
well
represented
in
numerical
models
as
their
heterogeneous
formation
mechanisms
the
atmosphere
remain
unclear.
Based
on
smog
chamber
experiments,
here
we
investigated
yield
and
pathway
of
SOA
acetone
photochemical
reactions
under
low-NOx
conditions
presence
preexisting
haze
particles
((NH4)2SO4
NH4HSO4)
saline
mineral
(Na2SO4)
ammonia-rich
conditions.
Our
results
showed
that
acetone-derived
is
remarkably
enhanced
via
multiphase
these
seeds,
especially
for
particles.
We
found
aerosol
acidity
a
key
factor
controlling
pathways
SOA,
which
acids,
alcohol,
carbonyls
produced
dissolve
into
aqueous
phase
seeds
subsequently
esterify
and/or
oligomerize
SOAs
consist
larger
molecules
acidic
but
smaller
neutral
aerosols.
Moreover,
light
absorption
ability
formed
(NH4)2SO4
stronger
than
Na2SO4
particles,
ammonia,
due
to
N-containing
organics.
Through
comparison
with
methylglyoxal
(MGly),
total
2.8–8.2
times
irreversible
uptake
MGly,
suggesting
only
considering
MGly
precursor
will
probably
underestimate
role
global
production
since
abundantly
exists
troposphere.