Toxics,
Год журнала:
2024,
Номер
12(2), С. 105 - 105
Опубликована: Янв. 26, 2024
Sulfate
(SO42−)
is
an
essential
chemical
species
in
atmospheric
aerosols
and
plays
influential
role
their
physical–chemical
characteristics.
The
mechanisms
of
secondary
SO42−
aerosol
have
been
intensively
studied
air-polluted
cities.
However,
few
studies
focused
on
cities
with
good
air
quality.
One-year
PM2.5
samples
were
collected
the
tropical
island
city
Haikou,
water-soluble
inorganic
ions,
as
well
Fe
Mn,
analyzed.
results
showed
that
non-sea-salt
(nss-SO42−)
was
dominant
accounting
for
40–57%
total
ions
Haikou.
S(IV)+H2O2
pathway
main
formation
wintertime
contributing
to
57%
formation.
By
contrast,
54%
produced
by
S(IV)+Fe×Mn
summer.
In
spring
autumn,
S(IV)+H2O2,
S(IV)+Fe×Mn,
S(IV)+NO2
pathways
contributed
equally
ionic
strength
controlling
parameter
pathway,
while
pH
identified
a
key
factor
mediates
produce
SO42−.
This
study
contributes
our
understanding
production
under
low
concentrations
but
high
percentages.
Environmental Science & Technology,
Год журнала:
2023,
Номер
57(46), С. 18282 - 18295
Опубликована: Апрель 28, 2023
Fine
particulate
matter
(PM2.5)
chemical
composition
has
strong
and
diverse
impacts
on
the
planetary
environment,
climate,
health.
These
effects
are
still
not
well
understood
due
to
limited
surface
observations
uncertainties
in
model
simulations.
We
developed
a
four-dimensional
spatiotemporal
deep
forest
(4D-STDF)
estimate
daily
PM2.5
at
spatial
resolution
of
1
km
China
since
2000
by
integrating
measurements
species
from
high-density
observation
network,
satellite
retrievals,
atmospheric
reanalyses,
Cross-validation
results
illustrate
reliability
sulfate
(SO42-),
nitrate
(NO3-),
ammonium
(NH4+),
chloride
(Cl-)
estimates,
with
high
coefficients
determination
(CV-R2)
ground-based
0.74,
0.75,
0.71,
0.66,
average
root-mean-square
errors
(RMSE)
6.0,
6.6,
4.3,
2.3
μg/m3,
respectively.
The
three
components
secondary
inorganic
aerosols
(SIAs)
account
for
21%
20%
14%
(NH4+)
total
mass
eastern
China;
we
observed
significant
reductions
40-43%
between
2013
2020,
slowing
down
2018.
Comparatively,
ratio
SIA
increased
7%
across
except
Beijing
nearby
areas,
accelerating
recent
years.
SO42-
been
dominant
component
China,
although
it
was
surpassed
NO3-
some
e.g.,
Beijing-Tianjin-Hebei
region
2016.
SIA,
accounting
nearly
half
(∼46%)
mass,
drove
explosive
formation
winter
haze
episodes
North
Plain.
A
sharp
decline
concentrations
an
increase
SIA-to-PM2.5
ratios
during
COVID-19
lockdown
were
also
revealed,
reflecting
enhanced
oxidation
capacity
particles.
Atmospheric chemistry and physics,
Год журнала:
2022,
Номер
22(20), С. 13467 - 13493
Опубликована: Окт. 19, 2022
Abstract.
The
importance
of
dust
heterogeneous
oxidation
in
the
removal
atmospheric
SO2
and
formation
sulfate
aerosols
is
not
adequately
understood.
In
this
study,
Fe-,
Ti-,
Al-bearing
components,
Na+,
Cl−,
K+,
Ca2+
surface,
were
discovered
to
be
closely
associated
with
sulfate.
Regression
models
then
developed
make
a
reliable
prediction
reactivity
based
on
particle
chemical
compositions.
Further,
recognized
gas-phase,
aqueous-phase,
routes
quantitatively
assessed
kinetically
compared
by
combining
laboratory
work
modelling
study.
presence
55
µg
m−3
airborne
dust,
accounts
for
approximately
28.6
%
secondary
during
nighttime,
while
proportion
decreases
13.1
solar
irradiation.
On
drivers
(e.g.
transition
metal
constituents,
water-soluble
ions)
are
more
efficient
than
surface-adsorbed
oxidants
H2O2,
NO2,
O3)
conversion
SO2,
particularly
nighttime.
Dust
offers
an
opportunity
explain
missing
source
severe
haze
pollution
events,
its
contribution
complex
environments
could
even
higher
current
calculation
results.
Overall,
surface
responsible
significant
have
profound
impacts
sulfur
cycling.
Advances in Atmospheric Sciences,
Год журнала:
2023,
Номер
40(8), С. 1339 - 1361
Опубликована: Апрель 28, 2023
Atmospheric
chemistry
research
has
been
growing
rapidly
in
China
the
last
25
years
since
concept
of
"air
pollution
complex"
was
first
proposed
by
Professor
Xiaoyan
TANG
1997.
For
papers
published
2021
on
air
(only
included
Web
Science
Core
Collection
database
were
considered),
more
than
24
000
authored
or
co-authored
scientists
working
China.
In
this
paper,
we
review
a
limited
number
representative
and
significant
studies
atmospheric
few
years,
including
(1)
sources
emission
inventories,
(2)
chemical
processes,
(3)
interactions
with
meteorology,
weather
climate,
(4)
between
biosphere
atmosphere,
(5)
data
assimilation.
The
intention
not
to
provide
complete
all
progress
made
but
rather
serve
as
starting
point
for
learning
about
advances
reviewed
paper
have
enabled
theoretical
framework
complex
be
established,
provided
robust
scientific
support
highly
successful
control
policies
China,
created
great
opportunities
education,
training,
career
development
many
graduate
students
young
scientists.
This
further
highlights
that
developing
low-income
countries
are
heavily
affected
can
benefit
from
these
advances,
whilst
at
same
time
acknowledging
challenges
still
remain
hopefully
addressed
over
next
decades.
Journal of the American Chemical Society,
Год журнала:
2024,
Номер
146(10), С. 6580 - 6590
Опубликована: Март 1, 2024
The
multiphase
oxidation
of
sulfur
dioxide
(SO2)
to
form
sulfate
is
a
complex
and
important
process
in
the
atmosphere.
While
conventional
photosensitized
reaction
mainly
explored
bulk
medium
reported
be
one
drivers
trigger
atmospheric
production,
how
this
scheme
functionalizes
at
air–water
interface
(AWI)
aerosol
remains
an
open
question.
Herein,
employing
advanced
size-controllable
microdroplet-printing
device,
surface-enhanced
Raman
scattering
(SERS)
analysis,
nanosecond
transient
adsorption
spectrometer,
molecular
level
theoretical
calculations,
we
revealed
previously
overlooked
interfacial
role
SO2
humic-like
substance
(HULIS)
aerosol,
where
3–4
orders
magnitude
increase
formation
rate
was
speculated
cloud
relevant-sized
particles
relative
bulk-phase
medium.
rapid
battery
reactive
oxygen
species
(ROS)
comes
from
accelerated
electron
transfer
AWI,
excited
triplet
state
HULIS
(3HULIS*)
incomplete
solvent
cage
can
readily
capture
electrons
HSO3–
way
that
more
efficient
than
fully
blocked
by
water
molecules.
This
phenomenon
could
explained
significantly
reduced
desolvation
energy
barrier
required
for
reagents
residing
AWI
region
with
shell.
Environmental Science & Technology,
Год журнала:
2024,
Номер
58(6), С. 2912 - 2921
Опубликована: Янв. 22, 2024
Currently,
atmospheric
sulfate
aerosols
cannot
be
predicted
reliably
by
numerical
models
because
the
pathways
and
kinetics
of
formation
are
unclear.
Here,
we
systematically
investigated
synergetic
catalyzing
role
transition-metal
ions
(TMIs,
Fe3+/Mn2+)
in
oxidation
SO2
O2
on
using
chamber
experiments.
Our
results
showed
that
effect
TMIs
is
critically
dependent
aerosol
pH
due
to
solubility
Fe(III)
species
sensitive
aqueous
phase
acidity,
which
effective
only
under
<
3
conditions.
The
rate
2
orders
magnitude
larger
than
bulk
solution
increases
significantly
smaller
aerosols,
suggesting
such
a
synergetic-catalyzed
occurs
surface.
kinetic
reaction
can
described
as
R
=
k*[H+]−2.95[Mn(II)][Fe(III)][S(IV)]
(pH
≤
3.0).
We
found
TMI-synergetic-catalyzed
dominant
pathway
Beijing
when
haze
particles
very
acidic,
while
heterogeneous
NO2
most
important
weakly
acidic.
work
for
first
time
clarified
periods,
parameterized
into
future
studies
formation.
Geophysical Research Letters,
Год журнала:
2024,
Номер
51(3)
Опубликована: Фев. 5, 2024
Abstract
Sulfate
aerosol
greatly
contributes
to
wintertime
haze
pollution
in
emission‐intensive
regions
like
the
North
China
Plain
(NCP)
China.
Fast
sulfate
increase
and
accumulation
are
usually
recorded
during
winter
haze;
however,
multiphase
oxidation
of
sulfur
dioxide
(SO
2
)
physical
processes
affecting
near‐surface
not
fully
understood.
By
combining
situ
observations
numerical
simulations,
we
found
that
high
ratios
(>0.6)
under
heavily
polluted
conditions
associated
with
low
clouds
fog
over
NCP,
induced
by
moist
southerly
airflow.
Thick
SO
levels
NCP
provide
a
reaction
environment
for
production.
The
production
rate
cloud
water
can
reach
0.5–1.3
μg
m
−3
h
−1
.
results
demonstrate
vertical
mixing
generated
within
surface
plays
significant
role
rapid
production,
highlighting
importance
understanding
cloud‐water
pollution.
npj Climate and Atmospheric Science,
Год журнала:
2023,
Номер
6(1)
Опубликована: Окт. 27, 2023
Abstract
Fine-particle
pollution
associated
with
high
sulfate
and
secondary
organic
aerosol
(SOA)
contents
still
occurs
in
winter,
despite
considerable
reductions
precursor
emissions
China.
The
chemical
mechanisms
involved
are
consistently
acknowledged
to
be
linked
water
but
remain
poorly
understood.
Here,
we
present
findings
demonstrating
that
the
synergistic
effect
of
elevated
content
particles
originating
from
fossil
fuel
combustion
significantly
enhanced
rapid
formation
SOAs
under
humidity
conditions
during
winter
northern
presence
promoted
aging
process
containing
elemental
carbon
(EC)
facilitated
SOAs.
Evidence
single
reveals
an
increased
potential
for
SOA
primary
aerosols
(POAs)
combustion,
increasing
water.
Under
relative
exceeding
85%,
multiphase
oxidation
SO
2
by
in-particle
nitrite/nitrous
acid,
generated
through
reactions
involving
aged
EC-containing
iron-rich
particles,
as
well
aqueous-phase
hydroxymethanesulfonate
(HMS),
led
a
substantial
increase
production.
This
study
emphasizes
critical
role
chemistry
concerning
SOAs,
highlighting
urgent
necessity
mitigate
combustion.
Atmospheric chemistry and physics,
Год журнала:
2024,
Номер
24(11), С. 6635 - 6662
Опубликована: Июнь 6, 2024
Abstract.
Winter
fog
and
severe
aerosol
loading
in
the
boundary
layer
over
northern
India,
particularly
Indo-Gangetic
Plain
(IGP),
disrupt
daily
lives
of
millions
people
region.
To
better
understand
role
aerosol–radiation
(AR)
feedback
on
occurrence,
spatial
extent,
persistence
winter
fog,
as
well
associated
aqueous
chemistry
IGP,
several
model
simulations
have
been
performed
using
Weather
Research
Forecasting
coupled
with
Chemistry
(WRF-Chem).
While
WRF-Chem
was
able
to
represent
formation
for
23–24
December
2017
event
central
IGP
comparison
station
satellite
observations,
underestimated
PM2.5
concentrations
compared
Central
Pollution
Control
Board
(CPCB)
India
monitoring
network.
evaluating
composition
events
we
found
that
quite
different
from
measurements
obtained
during
Fog
Experiment
(WiFEX)
Delhi,
secondary
aerosols,
chloride
fraction,
being
strongly
underpredicted
(∼
66.6
%).
Missing
emission
sources
(e.g.,
industry
residential
burning
cow
dung
trash)
processes
need
be
investigated
improve
model–observation
agreement.
By
investigating
a
weakens
turbulence,
lowers
height,
increases
relative
humidity
(RH)
within
layer.
Factors
affecting
include
loss
aerosols
through
deposition
cloud
droplets
internal
mixing
absorbing
scattering
aerosols.
Aqueous-phase
concentrations,
which
subsequently
affect
by
both
increased
mass
sizes.
With
interaction
aqueous-phase
chemistry,
began
1–2
h
earlier
caused
longer
duration
than
when
these
were
not
included
simulation.
The
increase
RH
experiments
important
it
promoted
growth
size
water
uptake,
increasing
content
IGP.
results
this
study
suggest
play
an
air
quality
intensity
lifetime
yet
other
feedbacks,
such
aerosol–cloud
interactions,
quantified.
One Earth,
Год журнала:
2024,
Номер
7(6), С. 1082 - 1095
Опубликована: Июнь 1, 2024
Aerosols
in
the
atmosphere
are
effective
microreactors
for
aqueous
reactions
converting
primary
pollutants
to
secondary
fine
particulate
matter
(PM2.5).
These
believed
scale
with
volume
of
water,
such
as
water
deliquesced
urban
aerosols.
Here,
using
single-particle
Raman
spectroscopy,
we
mapped
scaling
law
conversion
rate
sulfite
microdroplets,
a
key
reaction
producing
sulfate
PM2.5
and
driving
formation
China's
haze.
We
show
that,
droplets
below
approximately
100
μm,
this
scales
not
volume,
but
droplet
surface
area,
owing
kinetic
acceleration
at
air-water
interface.
Therefore,
when
linearly
extrapolating
rates
aerosol
air-quality
models
may
inaccurately
predict
rates.
predictions
likely
underpredictions,
if
adopt
parameters
measured
from
laboratory
systems,
i.e.,
bulk
solutions,
surface-area-to-volume
ratio
much
smaller
than
atmospheric