Journal of Geophysical Research Atmospheres,
Год журнала:
2023,
Номер
128(20)
Опубликована: Окт. 13, 2023
Abstract
Severe
haze
in
Beijing
is
characterized
by
the
rapid
formation
of
sulfate
via
multiphase
oxidation
SO
2
.
While
many
factors,
including
aerosol
oxidants
and
atmospheric
variables,
were
discovered
investigated,
their
relative
importance
remains
unclear.
Herein,
based
on
field
observation
data
obtained
Beijing,
China,
we
developed
a
kinetic
model
to
explore
key
factors
that
determine
sulfate.
Sensitivity
tests
give
kinetics
each
pathway
varying
with
pH
temperature,
which
total
rate
at
room
temperature
(298
K)
calculated
be
generally
greater
than
standard
(273
K),
especially
during
nighttime.
Interfacial
are
responsible
for
within
wide
range,
transition
metal
ions
become
more
efficient
increased
temperature.
The
chemistry
additionally
affected
liquid
water
content
(ALWC),
particle
radius
(R
p
),
ionic
strength
(IS).
Within
usual
acidity,
discrepancy
induced
different
ALWC
levels
significant
lower
contrast
dependence
related
R
,
effect
IS
depends
highly
pH.
Machine
learning
reveals
potential
Temperature
acidity
impactful
both
aqueous
interfacial
sulfates,
whereas
only
affects
processes.
between
nighttime
daytime
considered
throughout
this
study.
Overall,
study
recommended
evaluation
future
laboratory
research.
Journal of the American Chemical Society,
Год журнала:
2024,
Номер
146(2), С. 1467 - 1475
Опубликована: Янв. 8, 2024
We
present
a
novel
mechanism
for
the
formation
of
photocatalytic
oxidants
in
deliquescent
NaCl
particles,
which
can
greatly
promote
multiphase
photo-oxidation
SO2
to
produce
sulfate.
The
photoexcitation
[Cl––H3O+–O2]
complex
leads
generation
Cl
and
OH
radicals,
is
key
reason
enhancing
aqueous-phase
oxidation
accelerating
oxidation.
mass
normalization
rate
sulfate
production
from
photoreaction
on
droplets
could
be
estimated
0.80
×
10–4
μg·h–1
at
72%
RH
1.33
81%
RH,
equivalent
known
O3
liquid-phase
mechanism.
Our
findings
highlight
significance
particles
as
non-negligible
source
coastal
areas.
Furthermore,
this
study
underscores
importance
Cl–
photochemistry
atmosphere.
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.
Nature Communications,
Год журнала:
2024,
Номер
15(1)
Опубликована: Май 30, 2024
Abstract
Traditional
atmospheric
chemistry
posits
that
sulfur
dioxide
(SO
2
)
can
be
oxidized
to
sulfate
4
2–
through
aqueous-phase
reactions
in
clouds
and
gas-phase
oxidation.
Despite
adequate
knowledge
of
traditional
mechanisms,
several
studies
have
highlighted
the
potential
for
SO
oxidation
within
aerosol
water.
Given
widespread
presence
tropospheric
aerosols,
2−
production
water
could
a
pervasive
global
impact.
Here,
we
quantify
contributions
aqueous
pathways
formation
based
on
GEOS-Chem
simulations
subsequent
theoretical
calculations.
Hydrogen
peroxide
(H
O
significantly
influences
continental
regions
both
horizontally
vertically.
Over
past
two
decades,
shifts
typical
cities
reveal
an
intriguing
trend:
despite
reductions
emissions,
increased
capacities,
like
rising
H
levels,
prevent
steady
decline
concentrations.
Abating
oxidants
would
facilitate
benefit
reduction
positive
feedback
mitigation.
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.
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
Environmental Science & Technology,
Год журнала:
2025,
Номер
unknown
Опубликована: Фев. 2, 2025
Hydrogen
peroxide
(H2O2)
plays
a
key
role
in
atmospheric
chemistry,
but
knowledge
of
its
variation,
sources,
and
impact
on
sulfate
formation
remains
incomplete,
especially
the
urban
boundary
layer
aloft.
Here,
we
conducted
field
campaign
with
measurements
H2O2
related
species
at
tower-based
site
(∼528
m
above
ground
surface)
Beijing
spring
2022.
The
observed
hourly
concentration
reached
up
to
21.2
ppbv
an
average
value
3.4
±
3.7
during
entire
observation
period,
which
was
higher
than
values
from
previous
observations
throughout
world.
budget
revealed
that
two
known
sources
(self-reaction
HO2
radicals
ozonolysis
alkenes)
could
not
account
for
significant
H2O2,
leading
considerable
unknown
source
strength
(∼0.14–0.53
h–1)
noon
after
sunset.
Based
levoglucosan
signal,
distribution
fire
points,
backward
trajectories,
biomass
burning
emissions
southwest
(e.g.,
North
China
Plain)
were
found
contribute
greatly
formation.
Besides,
photochemical
aging
PM2.5
might
also
have
potential
production
noon.
unexpectedly
high
concentrations
aloft
made
vital
contribution
(0.2–1.1
μg
m–3
h–1),
be
transported
surface
turbulent
mixing.
Our
findings
provide
improved
understanding
chemistry
megacity,
as
well
