Environmental Science & Technology,
Год журнала:
2022,
Номер
56(24), С. 17569 - 17580
Опубликована: Дек. 6, 2022
Tropospheric
ozone
(O3)
is
a
harmful
gas
compound
to
humans
and
vegetation,
it
also
serves
as
climate
change
forcer.
O3
formed
in
the
reactions
of
nitrogen
oxides
volatile
organic
compounds
(VOCs)
with
light.
In
this
study,
an
pollution
episode
encountered
Shenzhen,
South
China
2018
was
investigated
illustrate
influence
aerosols
on
local
production.
We
used
box
model
comprehensive
heterogeneous
mechanisms
empirical
prediction
photolysis
rates
reproduce
episode.
Results
demonstrate
that
aerosol
light
extinction
NO2
showed
comparable
but
opposite
signs
Hence,
from
different
processes
largely
counteracted.
Sensitivity
tests
suggest
production
increases
further
reduction
while
continued
NOx
finally
shifts
NOx-limited
regime
respect
traditional
O3-NOx-VOC
sensitivity.
Our
results
shed
role
highlight
mitigation
not
only
limiting
helping
ease
particulate
nitrate,
path
for
cocontrol
fine
particle
pollution.
Atmospheric measurement techniques,
Год журнала:
2020,
Номер
13(10), С. 5441 - 5458
Опубликована: Окт. 13, 2020
Abstract.
The
PurpleAir
PA-II
unit
is
a
low-cost
sensor
for
monitoring
changes
in
the
concentrations
of
particulate
matter
(PM)
various
sizes.
There
are
currently
more
than
10
000
units
use
worldwide;
some
located
areas
where
no
other
reference
air
system
present.
Previous
studies
have
examined
performance
these
(or
sensors
within
them)
comparison
to
co-located
system.
However,
because
installed
by
customers,
most
not
with
and,
many
cases,
near
one.
This
study
aims
examine
how
each
performs
under
atmospheric
conditions
when
exposed
variety
pollutants
and
PM2.5
(PM
an
aerodynamic
diameter
smaller
2.5
µm),
at
distance
from
sensor.
We
perform
Environmental
Protection
Agency
(EPA)
Air
Quality
Monitoring
Stations
(AQMSs)
that
them.
For
this
study,
we
selected
four
different
regions,
containing
multiple
(minimum
seven
per
region).
In
addition,
region
needed
least
one
AQMS
was
unit,
all
be
up
5
km
between
other.
Correction
values
implemented
multivariate
linear
regression
(MLR),
taking
into
account
temperature
relative
humidity.
fit
coefficients,
received
MLR,
were
then
used
correct
remaining
region.
Hourly
measurements
compared
those
AQMSs
its
correction
improved
R-squared
value
(R2),
root-mean-square
error
(RMSE),
mean
absolute
(MAE)
slope
units.
found
good
agreement
(75
%
comparisons
had
R2>0.8);
they
measured
similar
followed
trends;
is,
increased
or
decreased,
so
did
high-pollution
events,
corrected
slightly
higher
AQMS.
Distance
impact
Overall,
after
corrections
values,
seems
promising
tool
identifying
concentration
potential
complement
sparsely
distributed
stations
aid
assessing
minimizing
public
exposure
PM.
Environmental Science & Technology,
Год журнала:
2020,
Номер
54(14), С. 8589 - 8600
Опубликована: Июнь 17, 2020
Efficient
prediction
of
the
air
quality
response
to
emission
changes
is
a
prerequisite
for
an
integrated
assessment
system
in
developing
effective
control
policies.
Yet,
representing
nonlinear
controls
with
accuracy
remains
major
barrier
quality-related
decision
making.
Here,
we
demonstrate
novel
method
that
combines
deep
learning
approaches
chemical
indicators
pollutant
formation
quickly
estimate
coefficients
functions
using
ambient
concentrations
18
simulated
comprehensive
atmospheric
transport
model
(CTM).
By
requiring
only
two
CTM
simulations
application,
new
significantly
enhances
computational
efficiency
compared
existing
methods
achieve
lower
despite
20+
(the
benchmark
statistical
model).
Our
results
utility
capturing
nonlinearity
chemistry
and
physics
prospects
support
policymaking
other
environment
systems.
Journal of Geophysical Research Atmospheres,
Год журнала:
2021,
Номер
126(9)
Опубликована: Апрель 24, 2021
Abstract
Studies
of
wintertime
air
quality
in
the
North
China
Plain
(NCP)
show
that
particulate‐nitrate
pollution
persists
despite
rapid
reduction
NO
x
emissions.
This
intriguing
‐nitrate
relationship
may
originate
from
non‐linear
nitrate‐formation
chemistry,
but
it
is
unclear
which
feedback
mechanisms
dominate
NCP.
In
this
study,
we
re‐interpret
observations
17
O
excess
nitrate
(∆
O(NO
3
−
))
Beijing
using
GEOS‐Chem
(GC)
chemical
transport
model
to
estimate
importance
various
nitrate‐production
pathways
and
how
their
contributions
change
with
intensity
haze
events.
We
also
analyze
relationships
between
other
metrics
y
chemistry
[PM
2.5
]
simulations.
find
on
average
has
a
negative
bias
−0.9‰
−36%
for
∆
)
[O
x,major
(≡
+
[NO
2
[p‐NO
]),
respectively,
while
overestimating
nitrogen
oxidation
ratio
([NO
]/([NO
]))
by
+0.12
intense
haze.
The
discrepancies
become
larger
more
attribute
biases
an
overestimate
‐uptake
aerosols
underestimate
concentrations.
Our
findings
highlight
need
address
uncertainties
related
heterogeneous
air‐quality
models.
combined
assessment
results
suggest
N
5
uptake
clouds
dominant
pathway
Beijing,
its
rate
limited
ozone
under
high‐NO
‐high‐PM
conditions.
Nitrate
production
rates
continue
increase
as
long
increases
],
creating
reduces
effectiveness
mitigation.
Environmental Science & Technology,
Год журнала:
2021,
Номер
55(15), С. 10280 - 10290
Опубликована: Июль 13, 2021
Understanding
the
efficiency
and
variability
of
photochemical
ozone
(O3)
production
from
western
wildfire
plumes
is
important
to
accurately
estimate
their
influence
on
North
American
air
quality.
A
set
measurements
were
made
NOAA
Twin
Otter
research
aircraft
as
a
part
Fire
Influence
Regional
Global
Environments
Air
Quality
(FIREX-AQ)
experiment.
We
use
zero-dimensional
(0-D)
box
model
investigate
chemistry
driving
O3
in
modeled
plumes.
Modeled
afternoon
reached
maximum
mixing
ratio
140
±
50
ppbv
(average
standard
deviation)
within
20
10
min
emission
compared
76
12
60
30
evening
Afternoon
isopleths
indicate
that
near
peak
NOx
efficiency.
radical
budget
describes
volatile
-
organic
compound
(VOC)
sensitivities
these
displayed
rapid
transition
VOC-sensitive
NOx-sensitive
chemistry,
driven
by
HOx
(=OH
+
HO2)
photolysis
nitrous
acid
(HONO)
(48
20%
primary
HOx)
formaldehyde
(HCHO)
(26
9%)
emitted
directly
fire.
Evening
exhibit
slower
caused
reduction
rates
fire
emissions.
controlled
HONO
(53
7%),
HCHO
(18
9%),
alkene
ozonolysis
(17
9%).
Atmospheric chemistry and physics,
Год журнала:
2022,
Номер
22(6), С. 4117 - 4128
Опубликована: Март 30, 2022
Abstract.
Volatile
organic
compounds
(VOCs)
regulate
atmospheric
oxidation
capacity,
and
the
reactions
of
VOCs
are
key
in
understanding
ozone
formation
its
mitigation
strategies.
When
evaluating
their
impact,
most
previous
studies
did
not
fully
consider
role
oxygenated
due
to
limitations
measurement
technology.
By
using
a
proton-transfer-reaction
time-of-flight
mass
spectrometer
(PTR-ToF-MS)
combined
with
gas
chromatograph–mass
(GC–MS),
large
number
(OVOCs)
have
been
quantified
Guangzhou
city,
China.
Based
on
new
dataset,
we
demonstrate
that
constraints
OVOC
observations
essential
modeling
radical
production,
as
modeled
OVOCs
can
be
substantially
lower
than
measurements,
potentially
primary
emissions
and/or
missing
secondary
sources.
Non-formaldehyde
(HCHO)
contribute
fractions
(22
%–44
%)
total
ROx
which
comparable
or
larger
contributions
from
nitrous
acid
formaldehyde.
Our
results
show
models
without
ambient
measurements
will
underestimate
production
rates
ozone,
they
may
also
affect
determination
sensitivity
regime
formation.
Therefore,
thorough
quantification
photodegradable
species
is
urgent
need
understand
accurately
chemistry
develop
effective
control
Atmospheric chemistry and physics,
Год журнала:
2021,
Номер
21(12), С. 9309 - 9327
Опубликована: Июнь 17, 2021
Abstract.
Air
pollution
is
one
of
the
main
causes
damages
to
human
health
in
Europe,
with
an
estimate
about
380
000
premature
deaths
per
year
EU28,
as
result
exposure
fine
particulate
matter
(PM2.5)
only.
In
this
work,
we
focus
on
specific
region
Po
basin,
a
where
chemical
regimes
are
most
complex,
showing
important
non-linear
processes,
especially
those
related
interactions
between
NOx
and
NH3.
We
analyse
sensitivity
PM2.5
concentration
NH3
emissions
by
means
set
EMEP
model
simulations
performed
different
levels
emission
reductions,
from
25
%
up
total
switch-off
emissions.
Both
single
combined
precursor
reduction
scenarios
applied
determine
efficient
strategies
quantify
reductions.
The
results
confirmed
peculiarity
secondary
formation
characterised
contrasting
within
distances
few
(hundred)
kilometres,
well
responses
reductions
during
wintertime.
One
striking
slight
increase
when
NOx-rich
areas,
such
surroundings
Bergamo.
increased
oxidative
capacity
atmosphere
cause
induced
emission.
This
process
could
have
contributed
absence
significant
decrease
COVID-19
lockdowns
many
European
cities.
It
account
for
designing
air
quality
plans,
since
it
lead
transitionary
increases
at
some
locations
winter
measures
gradually
implemented.
While
regimes,
determined
relative
importance
vs.
show
large
variations
seasonally
spatially,
they
not
very
sensitive
moderate
(up
50
%–60
%)
Beyond
strength,
concentrations
become
certain
areas
basin
mainly
Atmospheric chemistry and physics,
Год журнала:
2023,
Номер
23(9), С. 5043 - 5099
Опубликована: Май 4, 2023
Abstract.
Chemical
mechanisms
describe
the
atmospheric
transformations
of
organic
and
inorganic
species
connect
air
emissions
to
secondary
such
as
ozone,
fine
particles,
hazardous
pollutants
(HAPs)
like
formaldehyde.
Recent
advances
in
our
understanding
several
chemical
systems
shifts
drivers
chemistry
warrant
updates
used
transport
models
Community
Multiscale
Air
Quality
(CMAQ)
modeling
system.
This
work
builds
on
Regional
Atmospheric
Chemistry
Mechanism
version
2
(RACM2)
develops
Multiphase
(CRACMM)
1.0,
which
demonstrates
a
fully
coupled
representation
leading
ozone
aerosol
(SOA)
with
consideration
HAPs.
CRACMMv1.0
includes
178
gas-phase
species,
51
particulate
508
reactions
spanning
heterogeneous
pathways.
To
support
estimation
health
risks
associated
HAPs,
nine
CRACMM
cover
50
%
total
cancer
60
non-cancer
emission-weighted
toxicity
estimated
for
primary
HAPs
from
anthropogenic
biomass
burning
sources
US,
coverage
higher
(>
80
%)
when
formaldehyde
acrolein
are
considered.
In
addition,
new
mechanism
were
added
based
importance
their
aerosol,
or
burden
reactive
carbon
(ROC):
sesquiterpenes,
furans,
propylene
glycol,
alkane-like
low-
intermediate-volatility
compounds
(9
species),
oxygenated
(16
aromatic
hydrocarbons
(2
slowly
reacting
carbon.
Intermediate-
lower-volatility
increase
ROC
by
40
compared
current
operational
mechanisms.
Autoxidation,
reaction
particularly
effective
producing
SOA,
was
C10
larger
alkanes,
hydrocarbons,
monoterpene
including
second-generation
aldehydes.
Integrating
radical
SOA
put
additional
constraints
both
enabled
implementation
previously
unconsidered
pathways
phenolic
furanone
compounds,
predicted
account
∼
30
hydrocarbon
under
typical
conditions.
found
span
atmospherically
relevant
range
number,
number
oxygens
per
carbon,
oxidation
state
slight
high
bias
hydrogens
total,
11
emitted
implemented
precursors
CMAQv5.3.3
representations,
resulting
bottom-up
prediction
is
required
accurate
source
attribution
design
control
strategies.
available
CMAQv5.4.
npj Climate and Atmospheric Science,
Год журнала:
2023,
Номер
6(1)
Опубликована: Май 30, 2023
Abstract
Atmospheric
nitrous
acid
(HONO)
chemistry
is
of
critical
importance
to
air
quality
during
polluted
haze
events,
especially
in
China.
However,
current
models
(such
as
WRF-CHEM,
WRF-CMAQ,
Box-MCM)
generally
underestimate
the
concentration
HONO,
leading
a
lack
fundamental
understanding
pollution.
Here,
by
combining
field
observations
events
Beijing
and
modeling
results,
we
developed
new
parameterization
scheme
for
heterogeneous
nitrogen
dioxide
(NO
2
)
reaction
on
aerosol
surfaces
with
synergistic
effects
relative
humidity
ammonia,
which
has
not
been
considered
existing
models.
Including
NO
reactions
into
significantly
improves
estimation
accuracy
HONO
OH
levels,
contribution
reaching
up
91%
78%
pollution
episodes.
The
derived
can
partly
explain
high
concentrations
particulate
matter.
Together,
our
work
provides
approach
illustrate
formation
OH,
consideration
→
chemistry.