Environmental Science & Technology,
Год журнала:
2023,
Номер
57(48), С. 20085 - 20096
Опубликована: Ноя. 20, 2023
The
light
absorption
properties
of
brown
carbon
(BrC),
which
are
linked
to
molecular
chromophores,
may
play
a
significant
role
in
the
Earth's
energy
budget.
While
nitroaromatic
compounds
have
been
identified
as
strong
chromophores
wildfire-driven
BrC,
other
types
remain
be
investigated.
Given
electron-withdrawing
nature
carbonyls
ubiquitous
atmosphere,
we
characterized
carbonyl
BrC
samples
from
nighttime
oxidation
furan
and
pyrrole
derivatives,
important
but
understudied
precursors
secondary
organic
aerosols
primarily
found
wildfire
emissions.
Various
were
quantified
samples,
their
ultraviolet-visible
spectra
simulated
by
using
time-dependent
density
functional
theory.
Our
findings
suggest
that
with
bonded
nitrogen
(i.e.,
imides
amides)
derived
N-containing
heterocyclic
substantially
contribute
absorption.
contributed
over
40%
total
at
wavelengths
below
350
nm
above
430
BrC.
contributions
differed
significantly
wavelength,
highlighting
divergent
importance
different
wavelength
ranges.
Overall,
our
highlight
significance
underscore
need
for
further
investigation.
Journal of Geophysical Research Atmospheres,
Год журнала:
2022,
Номер
128(2)
Опубликована: Дек. 30, 2022
Abstract
The
NOAA/NASA
Fire
Influence
on
Regional
to
Global
Environments
and
Air
Quality
(FIREX‐AQ)
experiment
was
a
multi‐agency,
inter‐disciplinary
research
effort
to:
(a)
obtain
detailed
measurements
of
trace
gas
aerosol
emissions
from
wildfires
prescribed
fires
using
aircraft,
satellites
ground‐based
instruments,
(b)
make
extensive
suborbital
remote
sensing
fire
dynamics,
(c)
assess
local,
regional,
global
modeling
fires,
(d)
strengthen
connections
observables
the
ground
such
as
fuels
fuel
consumption
satellite
products
burned
area
radiative
power.
From
Boise,
ID
western
were
studied
with
NASA
DC‐8
two
NOAA
Twin
Otter
aircraft.
high‐altitude
ER‐2
deployed
Palmdale,
CA
observe
some
these
in
conjunction
overpasses
other
Further
conducted
three
mobile
laboratories
sites,
17
different
forecast
analyses
for
fire,
air
quality
climate
implications.
Salina,
KS
investigated
87
smaller
Southeast
in‐situ
data
collection.
Sampling
by
all
platforms
designed
measure
gases
aerosols
multiple
transects
capture
chemical
transformation
perform
observations
smoke
plumes
under
day
night
conditions.
linked
consumed
power
orbital
collected
during
overflights
sampling
fuels.
Atmospheric chemistry and physics,
Год журнала:
2024,
Номер
24(2), С. 929 - 956
Опубликована: Янв. 23, 2024
Abstract.
Extensive
airborne
measurements
of
non-methane
organic
gases
(NMOGs),
methane,
nitrogen
oxides,
reduced
species,
and
aerosol
emissions
from
US
wild
prescribed
fires
were
conducted
during
the
2019
NOAA/NASA
Fire
Influence
on
Regional
to
Global
Environments
Air
Quality
campaign
(FIREX-AQ).
Here,
we
report
atmospheric
enhancement
ratios
(ERs)
inferred
emission
factors
(EFs)
for
compounds
measured
board
NASA
DC-8
research
aircraft
nine
wildfires
one
fire,
which
encompass
a
range
vegetation
types.
We
use
photochemical
proxies
identify
young
smoke
reduce
effects
chemical
degradation
our
calculations.
ERs
EFs
calculated
FIREX-AQ
observations
agree
within
factor
2,
with
values
reported
previous
laboratory
field
studies
more
than
80
%
carbon-
nitrogen-containing
species.
Wildfire
are
parameterized
based
correlations
sum
NMOGs
reactive
oxides
(NOy)
modified
combustion
efficiency
(MCE)
as
well
other
signatures
indicative
flaming/smoldering
combustion,
including
carbon
monoxide
(CO),
dioxide
(NO2),
black
aerosol.
The
primary
NMOG
correlates
MCE
an
R2
0.68
slope
−296
±
51
g
kg−1,
consistent
studies.
mixing
CO
0.98
137
4
ppbv
per
parts
million
by
volume
(ppmv)
CO,
demonstrating
that
can
be
estimated
CO.
Individual
species
correlate
better
NO2,
NOy,
More
half
NOy
in
fresh
plumes
is
NO2
0.95
ratio
0.55
0.05
ppbv−1,
highlighting
fast
photochemistry
had
already
occurred
sampled
fire
plumes.
follows
trends
observed
experiments
increases
exponentially
MCE,
due
increased
key
at
higher
flaming
combustion.
These
parameterizations
will
provide
accurate
boundary
conditions
modeling
satellite
plume
chemistry
evolution
predict
downwind
formation
secondary
pollutants,
ozone
ACS ES&T Air,
Год журнала:
2024,
Номер
1(3), С. 200 - 222
Опубликована: Фев. 21, 2024
The
Alaskan
Layered
Pollution
And
Chemical
Analysis
(ALPACA)
field
experiment
was
a
collaborative
study
designed
to
improve
understanding
of
pollution
sources
and
chemical
processes
during
winter
(cold
climate
low-photochemical
activity),
investigate
indoor
pollution,
dispersion
as
affected
by
frequent
temperature
inversions.
A
number
the
research
goals
were
motivated
questions
raised
residents
Fairbanks,
Alaska,
where
held.
This
paper
describes
measurement
strategies
conditions
encountered
January
February
2022
experiment,
reports
early
examples
how
measurements
addressed
goals,
particularly
those
interest
residents.
Outdoor
air
showed
high
concentrations
particulate
matter
pollutant
gases
including
volatile
organic
carbon
species.
During
events,
low
winds
extremely
stable
atmospheric
trapped
below
73
m,
an
shallow
vertical
scale.
Tethered-balloon-based
intercepted
plumes
aloft,
which
associated
with
power
plant
point
through
transport
modeling.
Because
cold
spend
much
their
time
indoors,
included
quality
component,
made
inside
outside
house
infiltration
sources.
In
absence
activities
such
cooking
and/or
heating
pellet
stove,
lower
than
outdoors;
however,
stove
burns
often
caused
higher
outdoors.
mass-normalized
oxidative
potential,
health-relevant
property
measured
here
reactivity
dithiothreiol,
particles
varied
source,
having
less
potential
per
mass
particles.
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%).
Journal of Geophysical Research Atmospheres,
Год журнала:
2021,
Номер
126(15)
Опубликована: Июль 16, 2021
Abstract
Biomass
burning
(BB)
produces
large
quantities
of
carbonaceous
aerosol
(black
carbon
and
organic
aerosol,
BC
OA,
respectively),
which
significantly
degrade
air
quality
impact
climate.
absorbs
radiation,
warming
the
atmosphere,
while
OA
typically
scatters
leading
to
cooling.
However,
some
termed
brown
(BrC),
also
visible
near
UV
radiation;
although,
its
properties
are
not
well
constrained.
We
explore
three
aircraft
campaigns
from
important
BB
regions
with
different
dominant
fuel
fire
types
(Western
Wildfire
Experiment
for
Cloud
Chemistry,
Aerosol
Absorption,
Nitrogen
[WE‐CAN]
in
western
United
States
ObseRvations
Aerosols
above
CLouds
their
intEractionS
Cloud‐Aerosol‐Radiation
Interactions
Forcing
Year
downwind
southern
Africa)
compare
them
simulations
global
chemical
transport
model,
GEOS‐Chem
using
GFED4s.
The
model
generally
captures
observed
vertical
profiles
concentrations;
however,
we
find
that
emissions
underestimated
Africa.
Our
comparisons
suggest
and/or
BrC
absorption
is
substantially
higher
Africa
than
and,
Saleh
et
al.
(2014,
https://doi.org/10.1038/ngeo2220
)
FIREX
parameterizations
based
on
BC:OA
ratio
improve
model‐observation
agreement
regions,
they
do
sufficiently
differentiate
characteristics
at
short
wavelengths.
photochemical
whitening
decreases
burden
direct
radiative
effect
(annual
mean
+0.29
W
m
−2
without
+0.08
with).
required
explain
WE‐CAN
observations;
importance
African
fires
cannot
be
confirmed.
Qualitative
OMI
index
our
standard
scheme
may
too
fast
over
Journal of Geophysical Research Atmospheres,
Год журнала:
2022,
Номер
127(2)
Опубликована: Янв. 10, 2022
Abstract
Biomass
burning
(BB)
events
are
occurring
globally
with
increasing
frequency,
and
their
emissions
having
more
impacts
on
human
health
climate.
Large
ash
particles
recognized
as
a
BB
product
major
influences
soil
water
environments.
However,
fine‐ash
particles,
which
have
diameters
smaller
than
several
microns
characteristic
morphologies
compositions
(mainly
Ca
Mg
carbonates),
not
yet
been
explicitly
considered
aerosol
component
either
in
field
observations
or
climate
models.
This
study
measured
samples
using
transmission
electron
microscopy
(TEM)
ion
chromatography
during
the
Fire
Influence
Regional
to
Global
Environments
Air
Quality
(FIREX‐AQ)
campaign.
We
show
that
significant
amounts
of
fine
ash‐bearing
transported
>100
km
from
fire
sources.
Our
environmental
chamber
experiments
suggest
they
can
act
cloud
condensation
ice
nuclei.
also
found
considerable
TEM
collected
previous
campaigns
(Biomass
Burning
Observation
Project
Megacity
Initiative:
Local
Research
Observations).
These
commonly
mixed
organic
matter
make
up
∼8%
5%
smoke
by
number
mass,
respectively,
FIREX‐AQ
The
ash‐mass
concentrations
approximately
five
times
six
greater
those
black
carbon
potassium,
scaling
an
estimated
global
emission
11.6
Tg
yr
−1
range
8.8–16.3
.
Better
characterization
constraints
these
will
improve
measurements
strengthen
assessments
Environmental Science & Technology,
Год журнала:
2022,
Номер
56(12), С. 7564 - 7577
Опубликована: Май 17, 2022
Carbonaceous
emissions
from
wildfires
are
a
dynamic
mixture
of
gases
and
particles
that
have
important
impacts
on
air
quality
climate.
Emissions
feed
atmospheric
models
estimated
using
burned
area
fire
radiative
power
(FRP)
methods
rely
satellite
products.
These
approaches
show
wide
variability
large
uncertainties,
their
accuracy
is
challenging
to
evaluate
due
limited
aircraft
ground
measurements.
Here,
we
present
novel
method
estimate
plume-integrated
total
carbon
speciated
emission
rates
unique
combination
lidar
remote
sensing
aerosol
extinction
profiles
in
situ
measured
constituents.
We
strong
agreement
between
these
aircraft-derived
detailed
area-based
inventory
distributes
time
Geostationary
Operational
Environmental
Satellite
FRP
observations
(Fuel2Fire
inventory,
slope
=
1.33
±
0.04,
r2
0.93,
RMSE
0.27).
Other
more
commonly
used
inventories
strongly
correlate
with
but
wide-ranging
over-
under-predictions.
A
correlation
found
monoxide
those
derived
the
TROPOspheric
Monitoring
Instrument
(TROPOMI)
for
five
coincident
sampling
windows
(slope
0.99
0.18;
bias
28.5%).
Smoke
coefficients
(g
MJ–1)
enable
direct
estimations
primary
gas
observations,
derive
values
many
compounds
emitted
by
temperate
forest
fuels,
including
several
previously
unreported
species.
Environmental Science & Technology,
Год журнала:
2022,
Номер
56(6), С. 3645 - 3657
Опубликована: Март 1, 2022
Wildfire-influenced
air
masses
under
regional
background
conditions
were
characterized
at
the
Mt.
Bachelor
Observatory
(∼2800
m
a.s.l.)
in
summer
2019
to
provide
a
better
understanding
of
aging
biomass
burning
organic
aerosols
(BBOAs)
and
their
impacts
on
remote
troposphere
western
United
States.
Submicron
aerosol
(PM1)
concentrations
low
(average
±
1σ
=
2.2
1.9
μg
sm–3),
but
oxidized
BBOAs
O/C
0.84)
constantly
detected
throughout
study.
The
BBOA
correlated
well
with
black
carbon,
furfural,
acetonitrile
comprised
above
50%
PM1
during
plume
events
when
peak
concentration
reached
18.0
sm–3.
Wildfire
plumes
estimated
transport
times
varying
from
∼10
h
>10
days
identified.
showed
ΔOA/ΔCO
values
ranging
0.038
0.122
ppb
ppb–1
significant
negative
relation
age,
indicating
loss
relative
CO
long-range
transport.
Additionally,
increases
average
sizes
seen
more
aged
plumes.
mass-based
size
mode
was
approximately
700
nm
(Dva)
most
that
likely
originated
Siberia,
suggesting
aqueous-phase
processing
This
work
highlights
widespread
wildfire
emissions
have
properties,
thus
climate,
Environmental Science & Technology,
Год журнала:
2023,
Номер
57(39), С. 14648 - 14660
Опубликована: Сен. 13, 2023
The
frequency
of
wildfires
in
the
western
United
States
has
escalated
recent
decades.
Here
we
examine
impacts
on
ground-level
ozone
(O3)
precursors
and
O3-NOx-VOC
chemistry
from
source
to
downwind
urban
areas.
We
use
satellite
retrievals
nitrogen
dioxide
(NO2)
formaldehyde
(HCHO,
an
indicator
VOC)
Tropospheric
Monitoring
Instrument
(TROPOMI)
track
evolution
O3
over
California
2018
2020.
improved
these
by
updating
a
priori
profiles
explicitly
accounting
for
effects
smoke
aerosols.
TROPOMI
observations
reveal
that
extensive
intense
fire
2020
led
overall
increase
statewide
annual
average
HCHO
NO2
columns
16%
9%.
level
offsets
anthropogenic
NOx
emission
reduction
COVID-19
lockdown.
enhancement
within
plumes
is
concentrated
near
regions
actively
burning,
whereas
far-reaching,
extending
areas
due
secondary
production
longer-lived
VOCs
such
as
ethene.
Consequently,
larger
occurs
NOx-limited
regions,
while
greater
VOC-limited
areas,
both
contributing
more
efficient
production.
Wildfires
are
increasing
in
frequency,
raising
concerns
that
smoke
can
permeate
indoor
environments
and
expose
people
to
chemical
air
contaminants.
To
study
transformations
evaluate
mitigation
strategies,
we
added
a
test
house.
Many
volatile
organic
compounds
(VOCs)
persisted
days
following
the
injection,
providing
longer-term
exposure
pathway
for
humans.
Two
time
scales
control
VOC
partitioning:
faster
one
(1.0
5.2
hours)
describes
reach
equilibrium
between
adsorption
desorption
processes
slower
(4.8
21.2
ventilation
overtake
adsorption-desorption
equilibria
controlling
concentration.
These
rates
imply
vapor
pressure
controls
partitioning
behavior
house
plays
minor
role
removing
VOCs.
However,
surface
cleaning
activities
(vacuuming,
mopping,
dusting)
physically
removed
reservoirs
thus
reduced
concentrations
more
effectively
than
portable
cleaners
persistently
window
opening.