In situ measurements and modeling of reactive trace gases in a small biomass burning plume
An instrumented NASA P-3B aircraft was used for airborne sampling of trace gases in a plume that had emanated from a small forest understory fire in Georgia, USA. The plume was sampled at its origin to derive emission factors and followed ∼ 13.6 km downwind to observe chemical changes during th...
Main Authors: | , , , , , , , , , , , , , , |
---|---|
Format: | Article |
Language: | English |
Published: |
Copernicus Publications
2016-03-01
|
Series: | Atmospheric Chemistry and Physics |
Online Access: | https://www.atmos-chem-phys.net/16/3813/2016/acp-16-3813-2016.pdf |
id |
doaj-68f4224f61a34ef3af2209f6030c9d72 |
---|---|
record_format |
Article |
collection |
DOAJ |
language |
English |
format |
Article |
sources |
DOAJ |
author |
M. Müller M. Müller B. E. Anderson A. J. Beyersdorf J. H. Crawford G. S. Diskin P. Eichler A. Fried F. N. Keutsch T. Mikoviny K. L. Thornhill K. L. Thornhill J. G. Walega A. J. Weinheimer M. Yang R. J. Yokelson A. Wisthaler A. Wisthaler |
spellingShingle |
M. Müller M. Müller B. E. Anderson A. J. Beyersdorf J. H. Crawford G. S. Diskin P. Eichler A. Fried F. N. Keutsch T. Mikoviny K. L. Thornhill K. L. Thornhill J. G. Walega A. J. Weinheimer M. Yang R. J. Yokelson A. Wisthaler A. Wisthaler In situ measurements and modeling of reactive trace gases in a small biomass burning plume Atmospheric Chemistry and Physics |
author_facet |
M. Müller M. Müller B. E. Anderson A. J. Beyersdorf J. H. Crawford G. S. Diskin P. Eichler A. Fried F. N. Keutsch T. Mikoviny K. L. Thornhill K. L. Thornhill J. G. Walega A. J. Weinheimer M. Yang R. J. Yokelson A. Wisthaler A. Wisthaler |
author_sort |
M. Müller |
title |
In situ measurements and modeling of reactive trace gases in a small biomass burning plume |
title_short |
In situ measurements and modeling of reactive trace gases in a small biomass burning plume |
title_full |
In situ measurements and modeling of reactive trace gases in a small biomass burning plume |
title_fullStr |
In situ measurements and modeling of reactive trace gases in a small biomass burning plume |
title_full_unstemmed |
In situ measurements and modeling of reactive trace gases in a small biomass burning plume |
title_sort |
in situ measurements and modeling of reactive trace gases in a small biomass burning plume |
publisher |
Copernicus Publications |
series |
Atmospheric Chemistry and Physics |
issn |
1680-7316 1680-7324 |
publishDate |
2016-03-01 |
description |
An instrumented NASA P-3B aircraft was used for airborne sampling of trace
gases in a plume that had emanated from a small forest understory fire in
Georgia, USA. The plume was sampled at its origin to derive emission
factors and followed ∼ 13.6 km downwind to observe chemical changes
during the first hour of atmospheric aging. The P-3B payload included a
proton-transfer-reaction time-of-flight mass spectrometer (PTR-ToF-MS),
which measured non-methane organic gases (NMOGs) at unprecedented
spatiotemporal resolution (10 m spatial/0.1 s temporal). Quantitative emission data are
reported for CO<sub>2</sub>, CO, NO, NO<sub>2</sub>, HONO, NH<sub>3</sub>, and 16 NMOGs
(formaldehyde, methanol, acetonitrile, propene, acetaldehyde, formic acid,
acetone plus its isomer propanal, acetic acid plus its isomer
glycolaldehyde, furan, isoprene plus isomeric pentadienes and cyclopentene,
methyl vinyl ketone plus its isomers crotonaldehyde and methacrolein,
methylglyoxal, hydroxy acetone plus its isomers methyl acetate and propionic
acid, benzene, 2,3-butanedione, and 2-furfural) with molar emission ratios
relative to CO larger than 1 ppbV ppmV<sup>−1</sup>. Formaldehyde, acetaldehyde,
2-furfural, and methanol dominated NMOG emissions. No NMOGs with more than 10
carbon atoms were observed at mixing ratios larger than 50 pptV ppmV<sup>−1</sup> CO.
Downwind plume chemistry was investigated using the observations
and a 0-D photochemical box model simulation. The model was run on a
nearly explicit chemical mechanism (MCM v3.3) and initialized with measured
emission data. Ozone formation during the first hour of atmospheric aging
was well captured by the model, with carbonyls (formaldehyde, acetaldehyde,
2,3-butanedione, methylglyoxal, 2-furfural) in addition to CO and CH<sub>4</sub>
being the main drivers of peroxy radical chemistry. The model also
accurately reproduced the sequestration of NO<sub><i>x</i></sub> into peroxyacetyl nitrate (PAN) and the
OH-initiated degradation of furan and 2-furfural at an average OH
concentration of 7.45 ± 1.07 × 10<sup>6</sup> cm<sup>−3</sup> in the plume.
Formaldehyde, acetone/propanal,
acetic acid/glycolaldehyde, and maleic
acid/maleic anhydride (tentatively identified) were found to be the main
NMOGs to increase during 1 h of atmospheric plume processing, with the
model being unable to capture the observed increase. A mass balance analysis
suggests that about 50 % of the aerosol mass formed in the downwind plume
is organic in nature. |
url |
https://www.atmos-chem-phys.net/16/3813/2016/acp-16-3813-2016.pdf |
work_keys_str_mv |
AT mmuller insitumeasurementsandmodelingofreactivetracegasesinasmallbiomassburningplume AT mmuller insitumeasurementsandmodelingofreactivetracegasesinasmallbiomassburningplume AT beanderson insitumeasurementsandmodelingofreactivetracegasesinasmallbiomassburningplume AT ajbeyersdorf insitumeasurementsandmodelingofreactivetracegasesinasmallbiomassburningplume AT jhcrawford insitumeasurementsandmodelingofreactivetracegasesinasmallbiomassburningplume AT gsdiskin insitumeasurementsandmodelingofreactivetracegasesinasmallbiomassburningplume AT peichler insitumeasurementsandmodelingofreactivetracegasesinasmallbiomassburningplume AT afried insitumeasurementsandmodelingofreactivetracegasesinasmallbiomassburningplume AT fnkeutsch insitumeasurementsandmodelingofreactivetracegasesinasmallbiomassburningplume AT tmikoviny insitumeasurementsandmodelingofreactivetracegasesinasmallbiomassburningplume AT klthornhill insitumeasurementsandmodelingofreactivetracegasesinasmallbiomassburningplume AT klthornhill insitumeasurementsandmodelingofreactivetracegasesinasmallbiomassburningplume AT jgwalega insitumeasurementsandmodelingofreactivetracegasesinasmallbiomassburningplume AT ajweinheimer insitumeasurementsandmodelingofreactivetracegasesinasmallbiomassburningplume AT myang insitumeasurementsandmodelingofreactivetracegasesinasmallbiomassburningplume AT rjyokelson insitumeasurementsandmodelingofreactivetracegasesinasmallbiomassburningplume AT awisthaler insitumeasurementsandmodelingofreactivetracegasesinasmallbiomassburningplume AT awisthaler insitumeasurementsandmodelingofreactivetracegasesinasmallbiomassburningplume |
_version_ |
1725964345737740288 |
spelling |
doaj-68f4224f61a34ef3af2209f6030c9d722020-11-24T21:30:02ZengCopernicus PublicationsAtmospheric Chemistry and Physics1680-73161680-73242016-03-01163813382410.5194/acp-16-3813-2016In situ measurements and modeling of reactive trace gases in a small biomass burning plumeM. Müller0M. Müller1B. E. Anderson2A. J. Beyersdorf3J. H. Crawford4G. S. Diskin5P. Eichler6A. Fried7F. N. Keutsch8T. Mikoviny9K. L. Thornhill10K. L. Thornhill11J. G. Walega12A. J. Weinheimer13M. Yang14R. J. Yokelson15A. Wisthaler16A. Wisthaler17Institute of Ion Physics and Applied Physics, University of Innsbruck, Innsbruck, AustriaDepartment of Chemistry, University of Montana, Missoula, MT, USANASA Langley Research Center, Hampton, VA, USANASA Langley Research Center, Hampton, VA, USANASA Langley Research Center, Hampton, VA, USANASA Langley Research Center, Hampton, VA, USAInstitute of Ion Physics and Applied Physics, University of Innsbruck, Innsbruck, AustriaInstitute of Arctic and Alpine Research, University of Colorado, Boulder, CO, USASchool of Engineering and Applied Sciences, Department of Chemistry and Chemical Biology, Harvard University, Cambridge, MA, USADepartment of Chemistry, University of Oslo, Oslo, NorwayNASA Langley Research Center, Hampton, VA, USAScience Systems and Applications, Inc., Hampton, VA, USAInstitute of Arctic and Alpine Research, University of Colorado, Boulder, CO, USAAtmospheric Chemistry Observations and Modeling Laboratory, National Center for Atmospheric Research, Boulder, CO, USANASA Langley Research Center, Hampton, VA, USADepartment of Chemistry, University of Montana, Missoula, MT, USAInstitute of Ion Physics and Applied Physics, University of Innsbruck, Innsbruck, AustriaDepartment of Chemistry, University of Oslo, Oslo, NorwayAn instrumented NASA P-3B aircraft was used for airborne sampling of trace gases in a plume that had emanated from a small forest understory fire in Georgia, USA. The plume was sampled at its origin to derive emission factors and followed ∼ 13.6 km downwind to observe chemical changes during the first hour of atmospheric aging. The P-3B payload included a proton-transfer-reaction time-of-flight mass spectrometer (PTR-ToF-MS), which measured non-methane organic gases (NMOGs) at unprecedented spatiotemporal resolution (10 m spatial/0.1 s temporal). Quantitative emission data are reported for CO<sub>2</sub>, CO, NO, NO<sub>2</sub>, HONO, NH<sub>3</sub>, and 16 NMOGs (formaldehyde, methanol, acetonitrile, propene, acetaldehyde, formic acid, acetone plus its isomer propanal, acetic acid plus its isomer glycolaldehyde, furan, isoprene plus isomeric pentadienes and cyclopentene, methyl vinyl ketone plus its isomers crotonaldehyde and methacrolein, methylglyoxal, hydroxy acetone plus its isomers methyl acetate and propionic acid, benzene, 2,3-butanedione, and 2-furfural) with molar emission ratios relative to CO larger than 1 ppbV ppmV<sup>−1</sup>. Formaldehyde, acetaldehyde, 2-furfural, and methanol dominated NMOG emissions. No NMOGs with more than 10 carbon atoms were observed at mixing ratios larger than 50 pptV ppmV<sup>−1</sup> CO. Downwind plume chemistry was investigated using the observations and a 0-D photochemical box model simulation. The model was run on a nearly explicit chemical mechanism (MCM v3.3) and initialized with measured emission data. Ozone formation during the first hour of atmospheric aging was well captured by the model, with carbonyls (formaldehyde, acetaldehyde, 2,3-butanedione, methylglyoxal, 2-furfural) in addition to CO and CH<sub>4</sub> being the main drivers of peroxy radical chemistry. The model also accurately reproduced the sequestration of NO<sub><i>x</i></sub> into peroxyacetyl nitrate (PAN) and the OH-initiated degradation of furan and 2-furfural at an average OH concentration of 7.45 ± 1.07 × 10<sup>6</sup> cm<sup>−3</sup> in the plume. Formaldehyde, acetone/propanal, acetic acid/glycolaldehyde, and maleic acid/maleic anhydride (tentatively identified) were found to be the main NMOGs to increase during 1 h of atmospheric plume processing, with the model being unable to capture the observed increase. A mass balance analysis suggests that about 50 % of the aerosol mass formed in the downwind plume is organic in nature.https://www.atmos-chem-phys.net/16/3813/2016/acp-16-3813-2016.pdf |