journal article
Open Access
Sep 21, 2018
Insights into HO x and RO x chemistry in the boreal forest via measurement of peroxyacetic acid, peroxyacetic nitric anhydride (PAN) and hydrogen peroxide
Abstract
Abstract. Unlike many oxidised atmospheric trace gases, which have numerous production
pathways, peroxyacetic acid (PAA) and PAN are formed almost exclusively in
gas-phase reactions involving the hydroperoxy radical (HO2), the
acetyl peroxy radical (CH3C(O)O2) and NO2 and are not
believed to be directly emitted in significant amounts by vegetation. As the
self-reaction of HO2 is the main photochemical route to hydrogen
peroxide (H2O2), simultaneous observation of PAA, PAN and
H2O2 can provide insight into the HO2 budget. We present
an analysis of observations taken during a summertime campaign in a boreal
forest that, in addition to natural conditions, was temporarily impacted by
two biomass-burning plumes. The observations were analysed using an
expression based on a steady-state assumption using relative PAA-to-PAN
mixing ratios to derive HO2 concentrations. The steady-state approach
generated HO2 concentrations that were generally in reasonable
agreement with measurements but sometimes overestimated those observed by
factors of 2 or more. We also used a chemically simple, constrained box model
to analyse the formation and reaction of radicals that define the observed
mixing ratios of PAA and H2O2. After nudging the simulation
towards observations by adding extra, photochemical sources of HO2
and CH3C(O)O2, the box model replicated the observations of
PAA, H2O2, ROOH and OH throughout the campaign, including the
biomass-burning-influenced episodes during which significantly higher levels
of many oxidized trace gases were observed. A dominant fraction of
CH3O2 radical generation was found to arise via reactions of
the CH3C(O)O2 radical. The model indicates that organic
peroxy radicals were present at night in high concentrations that sometimes
exceeded those predicted for daytime, and initially divergent measured and
modelled HO2 concentrations and daily concentration profiles are
reconciled when organic peroxy radicals are detected (as HO2) at an
efficiency of 35 %. Organic peroxy radicals are found to play an
important role in the recycling of OH radicals subsequent to their loss via
reactions with volatile organic compounds.
pathways, peroxyacetic acid (PAA) and PAN are formed almost exclusively in
gas-phase reactions involving the hydroperoxy radical (HO2), the
acetyl peroxy radical (CH3C(O)O2) and NO2 and are not
believed to be directly emitted in significant amounts by vegetation. As the
self-reaction of HO2 is the main photochemical route to hydrogen
peroxide (H2O2), simultaneous observation of PAA, PAN and
H2O2 can provide insight into the HO2 budget. We present
an analysis of observations taken during a summertime campaign in a boreal
forest that, in addition to natural conditions, was temporarily impacted by
two biomass-burning plumes. The observations were analysed using an
expression based on a steady-state assumption using relative PAA-to-PAN
mixing ratios to derive HO2 concentrations. The steady-state approach
generated HO2 concentrations that were generally in reasonable
agreement with measurements but sometimes overestimated those observed by
factors of 2 or more. We also used a chemically simple, constrained box model
to analyse the formation and reaction of radicals that define the observed
mixing ratios of PAA and H2O2. After nudging the simulation
towards observations by adding extra, photochemical sources of HO2
and CH3C(O)O2, the box model replicated the observations of
PAA, H2O2, ROOH and OH throughout the campaign, including the
biomass-burning-influenced episodes during which significantly higher levels
of many oxidized trace gases were observed. A dominant fraction of
CH3O2 radical generation was found to arise via reactions of
the CH3C(O)O2 radical. The model indicates that organic
peroxy radicals were present at night in high concentrations that sometimes
exceeded those predicted for daytime, and initially divergent measured and
modelled HO2 concentrations and daily concentration profiles are
reconciled when organic peroxy radicals are detected (as HO2) at an
efficiency of 35 %. Organic peroxy radicals are found to play an
important role in the recycling of OH radicals subsequent to their loss via
reactions with volatile organic compounds.
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Showing 50 of 107 references
Cited By
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Reaction between CH
3
C(O)OOH (peracetic acid) and OH in the gas phase: a combined experimental and theoretical study of the kinetics and mechanism
Atmospheric Chemistry and Physics
Matias Berasategui, Damien Amedro · 2020
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Details
- Published
- Sep 21, 2018
- Vol/Issue
- 18(18)
- Pages
- 13457-13479
- License
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Authors
Cite This Article
John N. Crowley, Nicolas Pouvesle, G. J. Phillips, et al. (2018). Insights into HO
x
and RO
x
chemistry in the boreal forest via measurement of peroxyacetic acid, peroxyacetic nitric anhydride (PAN) and hydrogen peroxide. Atmospheric Chemistry and Physics, 18(18), 13457-13479. https://doi.org/10.5194/acp-18-13457-2018
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