An improved representation of fire non-methane organic gases (NMOGs) in models: emissions to reactivity

<jats:p>Abstract. Fires emit a substantial amount of non-methane organic gases (NMOGs), the atmospheric oxidation of which can contribute to ozone and secondary particulate matter formation. However, the abundance and reactivity of these fire NMOGs are uncertain and historically not well co...

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Main Authors: Carter, Therese S, Heald, Colette L, Kroll, Jesse H, Apel, Eric C, Blake, Donald, Coggon, Matthew, Edtbauer, Achim, Gkatzelis, Georgios, Hornbrook, Rebecca S, Peischl, Jeff, Pfannerstill, Eva Y, Piel, Felix, Reijrink, Nina G, Ringsdorf, Akima, Warneke, Carsten, Williams, Jonathan, Wisthaler, Armin, Xu, Lu
Other Authors: Massachusetts Institute of Technology. Department of Civil and Environmental Engineering
Format: Article
Language:English
Published: Copernicus GmbH 2023
Online Access:https://hdl.handle.net/1721.1/148580
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author Carter, Therese S
Heald, Colette L
Kroll, Jesse H
Apel, Eric C
Blake, Donald
Coggon, Matthew
Edtbauer, Achim
Gkatzelis, Georgios
Hornbrook, Rebecca S
Peischl, Jeff
Pfannerstill, Eva Y
Piel, Felix
Reijrink, Nina G
Ringsdorf, Akima
Warneke, Carsten
Williams, Jonathan
Wisthaler, Armin
Xu, Lu
author2 Massachusetts Institute of Technology. Department of Civil and Environmental Engineering
author_facet Massachusetts Institute of Technology. Department of Civil and Environmental Engineering
Carter, Therese S
Heald, Colette L
Kroll, Jesse H
Apel, Eric C
Blake, Donald
Coggon, Matthew
Edtbauer, Achim
Gkatzelis, Georgios
Hornbrook, Rebecca S
Peischl, Jeff
Pfannerstill, Eva Y
Piel, Felix
Reijrink, Nina G
Ringsdorf, Akima
Warneke, Carsten
Williams, Jonathan
Wisthaler, Armin
Xu, Lu
author_sort Carter, Therese S
collection MIT
description <jats:p>Abstract. Fires emit a substantial amount of non-methane organic gases (NMOGs), the atmospheric oxidation of which can contribute to ozone and secondary particulate matter formation. However, the abundance and reactivity of these fire NMOGs are uncertain and historically not well constrained. In this work, we expand the representation of fire NMOGs in a global chemical transport model, GEOS-Chem. We update emission factors to Andreae (2019) and the chemical mechanism to include recent aromatic and ethene and ethyne model improvements (Bates et al., 2021; Kwon et al., 2021). We expand the representation of NMOGs by adding lumped furans to the model (including their fire emission and oxidation chemistry) and by adding fire emissions of nine species already included in the model, prioritized for their reactivity using data from the Fire Influence on Regional to Global Environments (FIREX) laboratory studies. Based on quantified emissions factors, we estimate that our improved representation captures 72 % of emitted, identified NMOG carbon mass and 49 % of OH reactivity from savanna and temperate forest fires, a substantial increase from the standard model (49 % of mass, 28 % of OH reactivity). We evaluate fire NMOGs in our model with observations from the Amazon Tall Tower Observatory (ATTO) in Brazil, Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) and DC3 in the US, and Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) in boreal Canada. We show that NMOGs, including furan, are well simulated in the eastern US with some underestimates in the western US and that adding fire emissions improves our ability to simulate ethene in boreal Canada. We estimate that fires provide 15 % of annual mean simulated surface OH reactivity globally, as well as more than 75 % over fire source regions. Over continental regions about half of this simulated fire reactivity comes from NMOG species. We find that furans and ethene are important globally for reactivity, while phenol is more important at a local level in the boreal regions. This is the first global estimate of the impact of fire on atmospheric reactivity. </jats:p>
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spelling mit-1721.1/1485802023-03-17T03:53:35Z An improved representation of fire non-methane organic gases (NMOGs) in models: emissions to reactivity Carter, Therese S Heald, Colette L Kroll, Jesse H Apel, Eric C Blake, Donald Coggon, Matthew Edtbauer, Achim Gkatzelis, Georgios Hornbrook, Rebecca S Peischl, Jeff Pfannerstill, Eva Y Piel, Felix Reijrink, Nina G Ringsdorf, Akima Warneke, Carsten Williams, Jonathan Wisthaler, Armin Xu, Lu Massachusetts Institute of Technology. Department of Civil and Environmental Engineering <jats:p>Abstract. Fires emit a substantial amount of non-methane organic gases (NMOGs), the atmospheric oxidation of which can contribute to ozone and secondary particulate matter formation. However, the abundance and reactivity of these fire NMOGs are uncertain and historically not well constrained. In this work, we expand the representation of fire NMOGs in a global chemical transport model, GEOS-Chem. We update emission factors to Andreae (2019) and the chemical mechanism to include recent aromatic and ethene and ethyne model improvements (Bates et al., 2021; Kwon et al., 2021). We expand the representation of NMOGs by adding lumped furans to the model (including their fire emission and oxidation chemistry) and by adding fire emissions of nine species already included in the model, prioritized for their reactivity using data from the Fire Influence on Regional to Global Environments (FIREX) laboratory studies. Based on quantified emissions factors, we estimate that our improved representation captures 72 % of emitted, identified NMOG carbon mass and 49 % of OH reactivity from savanna and temperate forest fires, a substantial increase from the standard model (49 % of mass, 28 % of OH reactivity). We evaluate fire NMOGs in our model with observations from the Amazon Tall Tower Observatory (ATTO) in Brazil, Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) and DC3 in the US, and Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) in boreal Canada. We show that NMOGs, including furan, are well simulated in the eastern US with some underestimates in the western US and that adding fire emissions improves our ability to simulate ethene in boreal Canada. We estimate that fires provide 15 % of annual mean simulated surface OH reactivity globally, as well as more than 75 % over fire source regions. Over continental regions about half of this simulated fire reactivity comes from NMOG species. We find that furans and ethene are important globally for reactivity, while phenol is more important at a local level in the boreal regions. This is the first global estimate of the impact of fire on atmospheric reactivity. </jats:p> 2023-03-16T17:13:05Z 2023-03-16T17:13:05Z 2022 2023-03-16T17:06:28Z Article http://purl.org/eprint/type/JournalArticle https://hdl.handle.net/1721.1/148580 Carter, Therese S, Heald, Colette L, Kroll, Jesse H, Apel, Eric C, Blake, Donald et al. 2022. "An improved representation of fire non-methane organic gases (NMOGs) in models: emissions to reactivity." Atmospheric Chemistry and Physics, 22 (18). en 10.5194/ACP-22-12093-2022 Atmospheric Chemistry and Physics Creative Commons Attribution 4.0 International license https://creativecommons.org/licenses/by/4.0/ application/pdf Copernicus GmbH Copernicus Publications
spellingShingle Carter, Therese S
Heald, Colette L
Kroll, Jesse H
Apel, Eric C
Blake, Donald
Coggon, Matthew
Edtbauer, Achim
Gkatzelis, Georgios
Hornbrook, Rebecca S
Peischl, Jeff
Pfannerstill, Eva Y
Piel, Felix
Reijrink, Nina G
Ringsdorf, Akima
Warneke, Carsten
Williams, Jonathan
Wisthaler, Armin
Xu, Lu
An improved representation of fire non-methane organic gases (NMOGs) in models: emissions to reactivity
title An improved representation of fire non-methane organic gases (NMOGs) in models: emissions to reactivity
title_full An improved representation of fire non-methane organic gases (NMOGs) in models: emissions to reactivity
title_fullStr An improved representation of fire non-methane organic gases (NMOGs) in models: emissions to reactivity
title_full_unstemmed An improved representation of fire non-methane organic gases (NMOGs) in models: emissions to reactivity
title_short An improved representation of fire non-methane organic gases (NMOGs) in models: emissions to reactivity
title_sort improved representation of fire non methane organic gases nmogs in models emissions to reactivity
url https://hdl.handle.net/1721.1/148580
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