Indoor secondary organic aerosols: Towards an improved representation of their formation and composition in models

The formation of secondary organic aerosol (SOA) indoors is one of the many consequences of the rich and complex chemistry that occurs therein. Given particulate matter has well documented health effects, we need to understand the mechanism for SOA formation indoors and its resulting composition. Th...

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Vydané v:	Atmospheric Environment: X Ročník 240; s. 117784
Hlavní autori:	Kruza, M., McFiggans, G., Waring, M.S., Wells, J.R., Carslaw, N.
Médium:	Journal Article
Jazyk:	English
Vydavateľské údaje:	England Elsevier Ltd 01.11.2020
Predmet:	aerosols alcohols autoxidation environment Highly oxygenated organic molecules Indoor air chemistry model validation nitrates particulates Secondary organic aerosol vapor pressure vapors Vapour pressure Volatile organic compound Vapour pressure Indoor air chemistry Secondary organic aerosol Volatile organic compound Highly oxygenated organic molecules
ISSN:	1352-2310, 2590-1621, 1873-2844, 2590-1621
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Abstract	The formation of secondary organic aerosol (SOA) indoors is one of the many consequences of the rich and complex chemistry that occurs therein. Given particulate matter has well documented health effects, we need to understand the mechanism for SOA formation indoors and its resulting composition. This study evaluates some uncertainties that exist in quantifying gas-to-particle partitioning of SOA-forming compounds using an indoor detailed chemical model. In particular, we investigate the impacts of using different methods to estimate compound vapour pressures as well as simulating the formation of highly oxygenated organic molecules (HOM) via auto-oxidation on SOA formation indoors. Estimation of vapour pressures for 136 α-pinene oxidation species by six investigated methods led to standard deviations of 28–216%. Inclusion of HOM formation improved model performance across three of the six assessed vapour pressure estimation methods when comparing against experimental data, particularly when the NO2 concentration was relatively high. We also explored the predicted SOA composition using two product classification methods, the first assuming the molecule is dominated by one functionality according to its name, and the second accounting for the fractional weighting of each functional group within a molecule. The SOA composition was dominated by the HOM species when the NO2-to-α-terpineol ratio was high for both product classification methods, as these conditions promoted formation of the nitrate radical and hence formation of HOM monomers. As the NO2-to-α-terpineol ratio decreased, peroxides and acids dominated the simple classification, whereas for the fractional classification, carbonyl and alcohol groups became more important. •SOA concentration predictions are highly dependent on selected vapour pressure method used.•Highly oxygenated organic molecules form an important component of indoor SOA.•Composition of indoor SOA is highly complex and depends on indoor conditions.
AbstractList	The formation of secondary organic aerosol (SOA) indoors is one of the many consequences of the rich and complex chemistry that occurs therein. Given particulate matter has well documented health effects, we need to understand the mechanism for SOA formation indoors and its resulting composition. This study evaluates some uncertainties that exist in quantifying gas-to-particle partitioning of SOA-forming compounds using an indoor detailed chemical model. In particular, we investigate the impacts of using different methods to estimate compound vapour pressures as well as simulating the formation of highly oxygenated organic molecules (HOM) via auto-oxidation on SOA formation indoors. Estimation of vapour pressures for 136 α-pinene oxidation species by six investigated methods led to standard deviations of 28–216%. Inclusion of HOM formation improved model performance across three of the six assessed vapour pressure estimation methods when comparing against experimental data, particularly when the NO2 concentration was relatively high. We also explored the predicted SOA composition using two product classification methods, the first assuming the molecule is dominated by one functionality according to its name, and the second accounting for the fractional weighting of each functional group within a molecule. The SOA composition was dominated by the HOM species when the NO2-to-α-terpineol ratio was high for both product classification methods, as these conditions promoted formation of the nitrate radical and hence formation of HOM monomers. As the NO2-to-α-terpineol ratio decreased, peroxides and acids dominated the simple classification, whereas for the fractional classification, carbonyl and alcohol groups became more important. The formation of secondary organic aerosol (SOA) indoors is one of the many consequences of the rich and complex chemistry that occurs therein. Given particulate matter has well documented health effects, we need to understand the mechanism for SOA formation indoors and its resulting composition. This study evaluates some uncertainties that exist in quantifying gas-to-particle partitioning of SOA-forming compounds using an indoor detailed chemical model. In particular, we investigate the impacts of using different methods to estimate compound vapour pressures as well as simulating the formation of highly oxygenated organic molecules (HOM) via auto-oxidation on SOA formation indoors. Estimation of vapour pressures for 136 α-pinene oxidation species by six investigated methods led to standard deviations of 28-216%. Inclusion of HOM formation improved model performance across three of the six assessed vapour pressure estimation methods when comparing against experimental data, particularly when the NO concentration was relatively high. We also explored the predicted SOA composition using two product classification methods, the first assuming the molecule is dominated by one functionality according to its name, and the second accounting for the fractional weighting of each functional group within a molecule. The SOA composition was dominated by the HOM species when the NO -to-α-terpineol ratio was high for both product classification methods, as these conditions promoted formation of the nitrate radical and hence formation of HOM monomers. As the NO -to-α-terpineol ratio decreased, peroxides and acids dominated the simple classification, whereas for the fractional classification, carbonyl and alcohol groups became more important. The formation of secondary organic aerosol (SOA) indoors is one of the many consequences of the rich and complex chemistry that occurs therein. Given particulate matter has well documented health effects, we need to understand the mechanism for SOA formation indoors and its resulting composition. This study evaluates some uncertainties that exist in quantifying gas-to-particle partitioning of SOA-forming compounds using an indoor detailed chemical model. In particular, we investigate the impacts of using different methods to estimate compound vapour pressures as well as simulating the formation of highly oxygenated organic molecules (HOM) via auto-oxidation on SOA formation indoors. Estimation of vapour pressures for 136 α-pinene oxidation species by six investigated methods led to standard deviations of 28–216%. Inclusion of HOM formation improved model performance across three of the six assessed vapour pressure estimation methods when comparing against experimental data, particularly when the NO₂ concentration was relatively high. We also explored the predicted SOA composition using two product classification methods, the first assuming the molecule is dominated by one functionality according to its name, and the second accounting for the fractional weighting of each functional group within a molecule. The SOA composition was dominated by the HOM species when the NO₂-to-α-terpineol ratio was high for both product classification methods, as these conditions promoted formation of the nitrate radical and hence formation of HOM monomers. As the NO₂-to-α-terpineol ratio decreased, peroxides and acids dominated the simple classification, whereas for the fractional classification, carbonyl and alcohol groups became more important. The formation of secondary organic aerosol (SOA) indoors is one of the many consequences of the rich and complex chemistry that occurs therein. Given particulate matter has well documented health effects, we need to understand the mechanism for SOA formation indoors and its resulting composition. This study evaluates some uncertainties that exist in quantifying gas-to-particle partitioning of SOA-forming compounds using an indoor detailed chemical model. In particular, we investigate the impacts of using different methods to estimate compound vapour pressures as well as simulating the formation of highly oxygenated organic molecules (HOM) via auto-oxidation on SOA formation indoors. Estimation of vapour pressures for 136 α-pinene oxidation species by six investigated methods led to standard deviations of 28–216%. Inclusion of HOM formation improved model performance across three of the six assessed vapour pressure estimation methods when comparing against experimental data, particularly when the NO2 concentration was relatively high. We also explored the predicted SOA composition using two product classification methods, the first assuming the molecule is dominated by one functionality according to its name, and the second accounting for the fractional weighting of each functional group within a molecule. The SOA composition was dominated by the HOM species when the NO2-to-α-terpineol ratio was high for both product classification methods, as these conditions promoted formation of the nitrate radical and hence formation of HOM monomers. As the NO2-to-α-terpineol ratio decreased, peroxides and acids dominated the simple classification, whereas for the fractional classification, carbonyl and alcohol groups became more important. •SOA concentration predictions are highly dependent on selected vapour pressure method used.•Highly oxygenated organic molecules form an important component of indoor SOA.•Composition of indoor SOA is highly complex and depends on indoor conditions. The formation of secondary organic aerosol (SOA) indoors is one of the many consequences of the rich and complex chemistry that occurs therein. Given particulate matter has well documented health effects, we need to understand the mechanism for SOA formation indoors and its resulting composition. This study evaluates some uncertainties that exist in quantifying gas-to-particle partitioning of SOA-forming compounds using an indoor detailed chemical model. In particular, we investigate the impacts of using different methods to estimate compound vapour pressures as well as simulating the formation of highly oxygenated organic molecules (HOM) via auto-oxidation on SOA formation indoors. Estimation of vapour pressures for 136 α-pinene oxidation species by six investigated methods led to standard deviations of 28-216%. Inclusion of HOM formation improved model performance across three of the six assessed vapour pressure estimation methods when comparing against experimental data, particularly when the NO2 concentration was relatively high. We also explored the predicted SOA composition using two product classification methods, the first assuming the molecule is dominated by one functionality according to its name, and the second accounting for the fractional weighting of each functional group within a molecule. The SOA composition was dominated by the HOM species when the NO2-to-α-terpineol ratio was high for both product classification methods, as these conditions promoted formation of the nitrate radical and hence formation of HOM monomers. As the NO2-to-α-terpineol ratio decreased, peroxides and acids dominated the simple classification, whereas for the fractional classification, carbonyl and alcohol groups became more important.The formation of secondary organic aerosol (SOA) indoors is one of the many consequences of the rich and complex chemistry that occurs therein. Given particulate matter has well documented health effects, we need to understand the mechanism for SOA formation indoors and its resulting composition. This study evaluates some uncertainties that exist in quantifying gas-to-particle partitioning of SOA-forming compounds using an indoor detailed chemical model. In particular, we investigate the impacts of using different methods to estimate compound vapour pressures as well as simulating the formation of highly oxygenated organic molecules (HOM) via auto-oxidation on SOA formation indoors. Estimation of vapour pressures for 136 α-pinene oxidation species by six investigated methods led to standard deviations of 28-216%. Inclusion of HOM formation improved model performance across three of the six assessed vapour pressure estimation methods when comparing against experimental data, particularly when the NO2 concentration was relatively high. We also explored the predicted SOA composition using two product classification methods, the first assuming the molecule is dominated by one functionality according to its name, and the second accounting for the fractional weighting of each functional group within a molecule. The SOA composition was dominated by the HOM species when the NO2-to-α-terpineol ratio was high for both product classification methods, as these conditions promoted formation of the nitrate radical and hence formation of HOM monomers. As the NO2-to-α-terpineol ratio decreased, peroxides and acids dominated the simple classification, whereas for the fractional classification, carbonyl and alcohol groups became more important.
ArticleNumber	117784
Author	Carslaw, N. McFiggans, G. Waring, M.S. Kruza, M. Wells, J.R.
AuthorAffiliation	d National Institute for Occupational Safety and Health, Morgantown, WV, USA c Department of Civil, Architectural and Environmental Engineering, Drexel University, Philadelphia, PA, USA b School of Earth and Environmental Sciences, University of Manchester, Manchester, UK a Department of Environment and Geography, University of York, Wentworth Way, York, YO10 5NG, UK
AuthorAffiliation_xml	– name: c Department of Civil, Architectural and Environmental Engineering, Drexel University, Philadelphia, PA, USA – name: b School of Earth and Environmental Sciences, University of Manchester, Manchester, UK – name: d National Institute for Occupational Safety and Health, Morgantown, WV, USA – name: a Department of Environment and Geography, University of York, Wentworth Way, York, YO10 5NG, UK
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BackLink	https://www.ncbi.nlm.nih.gov/pubmed/33594348$$D View this record in MEDLINE/PubMed
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Notes	ObjectType-Article-1 SourceType-Scholarly Journals-1 ObjectType-Feature-2 content type line 23 M. Kruza: Methodology, Software, Formal analysis, Investigation, Writing - original draft. G. McFiggans: Conceptualization, Methodology, Writing - original draft. M.S. Waring: Methodology. J.R. Wells: Methodology, Writing - original draft. N. Carslaw: Conceptualization, Methodology, Software, Investigation, Writing - original draft, Funding acquisition. CRediT authorship contribution statement
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Snippet	The formation of secondary organic aerosol (SOA) indoors is one of the many consequences of the rich and complex chemistry that occurs therein. Given...
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SubjectTerms	aerosols alcohols autoxidation environment Highly oxygenated organic molecules Indoor air chemistry model validation nitrates particulates Secondary organic aerosol vapor pressure vapors Vapour pressure Volatile organic compound
Title	Indoor secondary organic aerosols: Towards an improved representation of their formation and composition in models
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