Alkylperoxy radicals are responsible for the formation of oxygenated primary organic aerosol

Omar El Hajj; Samuel W. Hartness; Gregory W. Vandergrift; Yensil Park; Chase K. Glenn; Anita Anosike; Annabelle R. Webb; Nicholas S. Dewey; Anna C. Doner; Zezhen Cheng; Gurneesh S. Jatana; Melanie Moses-DeBusk; Swarup China; Brandon Rotavera; Rawad Saleh

doi:10.1126/sciadv.adj2832

Alkylperoxy radicals are responsible for the formation of oxygenated primary organic aerosol

Omar El Hajj, Samuel W. Hartness, Gregory W. Vandergrift, Yensil Park, Chase K. Glenn, Anita Anosike, Annabelle R. Webb, Nicholas S. Dewey, Anna C. Doner, Zezhen Cheng, Gurneesh S. Jatana, Melanie Moses-DeBusk, Swarup China, Brandon Rotavera, Rawad Saleh

Research output: Contribution to journal › Article › peer-review

3 Scopus citations

Abstract

Organic aerosol (OA) is an air pollutant ubiquitous in urban atmospheres. Urban OA is usually apportioned into primary OA (POA), mostly emitted by mobile sources, and secondary OA (SOA), which forms in the atmosphere due to oxidation of gas-phase precursors from anthropogenic and biogenic sources. By performing coordinated measurements in the particle phase and the gas phase, we show that the alkylperoxy radical chemistry that is responsible for low-temperature ignition also leads to the formation of oxygenated POA (OxyPOA). OxyPOA is distinct from POA emitted during high-temperature ignition and is chemically similar to SOA. We present evidence for the prevalence of OxyPOA in emissions of a spark-ignition engine and a next-generation advanced compression-ignition engine, highlighting the importance of understanding OxyPOA for predicting urban air pollution patterns in current and future atmospheres.

Original language	English
Article number	eadj2832
Journal	Science Advances
Volume	9
Issue number	46
DOIs	https://doi.org/10.1126/sciadv.adj2832
State	Published - Nov 2023

Funding

The CDC and PCCI samples were collected as part of the Co-Optimization of Fuels & Engines (Co-Optima) project sponsored by the U.S. DOE Office of Energy Efficiency and Renewable Energy, Office of Bioenergy Technologies, and Office of Vehicle Technologies. The cold-start samples were collected as part of the Partnership to Advance Combustion Engines Consortium sponsored by the U.S. DOE Office of Vehicle Technologies. We thank K. Stork, M. Weismiller, and G. Singh for support of this work and S. Huff and S. Sluder for operating the diesel engine. We thank the University of Georgia Proteomics and Mass Spectrometry Core Facility for performing the LDI-MS and ESI-MS analyses. This work was supported by the National Science Foundation, Combustion and Fire Systems Program within the Division of Chemical, Bioengineering, Environmental, and Transport Systems under award CBET-2125064 (to R.S. and B.R.); Gas-Phase Chemical Physics program within the Division of Chemical Sciences, Geosciences and Biosciences, Office of Basic Energy Sciences (BES), U.S. DOE under award DE-SC0021337 (to B.R.); U.S. DOE Office of Science User Facility sponsored by the Biological and Environmental Research program under contract no. DE-AC05-76RL01830 (to G.W.V., Z.C., and S.C.); and National Institutes of Health award no. S10OD025118.

Funders	Funder number
Co-Optimization of Fuels & Engines
University of Georgia Proteomics and Mass Spectrometry Core Facility
National Science Foundation
National Institutes of Health	S10OD025118
U.S. Department of Energy	DE-SC0021337
Centers for Disease Control and Prevention
Division of Chemical, Bioengineering, Environmental, and Transport Systems	CBET-2125064
Office of Science
Office of Energy Efficiency and Renewable Energy
Basic Energy Sciences
Biological and Environmental Research	DE-AC05-76RL01830
Bioenergy Technologies Office
Vehicle Technologies Office

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Hajj, O. E., Hartness, S. W., Vandergrift, G. W., Park, Y., Glenn, C. K., Anosike, A., Webb, A. R., Dewey, N. S., Doner, A. C., Cheng, Z., Jatana, G. S., Moses-DeBusk, M., China, S., Rotavera, B., & Saleh, R. (2023). Alkylperoxy radicals are responsible for the formation of oxygenated primary organic aerosol. Science Advances, 9(46), Article eadj2832. https://doi.org/10.1126/sciadv.adj2832

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title = "Alkylperoxy radicals are responsible for the formation of oxygenated primary organic aerosol",

abstract = "Organic aerosol (OA) is an air pollutant ubiquitous in urban atmospheres. Urban OA is usually apportioned into primary OA (POA), mostly emitted by mobile sources, and secondary OA (SOA), which forms in the atmosphere due to oxidation of gas-phase precursors from anthropogenic and biogenic sources. By performing coordinated measurements in the particle phase and the gas phase, we show that the alkylperoxy radical chemistry that is responsible for low-temperature ignition also leads to the formation of oxygenated POA (OxyPOA). OxyPOA is distinct from POA emitted during high-temperature ignition and is chemically similar to SOA. We present evidence for the prevalence of OxyPOA in emissions of a spark-ignition engine and a next-generation advanced compression-ignition engine, highlighting the importance of understanding OxyPOA for predicting urban air pollution patterns in current and future atmospheres.",

author = "Hajj, {Omar El} and Hartness, {Samuel W.} and Vandergrift, {Gregory W.} and Yensil Park and Glenn, {Chase K.} and Anita Anosike and Webb, {Annabelle R.} and Dewey, {Nicholas S.} and Doner, {Anna C.} and Zezhen Cheng and Jatana, {Gurneesh S.} and Melanie Moses-DeBusk and Swarup China and Brandon Rotavera and Rawad Saleh",

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doi = "10.1126/sciadv.adj2832",

language = "English",

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T1 - Alkylperoxy radicals are responsible for the formation of oxygenated primary organic aerosol

AU - Hajj, Omar El

AU - Hartness, Samuel W.

AU - Vandergrift, Gregory W.

AU - Park, Yensil

AU - Glenn, Chase K.

AU - Anosike, Anita

AU - Webb, Annabelle R.

AU - Dewey, Nicholas S.

AU - Doner, Anna C.

AU - Cheng, Zezhen

AU - Jatana, Gurneesh S.

AU - Moses-DeBusk, Melanie

AU - China, Swarup

AU - Rotavera, Brandon

AU - Saleh, Rawad

PY - 2023/11

Y1 - 2023/11

N2 - Organic aerosol (OA) is an air pollutant ubiquitous in urban atmospheres. Urban OA is usually apportioned into primary OA (POA), mostly emitted by mobile sources, and secondary OA (SOA), which forms in the atmosphere due to oxidation of gas-phase precursors from anthropogenic and biogenic sources. By performing coordinated measurements in the particle phase and the gas phase, we show that the alkylperoxy radical chemistry that is responsible for low-temperature ignition also leads to the formation of oxygenated POA (OxyPOA). OxyPOA is distinct from POA emitted during high-temperature ignition and is chemically similar to SOA. We present evidence for the prevalence of OxyPOA in emissions of a spark-ignition engine and a next-generation advanced compression-ignition engine, highlighting the importance of understanding OxyPOA for predicting urban air pollution patterns in current and future atmospheres.

AB - Organic aerosol (OA) is an air pollutant ubiquitous in urban atmospheres. Urban OA is usually apportioned into primary OA (POA), mostly emitted by mobile sources, and secondary OA (SOA), which forms in the atmosphere due to oxidation of gas-phase precursors from anthropogenic and biogenic sources. By performing coordinated measurements in the particle phase and the gas phase, we show that the alkylperoxy radical chemistry that is responsible for low-temperature ignition also leads to the formation of oxygenated POA (OxyPOA). OxyPOA is distinct from POA emitted during high-temperature ignition and is chemically similar to SOA. We present evidence for the prevalence of OxyPOA in emissions of a spark-ignition engine and a next-generation advanced compression-ignition engine, highlighting the importance of understanding OxyPOA for predicting urban air pollution patterns in current and future atmospheres.

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JO - Science Advances

JF - Science Advances

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M1 - eadj2832

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Alkylperoxy radicals are responsible for the formation of oxygenated primary organic aerosol

Abstract

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