Cargando…

Time-Resolved Molecular Characterization of Secondary Organic Aerosol Formed from OH and NO(3) Radical Initiated Oxidation of a Mixture of Aromatic Precursors

[Image: see text] Aromatic hydrocarbons (ArHCs) and oxygenated aromatic hydrocarbons (ArHC–OHs) are emitted from a variety of anthropogenic activities and are important precursors of secondary organic aerosol (SOA) in urban areas. Here, we analyzed and compared the composition of SOA formed from the...

Descripción completa

Detalles Bibliográficos
Autores principales: Kumar, Varun, Slowik, Jay G., Baltensperger, Urs, Prevot, Andre S. H., Bell, David M.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2023
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10413940/
https://www.ncbi.nlm.nih.gov/pubmed/37496264
http://dx.doi.org/10.1021/acs.est.3c00225
_version_ 1785087241144500224
author Kumar, Varun
Slowik, Jay G.
Baltensperger, Urs
Prevot, Andre S. H.
Bell, David M.
author_facet Kumar, Varun
Slowik, Jay G.
Baltensperger, Urs
Prevot, Andre S. H.
Bell, David M.
author_sort Kumar, Varun
collection PubMed
description [Image: see text] Aromatic hydrocarbons (ArHCs) and oxygenated aromatic hydrocarbons (ArHC–OHs) are emitted from a variety of anthropogenic activities and are important precursors of secondary organic aerosol (SOA) in urban areas. Here, we analyzed and compared the composition of SOA formed from the oxidation of a mixture of aromatic VOCs by OH and NO(3) radicals. The VOC mixture was composed of toluene (C(7)H(8)), p-xylene + ethylbenzene (C(8)H(10)), 1,3,5-trimethylbenzene (C(9)H(12)), phenol (C(6)H(6)O), cresol (C(7)H(8)O), 2,6-dimethylphenol (C(8)H(10)O), and 2,4,6-trimethylphenol (C(9)H(12)O) in a proportion where the aromatic VOCs were chosen to approximate day-time traffic-related emissions in Delhi, and the aromatic alcohols make up 20% of the mixture. These VOCs are prominent in other cities as well, including those influenced by biomass combustion. In the NO(3) experiments, large contributions from C(x)H(y)O(z)N dimers (C(15)–C(18)) were observed, corresponding to fast SOA formation within 15–20 min after the start of chemistry. Additionally, the dimers were a mixture of different combinations of the initial VOCs, highlighting the importance of exploring SOAs from mixed VOC systems. In contrast, the experiments with OH radicals yielded gradual SOA mass formation, with C(x)H(y)O(z) monomers (C(6)–C(9)) being the dominant constituents. The evolution of SOA composition with time was tracked and a fast degradation of dimers was observed in the NO(3) experiments, with concurrent formation of monomer species. The rates of dimer decomposition in NO(3) SOA were ∼2–3 times higher compared to those previously determined for α-pinene + O(3) SOA, highlighting the dependence of particle-phase reactions on VOC precursors and oxidants. In contrast, the SOA produced in the OH experiments did not dramatically change over the same time frame. No measurable effects of humidity were observed on the composition and evolution of SOA.
format Online
Article
Text
id pubmed-10413940
institution National Center for Biotechnology Information
language English
publishDate 2023
publisher American Chemical Society
record_format MEDLINE/PubMed
spelling pubmed-104139402023-08-11 Time-Resolved Molecular Characterization of Secondary Organic Aerosol Formed from OH and NO(3) Radical Initiated Oxidation of a Mixture of Aromatic Precursors Kumar, Varun Slowik, Jay G. Baltensperger, Urs Prevot, Andre S. H. Bell, David M. Environ Sci Technol [Image: see text] Aromatic hydrocarbons (ArHCs) and oxygenated aromatic hydrocarbons (ArHC–OHs) are emitted from a variety of anthropogenic activities and are important precursors of secondary organic aerosol (SOA) in urban areas. Here, we analyzed and compared the composition of SOA formed from the oxidation of a mixture of aromatic VOCs by OH and NO(3) radicals. The VOC mixture was composed of toluene (C(7)H(8)), p-xylene + ethylbenzene (C(8)H(10)), 1,3,5-trimethylbenzene (C(9)H(12)), phenol (C(6)H(6)O), cresol (C(7)H(8)O), 2,6-dimethylphenol (C(8)H(10)O), and 2,4,6-trimethylphenol (C(9)H(12)O) in a proportion where the aromatic VOCs were chosen to approximate day-time traffic-related emissions in Delhi, and the aromatic alcohols make up 20% of the mixture. These VOCs are prominent in other cities as well, including those influenced by biomass combustion. In the NO(3) experiments, large contributions from C(x)H(y)O(z)N dimers (C(15)–C(18)) were observed, corresponding to fast SOA formation within 15–20 min after the start of chemistry. Additionally, the dimers were a mixture of different combinations of the initial VOCs, highlighting the importance of exploring SOAs from mixed VOC systems. In contrast, the experiments with OH radicals yielded gradual SOA mass formation, with C(x)H(y)O(z) monomers (C(6)–C(9)) being the dominant constituents. The evolution of SOA composition with time was tracked and a fast degradation of dimers was observed in the NO(3) experiments, with concurrent formation of monomer species. The rates of dimer decomposition in NO(3) SOA were ∼2–3 times higher compared to those previously determined for α-pinene + O(3) SOA, highlighting the dependence of particle-phase reactions on VOC precursors and oxidants. In contrast, the SOA produced in the OH experiments did not dramatically change over the same time frame. No measurable effects of humidity were observed on the composition and evolution of SOA. American Chemical Society 2023-07-27 /pmc/articles/PMC10413940/ /pubmed/37496264 http://dx.doi.org/10.1021/acs.est.3c00225 Text en © 2023 The Authors. Published by American Chemical Society https://creativecommons.org/licenses/by/4.0/Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained (https://creativecommons.org/licenses/by/4.0/).
spellingShingle Kumar, Varun
Slowik, Jay G.
Baltensperger, Urs
Prevot, Andre S. H.
Bell, David M.
Time-Resolved Molecular Characterization of Secondary Organic Aerosol Formed from OH and NO(3) Radical Initiated Oxidation of a Mixture of Aromatic Precursors
title Time-Resolved Molecular Characterization of Secondary Organic Aerosol Formed from OH and NO(3) Radical Initiated Oxidation of a Mixture of Aromatic Precursors
title_full Time-Resolved Molecular Characterization of Secondary Organic Aerosol Formed from OH and NO(3) Radical Initiated Oxidation of a Mixture of Aromatic Precursors
title_fullStr Time-Resolved Molecular Characterization of Secondary Organic Aerosol Formed from OH and NO(3) Radical Initiated Oxidation of a Mixture of Aromatic Precursors
title_full_unstemmed Time-Resolved Molecular Characterization of Secondary Organic Aerosol Formed from OH and NO(3) Radical Initiated Oxidation of a Mixture of Aromatic Precursors
title_short Time-Resolved Molecular Characterization of Secondary Organic Aerosol Formed from OH and NO(3) Radical Initiated Oxidation of a Mixture of Aromatic Precursors
title_sort time-resolved molecular characterization of secondary organic aerosol formed from oh and no(3) radical initiated oxidation of a mixture of aromatic precursors
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10413940/
https://www.ncbi.nlm.nih.gov/pubmed/37496264
http://dx.doi.org/10.1021/acs.est.3c00225
work_keys_str_mv AT kumarvarun timeresolvedmolecularcharacterizationofsecondaryorganicaerosolformedfromohandno3radicalinitiatedoxidationofamixtureofaromaticprecursors
AT slowikjayg timeresolvedmolecularcharacterizationofsecondaryorganicaerosolformedfromohandno3radicalinitiatedoxidationofamixtureofaromaticprecursors
AT baltenspergerurs timeresolvedmolecularcharacterizationofsecondaryorganicaerosolformedfromohandno3radicalinitiatedoxidationofamixtureofaromaticprecursors
AT prevotandresh timeresolvedmolecularcharacterizationofsecondaryorganicaerosolformedfromohandno3radicalinitiatedoxidationofamixtureofaromaticprecursors
AT belldavidm timeresolvedmolecularcharacterizationofsecondaryorganicaerosolformedfromohandno3radicalinitiatedoxidationofamixtureofaromaticprecursors