Molecular composition and volatility of isoprene photochemical oxidation secondary organic aerosol under low- and high-NO<sub><i>x</i></sub> conditions
Abstract
We present measurements of secondary organic aerosol (SOA) formation from isoprene photochemical oxidation in an environmental simulation chamber at a variety of oxidant conditions and using dry neutral seed particles to suppress acid-catalyzed multiphase chemistry. A high-resolution time-of-flight chemical ionization mass spectrometer (HR-ToF-CIMS) utilizing iodide-adduct ionization coupled to the Filter Inlet for Gases and Aerosols (FIGAERO) allowed for simultaneous online sampling of the gas and particle composition. Under high-HO2 and low-NO conditions, highly oxygenated (O : C ≥ 1) C5 compounds were major components (~50 %) of SOA. The SOA composition and effective volatility evolved both as a function of time and as a function of input NO concentrations. Organic nitrates increased in both the gas and particle phases as input NO increased, but the dominant non-nitrate particle-phase components monotonically decreased. We use comparisons of measured and predicted gas-particle partitioning of individual components to assess the validity of literature-based group-contribution methods for estimating saturation vapor concentrations. While there is evidence for equilibrium partitioning being achieved on the chamber residence timescale (5.2 h) for some individual components, significant errors in group-contribution methods are revealed. In addition, > 30 % of the SOA mass, detected as low-molecular-weight semivolatile compounds, cannot be reconciled withmore »
- Publication Date:
- Research Org.:
- Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC)
- OSTI Identifier:
- 1338140
- Alternate Identifier(s):
- OSTI ID: 1339791; OSTI ID: 1390603
- Report Number(s):
- PNNL-SA-119934
Journal ID: ISSN 1680-7324
- Grant/Contract Number:
- AC05-76RL01830; SC0011791
- Resource Type:
- Published Article
- Journal Name:
- Atmospheric Chemistry and Physics (Online)
- Additional Journal Information:
- Journal Name: Atmospheric Chemistry and Physics (Online) Journal Volume: 17 Journal Issue: 1; Journal ID: ISSN 1680-7324
- Publisher:
- Copernicus Publications, EGU
- Country of Publication:
- Germany
- Language:
- English
- Subject:
- 54 ENVIRONMENTAL SCIENCES; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; isoprene; photochemical oxidation; secondary organic aerosol
Citation Formats
D'Ambro, Emma L., Lee, Ben H., Liu, Jiumeng, Shilling, John E., Gaston, Cassandra J., Lopez-Hilfiker, Felipe D., Schobesberger, Siegfried, Zaveri, Rahul A., Mohr, Claudia, Lutz, Anna, Zhang, Zhenfa, Gold, Avram, Surratt, Jason D., Rivera-Rios, Jean C., Keutsch, Frank N., and Thornton, Joel A. Molecular composition and volatility of isoprene photochemical oxidation secondary organic aerosol under low- and high-NO<sub><i>x</i></sub> conditions. Germany: N. p., 2017.
Web. doi:10.5194/acp-17-159-2017.
D'Ambro, Emma L., Lee, Ben H., Liu, Jiumeng, Shilling, John E., Gaston, Cassandra J., Lopez-Hilfiker, Felipe D., Schobesberger, Siegfried, Zaveri, Rahul A., Mohr, Claudia, Lutz, Anna, Zhang, Zhenfa, Gold, Avram, Surratt, Jason D., Rivera-Rios, Jean C., Keutsch, Frank N., & Thornton, Joel A. Molecular composition and volatility of isoprene photochemical oxidation secondary organic aerosol under low- and high-NO<sub><i>x</i></sub> conditions. Germany. https://doi.org/10.5194/acp-17-159-2017
D'Ambro, Emma L., Lee, Ben H., Liu, Jiumeng, Shilling, John E., Gaston, Cassandra J., Lopez-Hilfiker, Felipe D., Schobesberger, Siegfried, Zaveri, Rahul A., Mohr, Claudia, Lutz, Anna, Zhang, Zhenfa, Gold, Avram, Surratt, Jason D., Rivera-Rios, Jean C., Keutsch, Frank N., and Thornton, Joel A. Wed .
"Molecular composition and volatility of isoprene photochemical oxidation secondary organic aerosol under low- and high-NO<sub><i>x</i></sub> conditions". Germany. https://doi.org/10.5194/acp-17-159-2017.
@article{osti_1338140,
title = {Molecular composition and volatility of isoprene photochemical oxidation secondary organic aerosol under low- and high-NO<sub><i>x</i></sub> conditions},
author = {D'Ambro, Emma L. and Lee, Ben H. and Liu, Jiumeng and Shilling, John E. and Gaston, Cassandra J. and Lopez-Hilfiker, Felipe D. and Schobesberger, Siegfried and Zaveri, Rahul A. and Mohr, Claudia and Lutz, Anna and Zhang, Zhenfa and Gold, Avram and Surratt, Jason D. and Rivera-Rios, Jean C. and Keutsch, Frank N. and Thornton, Joel A.},
abstractNote = {We present measurements of secondary organic aerosol (SOA) formation from isoprene photochemical oxidation in an environmental simulation chamber at a variety of oxidant conditions and using dry neutral seed particles to suppress acid-catalyzed multiphase chemistry. A high-resolution time-of-flight chemical ionization mass spectrometer (HR-ToF-CIMS) utilizing iodide-adduct ionization coupled to the Filter Inlet for Gases and Aerosols (FIGAERO) allowed for simultaneous online sampling of the gas and particle composition. Under high-HO2 and low-NO conditions, highly oxygenated (O : C ≥ 1) C5 compounds were major components (~50 %) of SOA. The SOA composition and effective volatility evolved both as a function of time and as a function of input NO concentrations. Organic nitrates increased in both the gas and particle phases as input NO increased, but the dominant non-nitrate particle-phase components monotonically decreased. We use comparisons of measured and predicted gas-particle partitioning of individual components to assess the validity of literature-based group-contribution methods for estimating saturation vapor concentrations. While there is evidence for equilibrium partitioning being achieved on the chamber residence timescale (5.2 h) for some individual components, significant errors in group-contribution methods are revealed. In addition, > 30 % of the SOA mass, detected as low-molecular-weight semivolatile compounds, cannot be reconciled with equilibrium partitioning. These compounds desorb from the FIGAERO at unexpectedly high temperatures given their molecular composition, which is indicative of thermal decomposition of effectively lower-volatility components such as larger molecular weight oligomers.},
doi = {10.5194/acp-17-159-2017},
journal = {Atmospheric Chemistry and Physics (Online)},
number = 1,
volume = 17,
place = {Germany},
year = {Wed Jan 04 00:00:00 EST 2017},
month = {Wed Jan 04 00:00:00 EST 2017}
}
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