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Title: In situ secondary organic aerosol formation from ambient pine forest air using an oxidation flow reactor

Abstract

An oxidation flow reactor (OFR) is a vessel inside which the concentration of a chosen oxidant can be increased for the purpose of studying SOA formation and aging by that oxidant. During the BEACHON-RoMBAS (Bio-hydro-atmosphere interactions of Energy, Aerosols, Carbon, H2O, Organics & Nitrogen–Rocky Mountain Biogenic Aerosol Study) field campaign, ambient pine forest air was oxidized by OH radicals in an OFR to measure the amount of SOA that could be formed from the real mix of ambient SOA precursor gases, and how that amount changed with time as precursors changed. High OH concentrations and short residence times allowed for semicontinuous cycling through a large range of OH exposures ranging from hours to weeks of equivalent (eq.) atmospheric aging. A simple model is derived and used to account for the relative timescales of condensation of low-volatility organic compounds (LVOCs) onto particles; condensational loss to the walls; and further reaction to produce volatile, non-condensing fragmentation products. More SOA production was observed in the OFR at nighttime (average 3 µg m–3 when LVOC fate corrected) compared to daytime (average 0.9 µg m–3 when LVOC fate corrected), with maximum formation observed at 0.4–1.5 eq. days of photochemical aging. SOA formation followed a similar diurnalmore » pattern to monoterpenes, sesquiterpenes, and toluene+p-cymene concentrations, including a substantial increase just after sunrise at 07:00 local time. Higher photochemical aging (>10 eq. days) led to a decrease in new SOA formation and a loss of preexisting OA due to heterogeneous oxidation followed by fragmentation and volatilization. When comparing two different commonly used methods of OH production in OFRs (OFR185 and OFR254-70), similar amounts of SOA formation were observed. We recommend the OFR185 mode for future forest studies. Concurrent gas-phase measurements of air after OH oxidation illustrate the decay of primary VOCs, production of small oxidized organic compounds, and net production at lower ages followed by net consumption of terpenoid oxidation products as photochemical age increased. New particle formation was observed in the reactor after oxidation, especially during times when precursor gas concentrations and SOA formation were largest. Approximately 4.4 times more SOA was formed in the reactor from OH oxidation than could be explained by the VOCs measured in ambient air. To our knowledge this is the first time that this has been shown when comparing VOC concentrations with SOA formation measured at the same time, rather than comparing measurements made at different times. Several recently developed instruments have quantified ambient semivolatile and intermediate-volatility organic compounds (S/IVOCs) that were not detected by a proton transfer reaction time-of-flight mass spectrometer (PTR-TOF-MS). An SOA yield of 18–58 % from those compounds can explain the observed SOA formation. S/IVOCs were the only pool of gas-phase carbon that was large enough to explain the observed SOA formation. This work suggests that these typically unmeasured gases play a substantial role in ambient SOA formation. Our results allow ruling out condensation sticking coefficients much lower than 1. Lastly, these measurements help clarify the magnitude of potential SOA formation from OH oxidation in forested environments and demonstrate methods for interpretation of ambient OFR measurements.« less

Authors:
ORCiD logo; ORCiD logo; ; ORCiD logo; ; ORCiD logo; ORCiD logo; ORCiD logo; ; ; ORCiD logo; ORCiD logo; ORCiD logo; ORCiD logo
Publication Date:
Research Org.:
Univ. of Colorado, Boulder, CO (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER)
OSTI Identifier:
1240759
Alternate Identifier(s):
OSTI ID: 1268269
Grant/Contract Number:  
SC0011105
Resource Type:
Published Article
Journal Name:
Atmospheric Chemistry and Physics (Online)
Additional Journal Information:
Journal Name: Atmospheric Chemistry and Physics (Online) Journal Volume: 16 Journal Issue: 5; Journal ID: ISSN 1680-7324
Publisher:
Copernicus Publications, EGU
Country of Publication:
Germany
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; cloud condensation nuclei; mass accommodation coefficient; beachon-rombas 2011; intermediate-volatility; soa formation; sulfuric-acid; mexico-city; chemical-composition; particle formation; radical chemistry

Citation Formats

Palm, Brett B., Campuzano-Jost, Pedro, Ortega, Amber M., Day, Douglas A., Kaser, Lisa, Jud, Werner, Karl, Thomas, Hansel, Armin, Hunter, James F., Cross, Eben S., Kroll, Jesse H., Peng, Zhe, Brune, William H., and Jimenez, Jose L. In situ secondary organic aerosol formation from ambient pine forest air using an oxidation flow reactor. Germany: N. p., 2016. Web. doi:10.5194/acp-16-2943-2016.
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Palm, Brett B., Campuzano-Jost, Pedro, Ortega, Amber M., Day, Douglas A., Kaser, Lisa, Jud, Werner, Karl, Thomas, Hansel, Armin, Hunter, James F., Cross, Eben S., Kroll, Jesse H., Peng, Zhe, Brune, William H., & Jimenez, Jose L. In situ secondary organic aerosol formation from ambient pine forest air using an oxidation flow reactor. Germany. https://doi.org/10.5194/acp-16-2943-2016
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Palm, Brett B., Campuzano-Jost, Pedro, Ortega, Amber M., Day, Douglas A., Kaser, Lisa, Jud, Werner, Karl, Thomas, Hansel, Armin, Hunter, James F., Cross, Eben S., Kroll, Jesse H., Peng, Zhe, Brune, William H., and Jimenez, Jose L. Tue . "In situ secondary organic aerosol formation from ambient pine forest air using an oxidation flow reactor". Germany. https://doi.org/10.5194/acp-16-2943-2016.
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@article{osti_1240759,
title = {In situ secondary organic aerosol formation from ambient pine forest air using an oxidation flow reactor},
author = {Palm, Brett B. and Campuzano-Jost, Pedro and Ortega, Amber M. and Day, Douglas A. and Kaser, Lisa and Jud, Werner and Karl, Thomas and Hansel, Armin and Hunter, James F. and Cross, Eben S. and Kroll, Jesse H. and Peng, Zhe and Brune, William H. and Jimenez, Jose L.},
abstractNote = {An oxidation flow reactor (OFR) is a vessel inside which the concentration of a chosen oxidant can be increased for the purpose of studying SOA formation and aging by that oxidant. During the BEACHON-RoMBAS (Bio-hydro-atmosphere interactions of Energy, Aerosols, Carbon, H2O, Organics & Nitrogen–Rocky Mountain Biogenic Aerosol Study) field campaign, ambient pine forest air was oxidized by OH radicals in an OFR to measure the amount of SOA that could be formed from the real mix of ambient SOA precursor gases, and how that amount changed with time as precursors changed. High OH concentrations and short residence times allowed for semicontinuous cycling through a large range of OH exposures ranging from hours to weeks of equivalent (eq.) atmospheric aging. A simple model is derived and used to account for the relative timescales of condensation of low-volatility organic compounds (LVOCs) onto particles; condensational loss to the walls; and further reaction to produce volatile, non-condensing fragmentation products. More SOA production was observed in the OFR at nighttime (average 3 µg m–3 when LVOC fate corrected) compared to daytime (average 0.9 µg m–3 when LVOC fate corrected), with maximum formation observed at 0.4–1.5 eq. days of photochemical aging. SOA formation followed a similar diurnal pattern to monoterpenes, sesquiterpenes, and toluene+p-cymene concentrations, including a substantial increase just after sunrise at 07:00 local time. Higher photochemical aging (>10 eq. days) led to a decrease in new SOA formation and a loss of preexisting OA due to heterogeneous oxidation followed by fragmentation and volatilization. When comparing two different commonly used methods of OH production in OFRs (OFR185 and OFR254-70), similar amounts of SOA formation were observed. We recommend the OFR185 mode for future forest studies. Concurrent gas-phase measurements of air after OH oxidation illustrate the decay of primary VOCs, production of small oxidized organic compounds, and net production at lower ages followed by net consumption of terpenoid oxidation products as photochemical age increased. New particle formation was observed in the reactor after oxidation, especially during times when precursor gas concentrations and SOA formation were largest. Approximately 4.4 times more SOA was formed in the reactor from OH oxidation than could be explained by the VOCs measured in ambient air. To our knowledge this is the first time that this has been shown when comparing VOC concentrations with SOA formation measured at the same time, rather than comparing measurements made at different times. Several recently developed instruments have quantified ambient semivolatile and intermediate-volatility organic compounds (S/IVOCs) that were not detected by a proton transfer reaction time-of-flight mass spectrometer (PTR-TOF-MS). An SOA yield of 18–58 % from those compounds can explain the observed SOA formation. S/IVOCs were the only pool of gas-phase carbon that was large enough to explain the observed SOA formation. This work suggests that these typically unmeasured gases play a substantial role in ambient SOA formation. Our results allow ruling out condensation sticking coefficients much lower than 1. Lastly, these measurements help clarify the magnitude of potential SOA formation from OH oxidation in forested environments and demonstrate methods for interpretation of ambient OFR measurements.},
doi = {10.5194/acp-16-2943-2016},
journal = {Atmospheric Chemistry and Physics (Online)},
number = 5,
volume = 16,
place = {Germany},
year = {Tue Mar 08 00:00:00 EST 2016},
month = {Tue Mar 08 00:00:00 EST 2016}
}
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https://doi.org/10.5194/acp-16-2943-2016
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The heterogeneous reaction of hydroxyl radicals with sub-micron squalane particles: a model system for understanding the oxidative aging of ambient aerosols
journal, January 2009

  • Smith, J. D.; Kroll, J. H.; Cappa, C. D.
  • Atmospheric Chemistry and Physics, Vol. 9, Issue 9
  • DOI: 10.5194/acp-9-3209-2009

Modeling the Radical Chemistry in an Oxidation Flow Reactor: Radical Formation and Recycling, Sensitivities, and the OH Exposure Estimation Equation
journal, November 2014

  • Li, Rui; Palm, Brett B.; Ortega, Amber M.
  • The Journal of Physical Chemistry A, Vol. 119, Issue 19
  • DOI: 10.1021/jp509534k

Size-resolved aerosol composition and its link to hygroscopicity at a forested site in Colorado
journal, January 2014

  • Levin, E. J. T.; Prenni, A. J.; Palm, B. B.
  • Atmospheric Chemistry and Physics, Vol. 14, Issue 5
  • DOI: 10.5194/acp-14-2657-2014

Effect of NO x on Secondary Organic Aerosol Concentrations
journal, August 2008

  • Lane, Timothy E.; Donahue, Neil M.; Pandis, Spyros N.
  • Environmental Science & Technology, Vol. 42, Issue 16
  • DOI: 10.1021/es703225a

Photo-Oxidation of Low-Volatility Organics Found in Motor Vehicle Emissions: Production and Chemical Evolution of Organic Aerosol Mass
journal, March 2010

  • Miracolo, Marissa A.; Presto, Albert A.; Lambe, Andrew T.
  • Environmental Science & Technology, Vol. 44, Issue 5
  • DOI: 10.1021/es902635c

Secondary Organic Aerosol Formation from High-NO x Photo-Oxidation of Low Volatility Precursors: n -Alkanes
journal, March 2010

  • Presto, Albert A.; Miracolo, Marissa A.; Donahue, Neil M.
  • Environmental Science & Technology, Vol. 44, Issue 6
  • DOI: 10.1021/es903712r

Gas-phase products and secondary aerosol yields from the photooxidation of 16 different terpenes
journal, January 2006

  • Lee, Anita; Goldstein, Allen H.; Kroll, Jesse H.
  • Journal of Geophysical Research, Vol. 111, Issue D17
  • DOI: 10.1029/2006JD007050

Real-time measurements of secondary organic aerosol formation and aging from ambient air in an oxidation flow reactor in the Los Angeles area
journal, January 2015

  • Ortega, A. M.; Hayes, P. L.; Peng, Z.
  • Atmospheric Chemistry and Physics Discussions, Vol. 15, Issue 15
  • DOI: 10.5194/acpd-15-21907-2015

Unexpected Epoxide Formation in the Gas-Phase Photooxidation of Isoprene
journal, August 2009

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