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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, H 2O, 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 followedmore » 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.« less

Authors:
 [1];  [1];  [2];  [1];  [3];  [4];  [5];  [4];  [6];  [6];  [7];  [1];  [8];  [1]
  1. Univ. of Colorado, Boulder, CO (United States). Cooperative Inst. for Research in Environmental Sciences; Dept. of Chemistry and Biochemistry
  2. Univ. of Colorado, Boulder, CO (United States). Cooperative Inst. for Research in Environmental Sciences; Dept. of Atmospheric and Oceanic Science
  3. National Center for Atmospheric Research, Boulder, CO (United States); Univ. of Innsbruck, Innsbruck (Austria). Inst. of Ion Physics and Applied Physics
  4. Univ. of Innsbruck, Innsbruck (Austria). Inst. of Ion Physics and Applied Physics
  5. Univ. of Innsbruck, Innsbruck (Austria). Inst. of Meteorology and Geophysics
  6. Massachusetts Inst. of Technology Cambridge, MA (United States). Dept. of Civil and Environmental Engineering
  7. Massachusetts Inst. of Technology Cambridge, MA (United States). Dept. of Civil and Environmental Engineering; Dept. of Chemical Engineering
  8. Pennsylvania State Univ., State College, PA (United States). Dept. of Meteorology
Publication Date:
Research Org.:
Univ. of Colorado, Boulder, CO (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23)
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:
European Geosciences Union
Country of Publication:
United States
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. United States: N. p., 2016. Web. doi:10.5194/acp-16-2943-2016.
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. United States. doi:10.5194/acp-16-2943-2016.
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". United States. doi:10.5194/acp-16-2943-2016.
@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 = {United States},
year = {2016},
month = {3}
}

Journal Article:
Free Publicly Available Full Text
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DOI: 10.5194/acp-16-2943-2016

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