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Title: Secondary organic aerosol formation from in situ OH, O3, and NO3 oxidation of ambient forest air in an oxidation flow reactor

Abstract

Ambient pine forest air was oxidized by OH, O3, or NO3 radicals using an oxidation flow reactor (OFR) during the BEACHON-RoMBAS (Bio–hydro–atmosphere interactions of Energy, Aerosols, Carbon, H2O, Organics and Nitrogen – Rocky Mountain Biogenic Aerosol Study) campaign to study biogenic secondary organic aerosol (SOA) formation and organic aerosol (OA) aging. A wide range of equivalent atmospheric photochemical ages was sampled, from hours up to days (for O3 and NO3) or weeks (for OH). Ambient air processed by the OFR was typically sampled every 20–30 min, in order to determine how the availability of SOA precursor gases in ambient air changed with diurnal and synoptic conditions, for each of the three oxidants. More SOA was formed during nighttime than daytime for all three oxidants, indicating that SOA precursor concentrations were higher at night. At all times of day, OH oxidation led to approximately 4 times more SOA formation than either O3 or NO3 oxidation. This is likely because O3 and NO3 will only react with gases containing C = C bonds (e.g., terpenes) to form SOA but will not react appreciably with many of their oxidation products or any species in the gas phase that lacks a C = Cmore » bond (e.g., pinonic acid, alkanes). In contrast, OH can continue to react with compounds that lack C = C bonds to produce SOA. Closure was achieved between the amount of SOA formed from O3 and NO3 oxidation in the OFR and the SOA predicted to form from measured concentrations of ambient monoterpenes and sesquiterpenes using published chamber yields. This is in contrast to previous work at this site (Palm et al., 2016), which has shown that a source of SOA from semi- and intermediate-volatility organic compounds (S/IVOCs) 3.4 times larger than the source from measured VOCs is needed to explain the measured SOA formation from OH oxidation. This work suggests that those S/IVOCs typically do not contain C = C bonds. O3 and NO3 oxidation produced SOA with elemental O : C and H : C similar to the least-oxidized OA observed in local ambient air, and neither oxidant led to net mass loss at the highest exposures, in contrast to OH oxidation. An OH exposure in the OFR equivalent to several hours of atmospheric aging also produced SOA with O : C and H : C values similar to ambient OA, while higher aging (days–weeks) led to formation of SOA with progressively higher O : C and lower H : C (and net mass loss at the highest exposures). NO3 oxidation led to the production of particulate organic nitrates (pRONO2), while OH and O3 oxidation (under low NO) did not, as expected. As a result, these measurements of SOA formation provide the first direct comparison of SOA formation potential and chemical evolution from OH, O3, and NO3 oxidation in the real atmosphere and help to clarify the oxidation processes that lead to SOA formation from biogenic hydrocarbons.« less

Authors:
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)
OSTI Identifier:
1352991
Alternate Identifier(s):
OSTI ID: 1368377
Grant/Contract Number:  
SC0011105; SC0016559
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: 8; Journal ID: ISSN 1680-7324
Publisher:
Copernicus Publications, EGU
Country of Publication:
Germany
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES

Citation Formats

Palm, Brett B., Campuzano-Jost, Pedro, Day, Douglas A., Ortega, Amber M., Fry, Juliane L., Brown, Steven S., Zarzana, Kyle J., Dube, William, Wagner, Nicholas L., Draper, Danielle C., Kaser, Lisa, Jud, Werner, Karl, Thomas, Hansel, Armin, Gutiérrez-Montes, Cándido, and Jimenez, Jose L. Secondary organic aerosol formation from in situ OH, O3, and NO3 oxidation of ambient forest air in an oxidation flow reactor. Germany: N. p., 2017. Web. doi:10.5194/acp-17-5331-2017.
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Palm, Brett B., Campuzano-Jost, Pedro, Day, Douglas A., Ortega, Amber M., Fry, Juliane L., Brown, Steven S., Zarzana, Kyle J., Dube, William, Wagner, Nicholas L., Draper, Danielle C., Kaser, Lisa, Jud, Werner, Karl, Thomas, Hansel, Armin, Gutiérrez-Montes, Cándido, & Jimenez, Jose L. Secondary organic aerosol formation from in situ OH, O3, and NO3 oxidation of ambient forest air in an oxidation flow reactor. Germany. https://doi.org/10.5194/acp-17-5331-2017
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Palm, Brett B., Campuzano-Jost, Pedro, Day, Douglas A., Ortega, Amber M., Fry, Juliane L., Brown, Steven S., Zarzana, Kyle J., Dube, William, Wagner, Nicholas L., Draper, Danielle C., Kaser, Lisa, Jud, Werner, Karl, Thomas, Hansel, Armin, Gutiérrez-Montes, Cándido, and Jimenez, Jose L. Tue . "Secondary organic aerosol formation from in situ OH, O3, and NO3 oxidation of ambient forest air in an oxidation flow reactor". Germany. https://doi.org/10.5194/acp-17-5331-2017.
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@article{osti_1352991,
title = {Secondary organic aerosol formation from in situ OH, O3, and NO3 oxidation of ambient forest air in an oxidation flow reactor},
author = {Palm, Brett B. and Campuzano-Jost, Pedro and Day, Douglas A. and Ortega, Amber M. and Fry, Juliane L. and Brown, Steven S. and Zarzana, Kyle J. and Dube, William and Wagner, Nicholas L. and Draper, Danielle C. and Kaser, Lisa and Jud, Werner and Karl, Thomas and Hansel, Armin and Gutiérrez-Montes, Cándido and Jimenez, Jose L.},
abstractNote = {Ambient pine forest air was oxidized by OH, O3, or NO3 radicals using an oxidation flow reactor (OFR) during the BEACHON-RoMBAS (Bio–hydro–atmosphere interactions of Energy, Aerosols, Carbon, H2O, Organics and Nitrogen – Rocky Mountain Biogenic Aerosol Study) campaign to study biogenic secondary organic aerosol (SOA) formation and organic aerosol (OA) aging. A wide range of equivalent atmospheric photochemical ages was sampled, from hours up to days (for O3 and NO3) or weeks (for OH). Ambient air processed by the OFR was typically sampled every 20–30 min, in order to determine how the availability of SOA precursor gases in ambient air changed with diurnal and synoptic conditions, for each of the three oxidants. More SOA was formed during nighttime than daytime for all three oxidants, indicating that SOA precursor concentrations were higher at night. At all times of day, OH oxidation led to approximately 4 times more SOA formation than either O3 or NO3 oxidation. This is likely because O3 and NO3 will only react with gases containing C = C bonds (e.g., terpenes) to form SOA but will not react appreciably with many of their oxidation products or any species in the gas phase that lacks a C = C bond (e.g., pinonic acid, alkanes). In contrast, OH can continue to react with compounds that lack C = C bonds to produce SOA. Closure was achieved between the amount of SOA formed from O3 and NO3 oxidation in the OFR and the SOA predicted to form from measured concentrations of ambient monoterpenes and sesquiterpenes using published chamber yields. This is in contrast to previous work at this site (Palm et al., 2016), which has shown that a source of SOA from semi- and intermediate-volatility organic compounds (S/IVOCs) 3.4 times larger than the source from measured VOCs is needed to explain the measured SOA formation from OH oxidation. This work suggests that those S/IVOCs typically do not contain C = C bonds. O3 and NO3 oxidation produced SOA with elemental O : C and H : C similar to the least-oxidized OA observed in local ambient air, and neither oxidant led to net mass loss at the highest exposures, in contrast to OH oxidation. An OH exposure in the OFR equivalent to several hours of atmospheric aging also produced SOA with O : C and H : C values similar to ambient OA, while higher aging (days–weeks) led to formation of SOA with progressively higher O : C and lower H : C (and net mass loss at the highest exposures). NO3 oxidation led to the production of particulate organic nitrates (pRONO2), while OH and O3 oxidation (under low NO) did not, as expected. As a result, these measurements of SOA formation provide the first direct comparison of SOA formation potential and chemical evolution from OH, O3, and NO3 oxidation in the real atmosphere and help to clarify the oxidation processes that lead to SOA formation from biogenic hydrocarbons.},
doi = {10.5194/acp-17-5331-2017},
journal = {Atmospheric Chemistry and Physics (Online)},
number = 8,
volume = 17,
place = {Germany},
year = {Tue Apr 25 00:00:00 EDT 2017},
month = {Tue Apr 25 00:00:00 EDT 2017}
}
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  • DOI: 10.1021/es9029864

Volatility and lifetime against OH heterogeneous reaction of ambient isoprene-epoxydiols-derived secondary organic aerosol (IEPOX-SOA)
journal, January 2016

  • Hu, Weiwei; Palm, Brett B.; Day, Douglas A.
  • Atmospheric Chemistry and Physics, Vol. 16, Issue 18
  • DOI: 10.5194/acp-16-11563-2016

Comparison of different real time VOC measurement techniques in a ponderosa pine forest
journal, January 2013

  • Kaser, L.; Karl, T.; Schnitzhofer, R.
  • Atmospheric Chemistry and Physics, Vol. 13, Issue 5
  • DOI: 10.5194/acp-13-2893-2013

Particle mass yield in secondary organic aerosol formed by the dark ozonolysis of α-pinene
journal, January 2008

  • Shilling, J. E.; Chen, Q.; King, S. M.
  • Atmospheric Chemistry and Physics, Vol. 8, Issue 7
  • DOI: 10.5194/acp-8-2073-2008

O/C and OM/OC Ratios of Primary, Secondary, and Ambient Organic Aerosols with High-Resolution Time-of-Flight Aerosol Mass Spectrometry
journal, June 2008

  • Aiken, Allison C.; DeCarlo, Peter F.; Kroll, Jesse H.
  • Environmental Science & Technology, Vol. 42, Issue 12
  • DOI: 10.1021/es703009q

Influence of seed aerosol surface area and oxidation rate on vapor wall deposition and SOA mass yields: a case study with α -pinene ozonolysis
journal, January 2016

  • Nah, Theodora; McVay, Renee C.; Zhang, Xuan
  • Atmospheric Chemistry and Physics, Vol. 16, Issue 14
  • DOI: 10.5194/acp-16-9361-2016

Changes in organic aerosol composition with aging inferred from aerosol mass spectra
journal, January 2011

  • Ng, N. L.; Canagaratna, M. R.; Jimenez, J. L.
  • Atmospheric Chemistry and Physics, Vol. 11, Issue 13
  • DOI: 10.5194/acp-11-6465-2011

Oxidative aging and cloud condensation nuclei activation of laboratory combustion soot
journal, January 2015

Evolution of Organic Aerosols in the Atmosphere
journal, December 2009

HO x radical chemistry in oxidation flow reactors with low-pressure mercury lamps systematically examined by modeling
journal, January 2015

  • Peng, Z.; Day, D. A.; Stark, H.
  • Atmospheric Measurement Techniques, Vol. 8, Issue 11
  • DOI: 10.5194/amt-8-4863-2015

Chemical and microphysical characterization of ambient aerosols with the aerodyne aerosol mass spectrometer
journal, January 2007

  • Canagaratna, M. R.; Jayne, J. T.; Jimenez, J. L.
  • Mass Spectrometry Reviews, Vol. 26, Issue 2
  • DOI: 10.1002/mas.20115

Dependence of SOA oxidation on organic aerosol mass concentration and OH exposure: experimental PAM chamber studies
journal, January 2011

  • Kang, E.; Toohey, D. W.; Brune, W. H.
  • Atmospheric Chemistry and Physics, Vol. 11, Issue 4
  • DOI: 10.5194/acp-11-1837-2011

Biogenic VOC oxidation and organic aerosol formation in an urban nocturnal boundary layer: aircraft vertical profiles in Houston, TX
journal, January 2013

  • Brown, S. S.; Dubé, W. P.; Bahreini, R.
  • Atmospheric Chemistry and Physics, Vol. 13, Issue 22
  • DOI: 10.5194/acp-13-11317-2013

The gas-phase ozonolysis of β-caryophyllene (C15H24). Part I: an experimental study
journal, January 2009

  • Winterhalter, Richard; Herrmann, Frank; Kanawati, Basem
  • Physical Chemistry Chemical Physics, Vol. 11, Issue 21
  • DOI: 10.1039/b817824k

Rapid deposition of oxidized biogenic compounds to a temperate forest
journal, January 2015

  • Nguyen, Tran B.; Crounse, John D.; Teng, Alex P.
  • Proceedings of the National Academy of Sciences, Vol. 112, Issue 5
  • DOI: 10.1073/pnas.1418702112

Response of an aerosol mass spectrometer to organonitrates and organosulfates and implications for atmospheric chemistry
journal, March 2010

  • Farmer, D. K.; Matsunaga, A.; Docherty, K. S.
  • Proceedings of the National Academy of Sciences, Vol. 107, Issue 15
  • DOI: 10.1073/pnas.0912340107

Using Elemental Ratios to Predict the Density of Organic Material Composed of Carbon, Hydrogen, and Oxygen
journal, December 2011

  • Kuwata, Mikinori; Zorn, Soeren R.; Martin, Scot T.
  • Environmental Science & Technology, Vol. 46, Issue 2
  • DOI: 10.1021/es202525q

Autoxidation of Organic Compounds in the Atmosphere
journal, September 2013

  • Crounse, John D.; Nielsen, Lasse B.; Jørgensen, Solvejg
  • The Journal of Physical Chemistry Letters, Vol. 4, Issue 20
  • DOI: 10.1021/jz4019207

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

Hydrolysis of Organonitrate Functional Groups in Aerosol Particles
journal, December 2012

Hydrogen shift reactions in four methyl-buten-ol (MBO) peroxy radicals and their impact on the atmosphere
journal, December 2016

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

Time-resolved characterization of primary particle emissions and secondary particle formation from a modern gasoline passenger car
journal, January 2016

  • Karjalainen, Panu; Timonen, Hilkka; Saukko, Erkka
  • Atmospheric Chemistry and Physics, Vol. 16, Issue 13
  • DOI: 10.5194/acp-16-8559-2016

Effects of aging on organic aerosol from open biomass burning smoke in aircraft and laboratory studies
journal, January 2011

  • Cubison, M. J.; Ortega, A. M.; Hayes, P. L.
  • Atmospheric Chemistry and Physics, Vol. 11, Issue 23
  • DOI: 10.5194/acp-11-12049-2011

Aerosol Wall Losses in Electrically Charged Chambers
journal, January 1985

Chemistry of secondary organic aerosol: Formation and evolution of low-volatility organics in the atmosphere
journal, May 2008

Ozonolysis of β-Pinene: Temperature Dependence of Secondary Organic Aerosol Mass Fraction
journal, July 2008

  • Pathak, Ravikant; Donahue, Neil M.; Pandis, Spyros N.
  • Environmental Science & Technology, Vol. 42, Issue 14
  • DOI: 10.1021/es070721z

Diode laser-based cavity ring-down instrument for NO 3 , N 2 O 5 , NO, NO 2 and O 3 from aircraft
journal, January 2011

  • Wagner, N. L.; Dubé, W. P.; Washenfelder, R. A.
  • Atmospheric Measurement Techniques, Vol. 4, Issue 6
  • DOI: 10.5194/amt-4-1227-2011
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