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Title: Chemical aging of single and multicomponent biomass burning aerosol surrogate-particles by OH: Implications for cloud condensation nucleus activity

Abstract

Multiphase OH and O₃ oxidation reactions with atmospheric organic aerosol (OA) can influence particle physicochemical properties including composition, morphology, and lifetime. Chemical aging of initially insoluble or low soluble single-component OA by OH and O₃ can increase their water-solubility and hygroscopicity, making them more active as cloud condensation nuclei (CCN) and susceptible to wet deposition. However, an outstanding problem is whether the effects of chemical aging on their CCN activity are preserved when mixed with other organic or inorganic compounds exhibiting greater water-solubility. In this work, the CCN activity of laboratory-generated biomass burning aerosol (BBA) surrogate-particles exposed to OH and O₃ is evaluated by determining the hygroscopicity parameter, κ, as a function of particle type, mixing state, and OH/O₃ exposure applying a CCN counter (CCNc) coupled to an aerosol flow reactor (AFR). Levoglucosan (LEV), 4-methyl-5-nitrocatechol (MNC), and potassium sulfate (KS) serve as representative BBA compounds that exhibit different hygroscopicity, water solubility, chemical functionalities, and reactivity with OH radicals, and thus exemplify the complexity of mixed inorganic/organic aerosol in the atmosphere. The CCN activities of all of the particles were unaffected by O₃ exposure. Following exposure to OH, κ of MNC was enhanced by an order of magnitude, from 0.009 tomore » ~0.1, indicating that chemically-aged MNC particles are better CCN and more prone to wet deposition than pure MNC particles. No significant enhancement in κ was observed for pure LEV particles following OH exposure. κ of the internally-mixed particles was not affected by OH oxidation. Furthermore, the CCN activity of OH exposed MNC-coated KS particles is similar to the OH unexposed atomized 1:1 by mass MNC: KS binary-component particles. Our results strongly suggest that when OA is dominated by water-soluble organic carbon (WSOC) or inorganic ions, chemical aging has no significant impact on OA hygroscopicity. The organic compounds exhibiting low solubility behave as if they are infinitely soluble when mixed with a sufficient amount of water-soluble compounds. At and beyond this point, the particles' CCN activity is governed entirely by the water-soluble fraction and not influenced by the oxidized organic fraction. Our results have important implications for heterogeneous oxidation and its impact on cloud formation given that atmospheric aerosol is a complex mixture of organic and inorganic compounds exhibiting a wide-range of solubilities.« less

Authors:
 [1];  [2];  [2];  [1]
+ Show Author Affiliations
  1. State Univ. of New York (SUNY), Stony Brook, NY (United States). School of Marine and Atmospheric Sciences.
  2. Brookhaven National Lab. (BNL), Upton, NY (United States). Dept. of Environmental and Climate Sciences.
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER)
OSTI Identifier:
1190765
Report Number(s):
BNL-107841-2015-JA
Journal ID: ISSN 1680-7375; R&D Project: 2016-BNL-EE630EECA-Budg; KP1701000
Grant/Contract Number:  
SC00112704
Resource Type:
Accepted Manuscript
Journal Name:
Atmospheric Chemistry and Physics Discussions (Online)
Additional Journal Information:
Journal Name: Atmospheric Chemistry and Physics Discussions (Online); Journal Volume: 15; Journal Issue: 5; Journal ID: ISSN 1680-7375
Publisher:
European Geosciences Union
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES

Citation Formats

Thalman, R., Thalman, R., Wang, J., and Knopf, D. A. Chemical aging of single and multicomponent biomass burning aerosol surrogate-particles by OH: Implications for cloud condensation nucleus activity. United States: N. p., 2015. Web. doi:10.5194/acpd-15-6771-2015.
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Thalman, R., Thalman, R., Wang, J., & Knopf, D. A. Chemical aging of single and multicomponent biomass burning aerosol surrogate-particles by OH: Implications for cloud condensation nucleus activity. United States. https://doi.org/10.5194/acpd-15-6771-2015
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Thalman, R., Thalman, R., Wang, J., and Knopf, D. A. Fri . "Chemical aging of single and multicomponent biomass burning aerosol surrogate-particles by OH: Implications for cloud condensation nucleus activity". United States. https://doi.org/10.5194/acpd-15-6771-2015. https://www.osti.gov/servlets/purl/1190765.
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@article{osti_1190765,
title = {Chemical aging of single and multicomponent biomass burning aerosol surrogate-particles by OH: Implications for cloud condensation nucleus activity},
author = {Thalman, R. and Thalman, R. and Wang, J. and Knopf, D. A.},
abstractNote = {Multiphase OH and O₃ oxidation reactions with atmospheric organic aerosol (OA) can influence particle physicochemical properties including composition, morphology, and lifetime. Chemical aging of initially insoluble or low soluble single-component OA by OH and O₃ can increase their water-solubility and hygroscopicity, making them more active as cloud condensation nuclei (CCN) and susceptible to wet deposition. However, an outstanding problem is whether the effects of chemical aging on their CCN activity are preserved when mixed with other organic or inorganic compounds exhibiting greater water-solubility. In this work, the CCN activity of laboratory-generated biomass burning aerosol (BBA) surrogate-particles exposed to OH and O₃ is evaluated by determining the hygroscopicity parameter, κ, as a function of particle type, mixing state, and OH/O₃ exposure applying a CCN counter (CCNc) coupled to an aerosol flow reactor (AFR). Levoglucosan (LEV), 4-methyl-5-nitrocatechol (MNC), and potassium sulfate (KS) serve as representative BBA compounds that exhibit different hygroscopicity, water solubility, chemical functionalities, and reactivity with OH radicals, and thus exemplify the complexity of mixed inorganic/organic aerosol in the atmosphere. The CCN activities of all of the particles were unaffected by O₃ exposure. Following exposure to OH, κ of MNC was enhanced by an order of magnitude, from 0.009 to ~0.1, indicating that chemically-aged MNC particles are better CCN and more prone to wet deposition than pure MNC particles. No significant enhancement in κ was observed for pure LEV particles following OH exposure. κ of the internally-mixed particles was not affected by OH oxidation. Furthermore, the CCN activity of OH exposed MNC-coated KS particles is similar to the OH unexposed atomized 1:1 by mass MNC: KS binary-component particles. Our results strongly suggest that when OA is dominated by water-soluble organic carbon (WSOC) or inorganic ions, chemical aging has no significant impact on OA hygroscopicity. The organic compounds exhibiting low solubility behave as if they are infinitely soluble when mixed with a sufficient amount of water-soluble compounds. At and beyond this point, the particles' CCN activity is governed entirely by the water-soluble fraction and not influenced by the oxidized organic fraction. Our results have important implications for heterogeneous oxidation and its impact on cloud formation given that atmospheric aerosol is a complex mixture of organic and inorganic compounds exhibiting a wide-range of solubilities.},
doi = {10.5194/acpd-15-6771-2015},
journal = {Atmospheric Chemistry and Physics Discussions (Online)},
number = 5,
volume = 15,
place = {United States},
year = {Fri Mar 06 00:00:00 EST 2015},
month = {Fri Mar 06 00:00:00 EST 2015}
}
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Hygroscopic growth and critical supersaturations for mixed aerosol particles of inorganic and organic compounds of atmospheric relevance
journal, January 2006

  • Svenningsson, B.; Rissler, J.; Swietlicki, E.
  • Atmospheric Chemistry and Physics, Vol. 6, Issue 7
  • DOI: 10.5194/acp-6-1937-2006

Characteristics, sources and water-solubility of ambient submicron organic aerosol in springtime in Helsinki, Finland
journal, February 2013

Interannual variability in global biomass burning emissions from 1997 to 2004
journal, January 2006

  • van der Werf, G. R.; Randerson, J. T.; Giglio, L.
  • Atmospheric Chemistry and Physics, Vol. 6, Issue 11
  • DOI: 10.5194/acp-6-3423-2006

A review of surface ozone background levels and trends
journal, July 2004

Heterogeneous ice nucleation on particles composed of humic-like substances impacted by O 3
journal, January 2011

  • Wang, Bingbing; Knopf, Daniel A.
  • Journal of Geophysical Research, Vol. 116, Issue D3
  • DOI: 10.1029/2010JD014964

Heterogeneous ice nucleation and water uptake by field-collected atmospheric particles below 273 K: ICE NUCLEATION BY ATMOSPHERIC PARTICLES
journal, September 2012

  • Wang, Bingbing; Laskin, Alexander; Roedel, Tobias
  • Journal of Geophysical Research: Atmospheres, Vol. 117, Issue D21
  • DOI: 10.1029/2012JD017446

Effects of aerosol organics on cloud condensation nucleus (CCN) concentration and first indirect aerosol effect
journal, January 2008

  • Wang, J.; Lee, Y. -N.; Daum, P. H.
  • Atmospheric Chemistry and Physics, Vol. 8, Issue 21
  • DOI: 10.5194/acp-8-6325-2008

Oxidation of ambient biogenic secondary organic aerosol by hydroxyl radicals: Effects on cloud condensation nuclei activity: OXIDATION OF AMBIENT SOA AND CCN ACTIVITY
journal, November 2011

  • Wong, J. P. S.; Lee, A. K. Y.; Slowik, J. G.
  • Geophysical Research Letters, Vol. 38, Issue 22
  • DOI: 10.1029/2011GL049351

Aqueous-phase photooxidation of levoglucosan – a mechanistic study using aerosol time-of-flight chemical ionization mass spectrometry (Aerosol ToF-CIMS)
journal, January 2014

  • Zhao, R.; Mungall, E. L.; Lee, A. K. Y.
  • Atmospheric Chemistry and Physics, Vol. 14, Issue 18
  • DOI: 10.5194/acp-14-9695-2014
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