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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 and 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 ofmore » 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 number of water-soluble compounds. At and beyond this point, the particles' CCN activity is governed entirely by the water-soluble fraction and is 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:
; ; ;
Publication Date:
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER)
OSTI Identifier:
1215767
Grant/Contract Number:  
AC02098CH10886
Resource Type:
Published Article
Journal Name:
Atmospheric Chemistry and Physics (Online)
Additional Journal Information:
Journal Name: Atmospheric Chemistry and Physics (Online) Journal Volume: 15 Journal Issue: 17; Journal ID: ISSN 1680-7324
Publisher:
Copernicus Publications, EGU
Country of Publication:
Germany
Language:
English

Citation Formats

Slade, J. H., 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. Germany: N. p., 2015. Web. doi:10.5194/acp-15-10183-2015.
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Slade, J. H., 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. Germany. https://doi.org/10.5194/acp-15-10183-2015
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Slade, J. H., Thalman, R., Wang, J., and Knopf, D. A. Mon . "Chemical aging of single and multicomponent biomass burning aerosol surrogate particles by OH: implications for cloud condensation nucleus activity". Germany. https://doi.org/10.5194/acp-15-10183-2015.
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@article{osti_1215767,
title = {Chemical aging of single and multicomponent biomass burning aerosol surrogate particles by OH: implications for cloud condensation nucleus activity},
author = {Slade, J. H. 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 and 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 number of water-soluble compounds. At and beyond this point, the particles' CCN activity is governed entirely by the water-soluble fraction and is 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/acp-15-10183-2015},
journal = {Atmospheric Chemistry and Physics (Online)},
number = 17,
volume = 15,
place = {Germany},
year = {Mon Sep 14 00:00:00 EDT 2015},
month = {Mon Sep 14 00:00:00 EDT 2015}
}
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  • Journal of Geophysical Research: Atmospheres, Vol. 104, Issue D9
  • DOI: 10.1029/1999JD900073

Nitrated phenols in the atmosphere: a review
journal, January 2005

Aging of Organic Aerosol: Bridging the Gap Between Laboratory and Field Studies
journal, May 2007

Laboratory study of the effect of oxalic acid on the cloud condensation nuclei activity of mineral dust aerosol
journal, January 2012

Smoking Rain Clouds over the Amazon
journal, February 2004

Importance of aerosol composition, mixing state, and morphology for heterogeneous ice nucleation: A combined field and laboratory approach: HETEROGENEOUS ICE NUCLEATION
journal, March 2012

  • Baustian, Kelly J.; Cziczo, Daniel J.; Wise, Matthew E.
  • Journal of Geophysical Research: Atmospheres, Vol. 117, Issue D6
  • DOI: 10.1029/2011JD016784

Water soluble organic compounds formed by oxidation of soot
journal, April 2002

Detailed heterogeneous chemistry in an urban plume box model: reversible co-adsorption of O 3 , NO 2 , and H 2 O on soot coated with benzo[a]pyrene
journal, January 2009

  • Springmann, M.; Knopf, D. A.; Riemer, N.
  • Atmospheric Chemistry and Physics, Vol. 9, Issue 19
  • DOI: 10.5194/acp-9-7461-2009

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

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

Modification of cloud condensation nucleus activity of organic aerosols by hydroxyl radical heterogeneous oxidation
journal, October 2009

The OH-initiated atmospheric reaction mechanism and kinetics for levoglucosan emitted in biomass burning
journal, November 2013

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
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