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Atmospheric Chemistry and Physics An interactive open-access journal of the European Geosciences Union
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Volume 14, issue 18
Atmos. Chem. Phys., 14, 10299–10314, 2014
© Author(s) 2014. This work is distributed under
the Creative Commons Attribution 3.0 License.
Atmos. Chem. Phys., 14, 10299–10314, 2014
© Author(s) 2014. This work is distributed under
the Creative Commons Attribution 3.0 License.

Research article 30 Sep 2014

Research article | 30 Sep 2014

A molecular-level approach for characterizing water-insoluble components of ambient organic aerosol particulates using ultrahigh-resolution mass spectrometry

A. S. Willoughby, A. S. Wozniak, and P. G. Hatcher A. S. Willoughby et al.
  • Department of Chemistry & Biochemistry, Old Dominion University, Norfolk, VA 23529, USA

Abstract. The chemical composition of organic aerosols in the atmosphere is strongly influenced by human emissions. The effect these have on the environment, human health, and climate change is determined by the molecular nature of these chemical species. The complexity of organic aerosol samples limits the ability to study the chemical composition, and therefore the associated properties and the impacts they have. Many studies have addressed the water-soluble fraction of organic aerosols and have had much success in identifying specific molecular formulas for thousands of compounds present. However, little attention is given to the water-insoluble portion, which can contain most of the fossil material that is emitted through human activity. Here we compare the organic aerosols present in water extracts and organic solvent extracts (pyridine and acetonitrile) of an ambient aerosol sample collected in a rural location that is impacted by natural and anthropogenic emission sources. A semiquantitative method was developed using proton nuclear magnetic resonance spectroscopy to determine that the amount of organic matter extracted by pyridine is comparable to that of water. Electrospray ionization Fourier transform ion cyclotron resonance mass spectra show that pyridine extracts a molecularly unique fraction of organic matter compared to water or acetonitrile, which extract chemically similar organic matter components. The molecular formulas unique to pyridine were less polar, more aliphatic, and reveal formulas containing sulfur to be an important component of insoluble aerosol organic matter.

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