Identification of water-soluble organic carbon in non-urban aerosols using ultrahigh-resolution FT-ICR mass spectrometry: organic anions

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doi:10.1071/EN11167

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Identification of water-soluble organic carbon in non-urban aerosols using ultrahigh-resolution FT-ICR mass spectrometry: organic anions

Lynn R. Mazzoleni ^A ^B ^E , Parichehr Saranjampour ^A , Megan M. Dalbec ^C , Vera Samburova ^D , A. Gannet Hallar ^D , Barbara Zielinska ^D , Douglas H. Lowenthal ^D and Steve Kohl ^D

^A Michigan Technological University, Department of Chemistry, Houghton, MI 49931, USA.
^B Michigan Technological University, Atmospheric Sciences Program, Houghton, MI 49931, USA.
^C Michigan Technological University, Department of Civil and Environmental Engineering, Houghton, MI 49931, USA.
^D Desert Research Institute, Division of Atmospheric Science, Reno, NV 89512, USA.
^E Corresponding author. Email: lrmazzol@mtu.edu

Environmental Chemistry 9(3) 285-297 http://dx.doi.org/10.1071/EN11167
Submitted: 21 December 2011 Accepted: 13 April 2012 Published: 20 June 2012





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Environmental context. Aerosol water-soluble organic carbon is a complex mixture of thousands of organic compounds which may have a significant influence on the climate-relevant properties of atmospheric aerosols. Using ultrahigh resolution mass spectrometry, more than 4000 individual molecular formulas were identified in non-urban aerosol water-soluble organic carbon. A significant fraction of the assigned molecular formulas were matched to assigned molecular formulas of laboratory generated secondary organic aerosols.

Abstract. Water-soluble organic carbon (WSOC) is a complex mixture of thousands of organic compounds which may have significant influence on the climate-relevant properties of atmospheric aerosols. An improved understanding of the molecular composition of WSOC is needed to evaluate the effect of aerosol composition upon aerosol physical properties. In this work, ultrahigh-resolution Fourier transform–ion cyclotron resonance mass spectrometry (FT-ICR MS) was used to characterise aerosol WSOC collected during the summer of 2010 at the Storm Peak Laboratory (3210 m ASL) near Steamboat Springs, CO. Approximately 4000 molecular formulas were assigned in the mass range of 100–800 Da after negative-ion electrospray ionisation and more than 50 % of them contained nitrogen or sulfur. The double bond equivalents (DBEs) of the molecular formulas were inversely proportional to the O : C ratio, despite a relatively constant H : C ratio of ~1.5. Despite the range of DBE values, the elemental ratios and the high number of oxygen atoms per formula indicate that a majority of the compounds are aliphatic to olefinic in nature. These trends indicate significant non-oxidative accretion reaction pathways for the formation of high molecular weight WSOC components. In addition, a significant number of molecular formulas assigned in this work matched those previously identified as secondary organic aerosol components of monoterpene and sesquiterpene ozonolysis.

Additional keywords: atmospheric organic matter, electrospray ionisation, FT-ICR MS, high-resolution MS, humic-like substances, nitrooxy organosulfates, organonitrates, organosulfates, secondary organic aerosol.

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