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Technical Note: Molecular characterization of aerosol-derived water soluble organic carbon using ultrahigh resolution electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry

by A S Wozniak, J E Bauer, R L Sleighter, R M Dickhut, P G Hatcher
Atmospheric Chemistry and Physics ()
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Despite the acknowledged relevance of aerosol- derivedwater-soluble organic carbon (WSOC) to climate and biogeochemical cycling, characterization of aerosol WSOC has been limited. Electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry (ESI FT-ICR MS) was utilized in this study to provide detailed molecular level characterization of the high molecular weight (HMW; m/z>223) component of aerosol-derived WSOC collected from rural sites in Virginia and New York, USA. More than 3000 peaks were detected by ESI FT-ICR MS within a m/z range of 223–600 for each sample. Approximately 86% (Vir- ginia) and 78% (New York) of these peaks were assigned molecular formulas using only carbon (C), hydrogen (H), oxygen (O), nitrogen (N), and sulfur (S) as elemental con- stituents. H/C and O/C molar ratios were plotted on van Krevelen diagrams and indicated a strong contribution of lignin-like and lipid-like compounds to the aerosol-derived WSOC samples. Approximately 1–4% of the peaks in the aerosol-derived WSOCmass spectra were classified as black carbon (BC) on the basis of double bond equivalents cal- culated from the assigned molecular formulas. In addition, several high-magnitude peaks in the mass spectra of sam- ples from both sites corresponded to molecular formulas pro- posed in previous secondary organic aerosol (SOA) labora- tory investigations indicating that SOAs are important con- stituents of the WSOC. Overall, ESI FT-ICR MS provides a level of resolution adequate for detailed compositional and source information of the HMW constituents of aerosol- derived WSOC.

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