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Published September 4, 2012 | Published + Supplemental Material
Journal Article Open

Organosulfates as Tracers for Secondary Organic Aerosol (SOA) Formation from 2‑Methyl-3-Buten-2-ol (MBO) in the Atmosphere


2-Methyl-3-buten-2-ol (MBO) is an important biogenic volatile organic compound (BVOC) emitted by pine trees and a potential precursor of atmospheric secondary organic aerosol (SOA) in forested regions. In the present study, hydroxyl radical (OH)-initiated oxidation of MBO was examined in smog chambers under varied initial nitric oxide (NO) and aerosol acidity levels. Results indicate measurable SOA from MBO under low-NO conditions. Moreover, increasing aerosol acidity was found to enhance MBO SOA. Chemical characterization of laboratory-generated MBO SOA reveals that an organosulfate species (C_5H_(12)O_6S, MW 200) formed and was substantially enhanced with elevated aerosol acidity. Ambient fine aerosol (PM_(2.5)) samples collected from the BEARPEX campaign during 2007 and 2009, as well as from the BEACHON-RoMBAS campaign during 2011, were also analyzed. The MBO-derived organosulfate characterized from laboratory-generated aerosol was observed in PM_(2.5) collected from these campaigns, demonstrating that it is a molecular tracer for MBO-initiated SOA in the atmosphere. Furthermore, mass concentrations of the MBO-derived organosulfate are well correlated with MBO mixing ratio, temperature, and acidity in the field campaigns. Importantly, this compound accounted for an average of 0.25% and as high as 1% of the total organic aerosol mass during BEARPEX 2009. An epoxide intermediate generated under low-NO conditions is tentatively proposed to produce MBO SOA.

Additional Information

© 2012 American Chemical Society. ACS AuthorChoice. Received: April 26, 2012. Revised: July 31, 2012. Accepted: July 31, 2012. Publication Date (Web): July 31, 2012. The authors declare no competing financial interest. This study was supported by an U.S. EPA contract (EP-W-09-023) to the University of North Carolina. The U.S. Environmental Protection Agency through its Office of Research and Development collaborated in the research described here under Contract EP-D-10-070 to Alion Science and Technology. The manuscript is subjected to external peer review and has been not been cleared for publication. Mention of trade names or commercial products does not constitute endorsement or recommendation. The BEARPEX measurements were supported by an NSF grant ATM-0922562 to the University of California, Berkeley, and ATM-0904203 to the University of California, San Diego. The BEACHON-RoMBAS measurements were supported by NSF sponsorship of the National Center for Atmospheric Research (NCAR). UPLC/ESI-HR-QTOFMS analyses were conducted in the UNC-CH Biomarker Mass Facility located within the Department of Environmental Sciences and Engineering, which is a part of the UNC-CH Center for Environmental Health and Susceptibility and is supported by NIEHS (Grant 5P20-ES10126). J.D.S. was supported in part by the Electric Power Research Institute (EPRI). Thanks to Ying-Hsuan Lin for helping to operate the UPLC/(−)ESI-HR-Q-TOFMS instrument. The meteorological measurements from BEACHON-RoMBAS were performed by Andrew A. Turnipseed. The IC measurements for BEARPEX 2009 were performed by M. P. Madsen. P.C.J., D.A.D., and J.L.J. were supported by NSF ATM-0919189 and DOE (BER/ASR Program)DE-SC0006035 and DESC0006711. GC-FID measurements by Texas A&M were funded by NSF ATM -0934345. Measurements conducted by the University of Innsbruck were supported by the Austrian Science Fund (FWF): L.K. is a recipient of a DOC-fFORTE-fellowship of the Austrian Academy of Sciences at the Institute of Ion Physics and Applied Physics.

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