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Ambient Gas-Particle Partitioning of Tracers for Biogenic Oxidation

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Download Hi-Res ImageDownload to MS-PowerPointCite This:Environ. Sci. Technol. 2016, 50, 18, 9952-9962
    Article

    Ambient Gas-Particle Partitioning of Tracers for Biogenic Oxidation
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    † Department. of Environmental Science, Policy, and Management, University of California, Berkeley, California 94720, United States
    ‡ Aerosol Dynamics Inc., Berkeley, California 94710, United States
    § Department of Civil and Environmental Engineering, University of California, Berkeley, California 94720, United States
    ∥ School of Engineering and Applied Sciences, Harvard University, Cambridge, Massachusetts 01451, United States
    ⊥ Department of Earth and Planetary Sciences, Harvard University, Cambridge, Massachusetts 01451, United States
    # Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland, Washington 99352, United States
    ∇ Department of Chemistry & Biochemistry and Cooperative Institute for Research in Environmental Sciences (CIRES), University of Colorado, Boulder, Colorado 80309, United States
    ○ Department of Environmental Sciences and Engineering, University of North Carolina, Chapel Hill, North Carolina 27599, United States
    ◆ Instituto Nacional de Pesquisas da Amazonia, Manaus, Amazonas, Brazil, 69060-001
    Atmospheric Research & Analysis, Inc., Cary, North Carolina 27513, United States
    ∞ Universidade do Estado do Amazonas, Manaus, Amazonas, Brazil, 69735-000
    ∏ Universidade de São Paulo, São Paulo, Brazil, 05508-020
    *E-mail: [email protected]
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    Environmental Science & Technology

    Cite this: Environ. Sci. Technol. 2016, 50, 18, 9952–9962
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    https://doi.org/10.1021/acs.est.6b01674
    Published August 23, 2016
    Copyright © 2016 American Chemical Society
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    Abstract

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    Exchange of atmospheric organic compounds between gas and particle phases is important in the production and chemistry of particle-phase mass but is poorly understood due to a lack of simultaneous measurements in both phases of individual compounds. Measurements of particle- and gas-phase organic compounds are reported here for the southeastern United States and central Amazonia. Polyols formed from isoprene oxidation contribute 8% and 15% on average to particle-phase organic mass at these sites but are also observed to have substantial gas-phase concentrations contrary to many models that treat these compounds as nonvolatile. The results of the present study show that the gas-particle partitioning of approximately 100 known and newly observed oxidation products is not well explained by environmental factors (e.g., temperature). Compounds having high vapor pressures have higher particle fractions than expected from absorptive equilibrium partitioning models. These observations support the conclusion that many commonly measured biogenic oxidation products may be bound in low-volatility mass (e.g., accretion products, inorganic–organic adducts) that decomposes to individual compounds on analysis. However, the nature and extent of any such bonding remains uncertain. Similar conclusions are reach for both study locations, and average particle fractions for a given compound are consistent within ∼25% across measurement sites.

    Copyright © 2016 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.est.6b01674.

    • Details on instrument operation and capabilities, descriptions of measurement locations, and discussion of models used in this work is provided in the Supporting Information. This information includes results impacting the interpretation and use of these data (e.g., model outputs, instrument validation, etc.) Additional detail is also provided on some results, including further exploration of partitioning correlations between compounds and sites, and tables providing average partitioning parameters for all observed compounds (data used in Figure 4) (PDF)

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    Cite this: Environ. Sci. Technol. 2016, 50, 18, 9952–9962
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