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Unifying Concepts Linking Dissolved Organic Matter Composition to Persistence in Aquatic Ecosystems

  • Anne M. Kellerman*
    Anne M. Kellerman
    National High Magnetic Field Laboratory Geochemistry Group and Department of Earth, Ocean, and Atmospheric Science, Florida State University, Tallahassee, Florida 32306, United States
    *E-mail: [email protected]
    More by Anne M. Kellerman
    Orcidhttp://orcid.org/0000-0002-7348-4814
  • , 
  • François Guillemette
    François Guillemette
    National High Magnetic Field Laboratory Geochemistry Group and Department of Earth, Ocean, and Atmospheric Science, Florida State University, Tallahassee, Florida 32306, United States
    More by François Guillemette
  • , 
  • David C. Podgorski
    David C. Podgorski
    National High Magnetic Field Laboratory Geochemistry Group and Department of Earth, Ocean, and Atmospheric Science, Florida State University, Tallahassee, Florida 32306, United States
    More by David C. Podgorski
  • , 
  • George R. Aiken
    George R. Aiken
    U.S. Geological Survey, 3215 Marine Street, Boulder, Colorado 80303, United States
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  • , 
  • Kenna D. Butler
    Kenna D. Butler
    U.S. Geological Survey, 3215 Marine Street, Boulder, Colorado 80303, United States
    More by Kenna D. Butler
  • , and 
  • Robert G. M. Spencer
    Robert G. M. Spencer
    National High Magnetic Field Laboratory Geochemistry Group and Department of Earth, Ocean, and Atmospheric Science, Florida State University, Tallahassee, Florida 32306, United States
    More by Robert G. M. Spencer
Cite this: Environ. Sci. Technol. 2018, 52, 5, 2538–2548
Publication Date (Web):February 2, 2018
https://doi.org/10.1021/acs.est.7b05513
Copyright © 2018 American Chemical Society
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    Abstract

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    The link between composition and reactivity of dissolved organic matter (DOM) is central to understanding the role aquatic systems play in the global carbon cycle; yet, unifying concepts driving molecular composition have yet to be established. We characterized 37 DOM isolates from diverse aquatic ecosystems, including their stable and radiocarbon isotopes (δ13C-dissolved organic carbon (DOC) and Δ14C-DOC), optical properties (absorbance and fluorescence), and molecular composition (ultrahigh resolution mass spectrometry). Isolates encompassed end-members of allochthonous and autochthonous DOM from sites across the United States, the Pacific Ocean, and Antarctic lakes. Modern Δ14C-DOC and optical properties reflecting increased aromaticity, such as carbon specific UV absorbance at 254 nm (SUVA254), were directly related to polyphenolic and polycyclic aromatic compounds, whereas enriched δ13C-DOC and optical properties reflecting autochthonous end-members were positively correlated to more aliphatic compounds. Furthermore, the two sets of autochthonous end-members (Pacific Ocean and Antarctic lakes) exhibited distinct molecular composition due to differences in extent of degradation. Across all sites and end-members studied, we find a consistent shift in composition with aging, highlighting the persistence of certain biomolecules concurrent with degradation time.

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.est.7b05513.

    • Loadings of PARAFAC components (Supplementary Figure 1), split-half analysis of PARAFAC components (Supplementary Figure 2), examples of excitation–emission matrices (Supplementary Figure 3), Van Krevelen diagrams of molecular relationships with SUVA254 and biological index (Supplementary Figure 4), sample names, site types, and coordinates (Supplementary Table 1), loadings of PARAFAC components (Supplementary Table 2), and additional data that were used in the multivariate ordination (NMDS; Supplementary Table 3) (PDF)

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