Persistence of dissolved organic matter in lakes related to its molecular characteristics

Abstract

Whether intrinsic molecular properties or extrinsic factors such as environmental conditions control the decomposition of natural organic matter across soil, marine and freshwater systems has been subject to debate1,2,3. Comprehensive evaluations of the controls that molecular structure exerts on organic matter’s persistence in the environment have been precluded by organic matter’s extreme complexity4. Here we examine dissolved organic matter from 109 Swedish lakes using ultrahigh-resolution mass spectrometry and optical spectroscopy to investigate the constraints on its persistence in the environment. We find that degradation processes preferentially remove oxidized, aromatic compounds, whereas reduced, aliphatic and N-containing compounds are either resistant to degradation or tightly cycled and thus persist in aquatic systems. The patterns we observe for individual molecules are consistent with our measurements of emergent bulk characteristics of organic matter at wide geographic and temporal scales, as reflected by optical properties. We conclude that intrinsic molecular properties are an important control of overall organic matter reactivity.

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Figure 1: Non-metric multidimensional scaling of dissolved organic molecules from 109 Swedish lakes.
Figure 2: Molecular associations between individual molecules and optical indices and components.
Figure 3: Average chemical characteristics of molecules most strongly associated with each fluorescence component and optical index.

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Acknowledgements

We thank J. Johansson, I. Ulber, M. Friebe, K. Einarsdóttir, H. Osterholz, M. Seidel and K. Klaproth for assistance in the laboratory and with data analysis. We thank the Swedish Agricultural University for sample collection and running analyses and B. Denfeld and R. Müller for help with GIS data. Discussions with M. Berga, C. Gudasz and H. Peter improved the manuscript. We would also like to thank N. Catalán and F. Guillemette for comments on early versions of the manuscript. The sampling campaign was funded by the Swedish Environmental Protection Agency. The project was funded by the project Color of Water financed by the Swedish Research Council for Environment, Agricultural Sciences and Spatial Planning (FORMAS).

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All authors participated in conceiving the study. A.M.K. conducted solid-phase extractions with assistance from D.N.K. and T.D. and FT-ICR-MS analyses with guidance from T.D. A.M.K. conducted all statistical analyses, with comments and suggestions from D.N.K., L.J.T. and T.D. A.M.K. wrote the manuscript with significant assistance and comments from L.J.T. and D.N.K.

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Correspondence to Anne M. Kellerman.

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The authors declare no competing financial interests.

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Kellerman, A., Kothawala, D., Dittmar, T. et al. Persistence of dissolved organic matter in lakes related to its molecular characteristics. Nature Geosci 8, 454–457 (2015). https://doi.org/10.1038/ngeo2440

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