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Carbon isotope equilibration during sulphate-limited anaerobic oxidation of methane

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Abstract

Collectively, marine sediments comprise the largest reservoir of methane on Earth. The flux of methane from the sea bed to the overlying water column is mitigated by the sulphate-dependent anaerobic oxidation of methane by marine microbes within a discrete sedimentary horizon termed the sulphate–methane transition zone. According to conventional isotope systematics, the biological consumption of methane leaves a residue of methane enriched in 13C (refs 1, 2, 3). However, in many instances the methane within sulphate–methane transition zones is depleted in 13C, consistent with the production of methane, and interpreted as evidence for the intertwined anaerobic oxidation and production of methane4,5,6. Here, we report results from experiments in which we incubated cultures of microbial methane consumers with methane and low levels of sulphate, and monitored the stable isotope composition of the methane and dissolved inorganic carbon pools over time. Residual methane became progressively enriched in 13C at sulphate concentrations above 0.5 mM, and progressively depleted in 13C below this threshold. We attribute the shift to 13C depletion during the anaerobic oxidation of methane at low sulphate concentrations to the microbially mediated carbon isotope equilibration between methane and carbon dioxide. We suggest that this isotopic effect could help to explain the 13C-depletion of methane in subseafloor sulphate–methane transition zones.

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Figure 1: Typical geochemical and δ13C pore water profiles in marine sediments.
Figure 2: Experimental data (symbols) and model output (lines) for AOM culture incubations: Hydrate Ridge 1 (left column) and Amon Mud Volcano 1 (right column).
Figure 3: Methane carbon isotope patterns in diffusion-controlled marine sediments.

Change history

  • 07 February 2014

    In the version of this Letter originally published online, the Δ symbol was erroneously added to or missing from a few instances of ' Δδ 13 C CH 4 ' in the text and figures. This has been corrected in all versions of the Letter.

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Acknowledgements

We thank A. Boetius for providing the investigated seep sediments, G. Spence and the crew of the CCGV John P. Tully for shipboard support at Bullseye vent, G. Klockgether, M. Segl and K. Imhoff for analytical assistance, M. Y. Kellermann for providing the artwork on figures, J. Lipp and F. Schubotz for pore water data from various marine sediments and F. Widdel for insightful discussions. M.Y.Y. was supported by the Alexander von Humboldt Foundation and the European Research Council under the European Union’s Seventh Framework Programme—‘Ideas’ Specific Programme, ERC grant agreement No. 247153 (to K-U.H.); G.W. was funded by the Gottfried Wilhelm Leibniz Program of the Deutsche Forschungsgemeinschaft (A. Boetius); T.G. and G.W. were funded by the Deutsche Forschungsgemeinschaft (through the Research Center/Excellence Cluster MARUM-Center for Marine Environmental Sciences); T.H., G.W., B.B. and M.M.M.K. were funded through the Max-Planck Society. Any use of trade names is only for descriptive purposes and does not imply endorsement by the US Government.

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M.Y.Y., T.H., T.G., G.W. and M.E. designed and performed research; M.Y.Y., T.H., T.G., G.W. and J.W.P. analysed data; all authors contributed to manuscript preparation.

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Correspondence to Marcos Y. Yoshinaga or Gunter Wegener.

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Yoshinaga, M., Holler, T., Goldhammer, T. et al. Carbon isotope equilibration during sulphate-limited anaerobic oxidation of methane. Nature Geosci 7, 190–194 (2014). https://doi.org/10.1038/ngeo2069

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