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Gas hydrate decomposition recorded by authigenic barite at pockmark sites of the northern Congo Fan

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Abstract

The geochemical cycling of barium was investigated in sediments of pockmarks of the northern Congo Fan, characterized by surface and subsurface gas hydrates, chemosynthetic fauna, and authigenic carbonates. Two gravity cores retrieved from the so-called Hydrate Hole and Worm Hole pockmarks were examined using high-resolution pore-water and solid-phase analyses. The results indicate that, although gas hydrates in the study area are stable with respect to pressure and temperature, they are and have been subject to dissolution due to methane-undersaturated pore waters. The process significantly driving dissolution is the anaerobic oxidation of methane (AOM) above the shallowest hydrate-bearing sediment layer. It is suggested that episodic seep events temporarily increase the upward flux of methane, and induce hydrate formation close to the sediment surface. AOM establishes at a sediment depth where the upward flux of methane from the uppermost hydrate layer counterbalances the downward flux of seawater sulfate. After seepage ceases, AOM continues to consume methane at the sulfate/methane transition (SMT) above the hydrates, thereby driving the progressive dissolution of the hydrates “from above”. As a result the SMT migrates downward, leaving behind enrichments of authigenic barite and carbonates that typically precipitate at this biogeochemical reaction front. Calculation of the time needed to produce the observed solid-phase barium enrichments above the present-day depths of the SMT served to track the net downward migration of the SMT and to estimate the total time of hydrate dissolution in the recovered sediments. Methane fluxes were higher, and the SMT was located closer to the sediment surface in the past at both sites. Active seepage and hydrate formation are inferred to have occurred only a few thousands of years ago at the Hydrate Hole site. By contrast, AOM-driven hydrate dissolution as a consequence of an overall net decrease in upward methane flux seems to have persisted for a considerably longer time at the Worm Hole site, amounting to a few tens of thousands of years.

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Acknowledgments

We thank the master and crew of RV Meteor during cruise M47/3. For technical assistance on board ship and in the home laboratory, we are indebted to Anja Reitz, Karsten Enneking, Silvana Pape, and Susanne Siemer. We thank Michael Schweizer for performing the solid-phase analyses, and Volker Thiel for numerous fruitful discussions. The manuscript benefitted from very constructive and insightful reviews by G. Dickens and one anonymous referee, as well as comments by the editors M.T. Delafontaine and B.W. Flemming. This research was funded by the Deutsche Forschungsgemeinschaft DFG (RV Meteor cruise M47/3). We acknowledge further financial support from the Helmholtz Association (Alfred Wegener Institute, Bremerhaven). The full set of pore-water and solid-phase data is available via the geological data network PANGAEA (http://www.pangaea.de).

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Kasten, S., Nöthen, K., Hensen, C. et al. Gas hydrate decomposition recorded by authigenic barite at pockmark sites of the northern Congo Fan. Geo-Mar Lett 32, 515–524 (2012). https://doi.org/10.1007/s00367-012-0288-9

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