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Geochemical Perspectives Letters: Exchange catalysis during anaerobic methanotrophy revealed by 12CH2D2 and 13CH3D in methane

Jeanine L. Ash, Matthias Egger, Tina Treude, Issaku Kohl, Barry Cragg, R. John Parkes, Caroline Slomp, Barbara Sherwood Lollar and Edward D. Young

Abstract:  The anaerobic oxidation of methane (AOM) is a crucial component of the methane cycle, but quantifying its role in situ under dynamic environmental conditions remains challenging. We use sediment samples collected during IODP Expedition 347 to the Baltic Sea to show that relative abundances of 12CH2Dand 13CH3D in methane remaining after microbial oxidation are in internal, thermodynamic isotopic equilibrium, and we attribute this phenomenon to the reversibility of the initial step of AOM. These data suggest that 12CH2Dand 13CH3D together can identify the influence of anaerobic methanotrophy in environments where conventional bulk isotope ratios are ambiguous, and these findings may lead to new insights regarding the global significance of enzymatic back reaction in the methane cycle.

 

 

Pore water geochemistry along continental slopes north of the East Siberian Sea: inference of low methane concentrations

Clint M. Miller, Gerald R. Dickens, Martin Jakobsson, Carina Johansson, Andrey Koshurnikov, Matt O’Regan,
Francesco Muschitiello, Christian Stranne, and Carl-Magnus Mörth

Abstract. Continental slopes north of the East Siberian Sea potentially hold large amounts of methane (CH4) in sediments as gas hydrate and free gas. Although release of this CH4 to the ocean and atmosphere has become a topic of discussion, the region remains sparingly explored. Here we present pore water chemistry results from 32 sediment cores taken during Leg 2 of the 2014 joint Swedish–Russian–US Arctic Ocean Investigation of Climate–Cryosphere–Carbon Interactions (SWERUS-C3) expedition. The cores come from depth transects across the slope and rise extending between the Mendeleev and the Lomonosov ridges, north of Wrangel Island and the New Siberian Islands, respectively. Upward CH4 flux towards the seafloor, as inferred from profiles of dissolved sulfate (SO2−4), alkalinity, and the δ13C of dissolved inorganic carbon (DIC), is negligible at all stations east of 143◦ E longitude. In the upper
8 m of these cores, downward SO2−4 flux never exceeds 6.2 mol m−2 kyr−1, the upward alkalinity flux never exceeds
6.8 mol m−2 kyr−1, and δ13C composition of DIC (δ13CDIC) only moderately decreases with depth (−3.6 ‰ m−1 on
average). Moreover, upon addition of Zn acetate to pore water samples, ZnS did not precipitate, indicating a lack of dissolved H2S. Phosphate, ammonium, and metal profiles reveal that metal oxide reduction by organic carbon dominates the geochemical environment and supports very low organic carbon turnover rates. A single core on the Lomonosov Ridge differs, as diffusive fluxes for SO2−4 and alkalinity were 13.9 and 11.3 mol m−2 kyr−1, respectively, the δ13C-DIC gradient was 5.6 ‰ m−1, and Mn2+ reduction terminated within 1.3 m of the seafloor. These are among the first pore water results generated from this vast climatically sensitive region, and they imply that abundant CH4, including gas hydrates, do not characterize the East Siberian Sea slope or rise along the
investigated depth transects. This contradicts previous modeling and discussions, which due to the lack of data are almost entirely based on assumption.

Biogeosciences, 14, 2929–2953, 2017
https://doi.org/10.5194/bg-14-2929-2017
© Author(s) 2017. This work is distributed under
the Creative Commons Attribution 3.0 License