The origin of methane in the East Siberian Arctic Shelf unraveled with triple isotope analysis
Abstract. Methane (CH4) is a strong greenhouse gas emitted by human activity and natural processes that are highly sensitive to climate change. The Arctic Ocean, especially the East Siberian Arctic Shelf (ESAS) overlays large areas of subsea permafrost that is degrading. The release of large amount of CH4 originally stored or formed there could create a strong positive climate feedback. Large scale CH4 super-saturation has been observed in the ESAS waters, pointing to leakages of CH4 through the sea floor and possibly to the atmosphere, but the origin of this gas is still debated. Here, we present CH4 concentration and triple isotope data analyzed on gas extracted from sediment and water sampled over the shallow ESAS from 2007 to 2013. We find high concentrations (up to 500 μM) of CH4 in the pore water of the partially thawed subsea permafrost of this region. For all sediment cores, both hydrogen and carbon CH4 isotope data reveal the predominant presence of CH4 that is not of thermogenic/natural gas origin as it has long been thought, but resultant from microbial CH4 formation using as primary substrate glacial water and old organic matter preserved in the subsea permafrost or below. Radiocarbon data demonstrate that the CH4 present in the ESAS sediment is of Pleistocene age or older, but a small contribution of highly 14C-enriched CH4, from unknown origin, prohibits precise age determination for one sediment core and in the water column. Our data suggest that at locations where bubble plumes have been observed, CH4 can escape anaerobic oxidation in the surface sediment. CH4 will then rapidly migrate through the very shallow water column of the ESAS to escape to the atmosphere generating a positive radiative feedback.