Microbial methane formation in deep aquifers associated with the sediment burial history at a coastal site

Abstract. Elucidating the mechanisms underlying microbial methane formation in subsurface environments is essential to understanding the global carbon cycle. This study examined how microbial methane formation (i.e., methanogenesis) occurs in natural-gas-bearing sedimentary aquifers throughout the sediment burial history. Water samples collected from six aquifers of different depths exhibited ascending vertical gradients in salinity from brine to fresh water and in temperature from mesophilic to psychrophilic conditions. Analyses of gas and water isotopic ratios and microbial communities indicated the predominance of methanogenesis via CO2 reduction. However, the hydrogen isotopic ratio of water changed along the depth and salinity gradient, whereas the ratio of methane changed little, suggesting that in situ methanogenesis in shallow sediments does not significantly contribute to methane in the aquifers. The population of methane-producing microorganisms (methanogens) was highest in the deepest saline aquifers, where the water temperature, salinity, and total organic carbon content of the adjacent mud sediments were the highest. Cultivation of the dominant hydrogenotrophic methanogens in the aquifers showed that the methanogenesis rate was maximized at the temperature corresponding to that of the deepest aquifer. These results suggest that high-temperature conditions in deeply buried sediments are associated with enhanced in situ methanogenesis and that methane that forms in the deepest aquifer migrates upward into the shallower aquifers by diffusion.