[1] There is growing concern about the transfer of methane originating from water bodies to the atmosphere. Methane from sediments can reach the atmosphere directly via bubbles or indirectly via vertical turbulent transport. This work quantifies methane gas bubble dissolution using a combination of bubble modeling and acoustic observations of rising bubbles to determine what fraction of the methane transported by bubbles will reach the atmosphere. The bubble model predicts the evolving bubble size, gas composition, and rise distance and is suitable for almost all aquatic environments. The model was validated using methane and argon bubble dissolution measurements obtained from the literature for deep, oxic, saline water with excellent results. Methane bubbles from within the hydrate stability zone (typically below $500 m water depth in the ocean) are believed to form an outer hydrate rim. To explain the subsequent slow dissolution, a model calibration was performed using bubble dissolution data from the literature measured within the hydrate stability zone. The calibrated model explains the impressively tall flares (>1300 m) observed in the hydrate stability zone of the Black Sea. This study suggests that only a small amount of methane reaches the surface at active seep sites in the Black Sea, and this only from very shallow water areas (<100 m). Clearly, the Black Sea and the ocean are rather effective barriers against the transfer of bubble methane to the atmosphere, although substantial amounts of methane may reach the surface in shallow lakes and reservoirs.

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The Dnepr paleo-delta area in the NW Black Sea is characterized by an abundant presence of methane seeps. During the expeditions of May-June 2003 and within the EU-funded CRIMEA project, detailed multibeam, seismic and hydro-acoustic water-column investigations were carried out to study the relation between the spatial distribution of methane seeps, sea-floor morphology and sub-surface structures.2778 new methane seeps were detected on echosounding records in an area of 1540 km 2 . All seeps are located in the transition zone between the continental shelf and slope, in water depths of 66 to 825 m. The integration of the different geophysical datasets clearly indicates that methane seeps are not randomly distributed in this area, but are concentrated in specific locations.The depth limit for the majority of the detected seeps is 725 m water depth, which corresponds more or less with the stability limit for pure methane hydrate at the ambient bottom temperature (8.9 8C) in this part of the Black Sea. This suggests that, where gas hydrates are stable, they play the role of buffer for the upward migration of methane gas and thus prevent seepage of methane bubbles into the water column.Higher up on the margin, gas seeps are widespread, but accurate mapping illustrates that seeps occur preferentially in association with particular morphological and sub-surface features. On the shelf, the highest concentration of seeps is found in elongated depressions (pockmarks) above the margins of filled channels. On the continental slope where no pockmarks have been observed, seepage occurs along crests of sedimentary ridges. There, seepage is focussed by a parallel-stratified sediment cover that thins out towards the ridge crests. On the slope, seepage also appears in the vicinity of canyons (bottom, flanks and margins) or near the scarps of submarine landslides where mass-wasting breaches the fine-grained sediment cover that acts as a stratigraphic seal. The seismic data show the presence of a distinct bgas front,Q which has been used to map the depth of the free gas within the sea-floor sediments. The depth of this gas front is variable and locally domes up to the sea floor. Where the gas front approaches the seafloor, gas bubbles were detected in the water column. A regional map of the sub-surface depth of the gas front emphasises this bgas front-versus-seepQ relationship. The integration of all data sets indicates that the spatial distribution of methane seeps in the Dnepr paleo-delta is mainly controlled by the gas-hydrate stability zone as well as by stratigraphic and sedimentary factors. D

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The relation between acoustic seafloor backscatter and seep distribution is examined by integrating multibeam backscatter data and seep locations detected by single-beam echosounder. This study is further supported by side scan sonar recordings, high-resolution 5 kHz seismic data, pore-water analysis, grain-size analysis and visual seafloor observations. The datasets were acquired during the 2003 and 2004 expeditions of the EC-funded CRIMEA project in the Dnepr paleo-delta area, northwestern Black Sea.More than 600 active methane seeps were hydro-acoustically detected within a small (3.96 km by 3.72 km) area on the continental shelf of the Dnepr paleo-delta in water depths ranging from -72 m to -156 m. Multibeam and side scan sonar recordings show backscatter patterns that are clearly associated with seepage or with a present dune area. Seeps generally occur within medium-to highbackscatter areas which often coincide with pockmarks.High-resolution seismic data reveal the presence of an undulating gas front, i.e. the top of the free gas in the subsurface, which domes up towards and intersects the seafloor at locations where gas seeps and medium-to high-backscatter values are detected. Pore-water analysis of 4 multi-cores, taken at different backscatter intensity sites, shows a clear correlation between backscatter intensity and dissolved methane fluxes. All analyzed chemical species indicate increasing anaerobic oxidation of methane (AOM) from medium-to high-backscatter locations. This is confirmed by visual seafloor observations, showing bacterial mats and authigenic carbonates formed by AOM. Grain-size analysis of the 4 multi-cores only reveals negligible variations between the different backscatter sites.Integration of all datasets leads to the conclusion that the observed backscatter patterns are the result of ongoing methane seepage and the precipitation of methane-derived authigenic carbonates (MDACs) caused by AOM. The carbonate formation also appears to lead to a gradual (self-)sealing of the seeps by cementing fluid pathways/horizons followed by a relocation of the bubble-releasing locations. KeywordsMethane seeps; acoustic seafloor backscatter; anaerobic oxidation of methane; bacterial mats; pockmarks; methane-derived authigenic carbonates

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