Newly developed high-speed, synchrotron-based X-ray computed microtomography enabled us to directly image pore-scale displacement events in porous rock in real time. Common approaches to modeling macroscopic fluid behavior are phenomenological, have many shortcomings, and lack consistent links to elementary porescale displacement processes, such as Haines jumps and snap-off. Unlike the common singular pore jump paradigm based on observations of restricted artificial capillaries, we found that Haines jumps typically cascade through 10-20 geometrically defined pores per event, accounting for 64% of the energy dissipation. Real-time imaging provided a more detailed fundamental understanding of the elementary processes in porous media, such as hysteresis, snapoff, and nonwetting phase entrapment, and it opens the way for a rigorous process for upscaling based on thermodynamic models.hydrology | oil recovery | multiphase flow

Detailed knowledge of the extent of post-genetic modifications affecting shallow submarine hydrocarbons fueled from the deep subsurface is fundamental for evaluating source and reservoir properties. We investigated gases from a submarine high-flux seepage site in the anoxic Eastern Black Sea in order to elucidate molecular and isotopic alterations of low-molecular-weight hydrocarbons (LMWHC) associated with upward migration through the sediment and precipitation of shallow gas hydrates. For this, nearsurface sediment pressure cores and free gas venting from the seafloor were collected using autoclave technology at the Batumi seep area at 845 m water depth within the gas hydrate stability zone. Vent gas, gas from pressure core degassing, and from hydrate dissociation were strongly dominated by methane (> 99.85 mol.% of ∑[C 1 -C 4 , CO 2 ]). Molecular ratios of LMWHC (C 1 /[C 2 + C 3 ] > 1000) and stable isotopic compositions of methane (δ 13 C = − 53.5‰ V-PDB; D/H around − 175‰ SMOW) indicated predominant microbial methane formation. C 1 /C 2+ ratios and stable isotopic compositions of LMWHC distinguished three gas types prevailing in the seepage area. Vent gas discharged into bottom waters was depleted in methane by > 0.03 mol.% (∑[C 1 -C 4 , CO 2 ]) relative to the other gas types and the virtual lack of 14 C-CH 4 indicated a negligible input of methane from degradation of fresh organic matter. Of all gas types analyzed, vent gas was least affected by molecular fractionation, thus, its origin from the deep subsurface rather than from decomposing hydrates in near-surface sediments is likely. As a result of the anaerobic oxidation of methane, LMWHC in pressure cores in top sediments included smaller methane fractions [0.03 mol.% ∑(C 1 -C 4 , CO 2 )] than gas released from pressure cores of more deeply buried sediments, where the fraction of methane was maximal due to its preferential incorporation in hydrate lattices. No indications for stable carbon isotopic fractionations of methane during hydrate crystallization from vent gas were found. Enrichments of 14 C-CH 4 (1.4 pMC) in short cores relative to lower abundances (max. 0.6 pMC) in gas from long cores and gas hydrates substantiates recent methanogenesis utilizing modern organic matter deposited in top sediments of this high-flux hydrocarbon seep area.

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Due to experimental difficulties grain size distributions of gas hydrate crystallites are largely unknown in natural samples. For the first time, we were able to determine grain size distributions of six natural gas hydrates for samples retrieved from the Gulf of Mexico and from Hydrate Ridge offshore Oregon from varying depths. High‐energy synchrotron radiation provides high photon fluxes as well as high penetration depth and thus allows for investigation of bulk sediment samples. The gas hydrate crystallites appear to be (log‐) normally distributed in the natural samples and to be of roughly globular shape. The mean grain sizes are in the range from 300–600 μm with a tendency for bigger grains to occur in greater depth, possibly indicating a difference in the formation age. Laboratory produced methane hydrate, starting from ice and aged for 3 weeks, shows half a log‐normal curve with a mean value of ∼40 μm. This one order‐of‐magnitude smaller grain sizes suggests that care must be taken when transposing grain‐size sensitive (petro‐)physical data from laboratory‐made gas hydrates to natural settings.

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