The formation process of gas hydrates in sedimentary matrices is of crucial importance for the physical and transport properties of the resulting aggregates. This process has never been observed in situ at submicron resolution. Here we report on synchrotron-based microtomographic studies by which the nucleation and growth processes of gas hydrate were observed at 276 K in various sedimentary matrices such as natural quartz (with and without admixtures of montmorillonite type clay) or glass beads with different surface properties, at varying water saturation. Both juvenile water and metastably gas-enriched water obtained from gas hydrate decomposition was used. Xenon gas was employed to enhance the density contrast between gas hydrate and the fluid phases involved. The nucleation sites can be easily identified and the various growth patterns are clearly established. In sediments under-saturated with juvenile water, nucleation starts at the water-gas interface resulting in an initially several micrometer thick gas hydrate film; further growth proceeds to form isometric single crystals of 10-20 mm size. The growth of gas hydrate from gas-enriched water follows a different pattern, via the nucleation in the bulk of liquid producing polyhedral single crystals. A striking feature in both cases is the systematic appearance of a fluid phase film of up to several micron thickness between gas hydrates and the surface of the quartz grains. These microstructural findings are relevant for future efforts of quantitative rock physics modeling of gas hydrates in sedimentary matrices and explain the anomalous attenuation of seismic/sonic waves.

Abstract. To date, very little is known about the distribution of natural gas hydrates in sedimentary matrices and its influence on the seismic properties of the host rock, in particular at low hydrate concentration. Digital rock physics offers a unique approach to this issue yet requires good quality, highresolution 3-D representations for the accurate modeling of petrophysical and transport properties. Although such models are readily available via in situ synchrotron radiation Xray tomography, the analysis of such data asks for complex workflows and high computational power to maintain valuable results. Here, we present a best-practice procedure complementing data from Chaouachi et al. (2015) with data postprocessing, including image enhancement and segmentation as well as exemplary numerical simulations of an acoustic wave propagation in 3-D using the derived results. A combination of the tomography and 3-D modeling opens a path to a more reliable deduction of properties of gas hydrate-bearing sediments without a reliance on idealized and frequently imprecise models.

We combined a noninvasive tomographic imaging technique with an invasive open-system core-flooding experiment and compared the results of the pre- and postflooded states of an experimental sandstone core sample from an ongoing field trial for carbon dioxide geosequestration. For the experiment, a rock core sample of 80 mL volume was taken from the 629 m Stuttgart Formation storage domain of a saline sandstone aquifer at the CCS research pilot plant Ketzin, Germany. Supercritical carbon dioxide and synthetical brine were injected under in situ reservoir p/T-conditions at an average flow rate of 0.1 mL/min for 256 h. X-ray computed microtomographic imaging was carried out before and after the core-flooding experiment at a spatial voxel resolution of 27 μm. No significant changes in microstructure were found at the tomographic imaging resolution including porosity and pore size distribution, except of an increase of depositional heterogeneous distribution of clay minerals in the pores. The digitized rock data were used as direct real microstructure input to the GeoDict software package, to simulate Navier-Stokes flow by a lattice Boltzmann equation solver. This procedure yielded 3D pressure and flow velocity fields, and revealed that the migration of clay particles decreased the permeability tensor probably due to clogging of pore openings.

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Abstract. Sediments containing gas hydrate dispersed in the pore space are known to show a characteristic seismic anomaly which is a high attenuation along with increasing seismic velocities. Currently, this observation cannot be fully explained albeit squirt-flow type mechanisms on the microscale have been speculated to be the cause. Recent major findings from in situ experiments, using the "gas in excess" and "water in excess" formation method, and coupled with high-resolution synchrotron-based X-ray micro-tomography, have revealed the systematic presence of thin water films between the quartz grains and the encrusting hydrate. The data obtained from these experiments underwent an image processing procedure to quantify the thicknesses and geometries of the aforementioned interfacial water films. Overall, the water films vary from sub-micrometer to a few micrometers in thickness. In addition, some of the water films interconnect through water bridges. This geometrical analysis is used to propose a new conceptual squirt flow model for hydrate bearing sediments. A series of numerical simulations is performed considering variations of the proposed model to study seismic attenuation caused by such thin water films. Our results support previous speculation that squirt flow can explain high attenuation at seismic frequencies in hydrate bearing sediments, but based on a conceptual squirt flow model which is geometrically different than those previously considered.