Characterizing the wettability of hydrogen (H₂)–methane (CH₄) mixtures in subsurface reservoirs is the first step towards understanding containment and transport properties for underground hydrogen storage (UHS). In this study, we investigate the static contact angles of H₂–CH₄ mixtures, in contact with brine and Bentheimer sandstone rock using a captive-bubble cell device at different pressures, temperatures and brine salinity values. It is found that, under the studied conditions, H₂ and CH₄ show comparable wettability behaviour with contact angles ranging between [25°–45°]; and consequently their mixtures behave similar to the pure gas systems, independent of composition, pressure, temperature and salinity. For the system at rest, the acting buoyancy and surface forces allow for theoretical sensitivity analysis for the captive-bubble cell approach to characterize the wettability. Moreover, it is theoretically validated that under similar Bond numbers and similar bubble sizes, the contact angles of H₂ and CH₄ bubbles and their mixtures are indeed comparable. Consequently, in large-scale subsurface storage systems where buoyancy and capillary are the main acting forces, H₂, CH₄ and their mixtures will have similar wettability characteristics.

Subsurface porous formations provide large capacities for underground hydrogen storage (UHS). Successful utilization of these porous reservoirs for UHS depends on accurate quantification of the hydrogen transport characteristics at continuum (macro) scale, specially in contact with other reservoir fluids. Relative-permeability and capillary-pressure curves are among the macro-scale transport characteristics which play crucial roles in quantification of the storage capacity and efficiency. For a given rock sample, these functions can be determined if pore-scale (micro-scale) surface properties, specially contact angles, are known. For hydrogen/brine/rock system, these properties are yet to a large extent unknown. In this study, we characterize the contact angles of hydrogen in contact with brine and Bentheimer and Berea sandstones at various pressure, temperature, and brine salinity using captive-bubble method. The experiments are conducted close to the in-situ conditions, which resulted in water-wet intrinsic contact angles, about 25 to 45 degrees. Moreover, no meaningful correlation was found with changing tested parameters. We monitor the bubbles over time and report the average contact angles with their minimum and maximum variations. Given rock pore structures, using the contact angles reported in this study, one can define relative-permeability and capillary-pressure functions for reservoir-scale simulations and storage optimization.