Subsurface porous rocks hold significant hydrogen (H₂) storage potential to support an H₂-based energy future. Understanding H₂ flow and trapping in subsurface rocks is crucial to reliably evaluate their storage efficiency. In this work, we perform cyclic H₂ flow visualization experiments on a layered rock sample with varying pore and throat sizes. During drainage, H₂ follows a path consisting of large pores and throats, through a low permeability rock layer, substantially reducing H₂ storage capacity. Moreover, due to the rock heterogeneity and depending on the experimental flow strategy, imbibition unexpectedly results in higher H₂ saturation compared to drainage. These results emphasize that small-scale rock heterogeneity, which is often unaccounted for in reservoir-scale models, plays a vital role in H₂ displacement and trapping in subsurface porous media, with implications for efficient storage strategies.

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Hypothesis

Underground hydrogen (H2) storage is a potentially viable solution for large-scale cyclic H2 storage; however, the behavior of H2 at subsurface pressure and temperature conditions is poorly known. This work investigates if the pore-scale displacement processes in H2-brine systems in a porous sandstone can be sufficiently well defined to enable effective and economic storage operations. In particular, this study investigates trapping, dissolution, and wettability of H2-brine systems at the pore-scale, at conditions that are realistic for subsurface H2 storage.

Experiments

We have performed in situ X-ray imaging during a flow experiment to investigate pore-scale processes during H2 injection and displacement in a brine saturated Bentheimer sandstone sample at temperature and pressure conditions representative of underground reservoirs. Two injection schemes were followed for imbibition: displacement of H2 with H2-equilibrated brine and with non-H2-equilibrated brine. The results from the two cycles were compared with each other.

Findings

The sandstone was found to be wetting to the brine and non-wetting to H2 after both displacement cycles, with average contact angles of 54° and 53°, for H2-equilibrated and non-H2-equilibrated brine, respectively. We also found a higher recovery of H2 (43.1%) when displaced with non-H2-equilibrated brine compared to that of H2-equilibrated brine (31.6%), indicating potential dissolution of H2 in the unequilibrated, imbibing brine at reservoir conditions. Our results suggest that underground H2 storage may indeed be a suitable strategy for energy storage, but considerable further research is needed to fully comprehend the pore-scale interactions at reservoir conditions.@en