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Subsurface porous rocks have the potential to store large volumes of hydrogen (H$_2$) required for transitioning towards a H$_2$-based energy future. Understanding the flow and trapping behavior of H$_2$ in subsurface storage systems, which is influenced by pore-scale heterogeneities inherent to subsurface rocks, is crucial to reliably evaluate the storage efficiency of a geological formation. In this work, we performed 3D X-ray imaging and flow experiments to investigate the impact of pore-scale heterogeneity on H$_2$ distribution after its cyclic injection (drainage) and withdrawal (imbibition) from a layered rock sample, characterized by varying pore and throat sizes. Our findings reveal that even subtle variations in rock structure and properties significantly influence H$_2$ displacement and storage efficiency. During drainage, H$_2$ follows a path consisting of large pores and throats, bypassing the majority of the low permeability rock layer consisting of smaller pores and throats. This bypassing substantially reduces the H$_2$ storage capacity. Moreover, due to the varying pore and throat sizes in the layered sample, depending on the experimental flow strategy, we observe a higher H$_2$ saturation after imbibition compared to drainage, which is counterintuitive and opposite to that observed in homogeneous rocks. These findings emphasize that small-scale rock heterogeneity, which is often unaccounted for in reservoir-scale models, can play a vital role in the displacement and trapping of H$_2$ in subsurface porous media.

The global commitment to achieve net-zero has led to increasing investment towards the production and usage of green hydrogen (H2).However, the massive quantity needed to match future demand will require new storage facilities. Underground storage of H2 is a potentially viable solution, but poses unique challenges due to the distinctive physical and chemical properties of H2, that have yet to be studied quantitatively in the subsurface environment. We have performed in situ X-ray flow experiments to investigate the fundamentals of pore-scale fluid displacement processes during H2 injection into an initially brine saturated Bentheimer sandstone sample. Two different injection schemes were followed, the displacement of H2 with H2-equilibrated brine and non-H2-equilibrated brine both at temperature and pressure conditions representative of deep underground reservoirs. H2 was found to be non-wetting to brine after both displacement cycles, with average contact angles between 53.72 and 52.72, respectively. We also found a higher recovery of H2 (43.1%) for non-H2-equilibrated brine compared to that of H2-equilibrated brine (31.6%), indicating potential dissolution of H2 in unequilibrated brine at reservoir conditions. Our results suggest that 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.