Using X-ray computed tomography and pore-scale numerical modeling to study the role of heterogeneous rock surface wettability on hydrogen-brine two-phase flow in underground hydrogen storage

Underground hydrogen storage (UHS) is receiving increasing attention to address the challenges in hydrogen storage. A crucial aspect of UHS is understanding the transport of hydrogen in subsurface porous media. In this work, hydrogen core flooding experiments were conducted in a sandstone sample and then the pore-scale distribution of hydrogen and brine was visualized using high-resolution X-ray micro-computed tomography (micro-CT). After CT image processing, we measured the surface contact angles (CAs) on rock surfaces and found that the measured CAs followed a log-normal distribution. To investigate the influence of rock surface wettability on the transport properties in the hydrogen-brine-sandstone system, the lattice Boltzmann (LB) method was used to simulate two-phase flows with different surface CA distributions; hydrogen-brine relative permeability and capillary pressure curves through the primary drainage, imbibition, and secondary drainage processes were obtained by LB simulations. X-ray CT scanning showed that hydrogen resided in both large pores and small pores and pore throats after the primary drainage process (i.e., hydrogen displacing brine), whereas after the imbibition process (i.e., brine displacing hydrogen) hydrogen stayed primarily in large pores where the capillary pressure barriers were low. The LB two-phase flow modeling illustrated that water's relative permeability increased whereas hydrogen's relative permeability decreased when the core flooding moved from primary drainage to imbibition; in contrast, when the core flooding moved from imbibition to secondary drainage, water's relative permeability decreased whereas hydrogen's relative permeability increased. Decreasing the surface CA increased the capillary pressure and reduced the hydrogen residual rate, which indicates high hydrogen retrievability and thus is favorable for UHS practice. The change in CA's standard deviation did not cause noticeable changes in water's relative permeability curves, whereas it resulted in noticeable changes in hydrogen's relative permeability curves. This work is the first study that utilizes X-ray micro-CT scanning and pore-scale multiphase flow modeling to quantitatively and comprehensively investigate hydrogen-brine two-phase flow properties under different rock surface wettability distributions. The research findings from this study will advance the understanding of hydrogen transport in an underground storage system and provide essential data for large-scale field studies in UHS.