Ostwald Ripening in Underground Gas Storage

Abstract

Underground gas storage is central to both climate mitigation and energy transition strategies, supporting both long-term carbon sequestration and seasonal hydrogen storage. A key mechanism governing the fate of injected gases is Ostwald ripening, the curvature-driven mass transfer between trapped gas ganglia in porous media. While ripening is well understood in open systems, its behavior in geometrically confined porous structures remains poorly characterized, especially over long timescales relevant to subsurface operations. Here, we present ultra-high-resolution microfluidic experiments that capture the evolution of residually trapped hydrogen over weeks in realistic, heterogeneous pore geometries under well-defined boundary conditions. We observe a distinct two-stage dynamic: a rapid local equilibration among neighboring bubbles, followed by slow global depletion driven by long-range diffusion toward low-chemical potential boundaries. Building on these insights, we develop and validate a continuum model that couples microscale capillary pressure-saturation (Pc-s) relationships, extracted via the pore-morphology method, with macroscopic diffusive transport. The model accurately predicts gas saturation evolution without fitting parameters and collapses experimental results across a range of experimental conditions. Extending the model to reservoir scales, we estimate equilibration timescales for CO2 and H2 in homogeneous sandstone aquifers. We find that ripening occurs much faster than convective dissolution in CO2 sequestration, and on timescales comparable to seasonal H2 storage operations. These findings establish a quantitative framework linking pore-scale heterogeneity to field-scale gas redistribution, with implications for the design and longevity of subsurface storage strategies.