Underground Hydrogen Storage (UHS) provides a large-scale and safe solution to balance the fluctuations in energy production from renewable sources and energy consumption but requires a proper and detailed characterization of the candidate reservoirs. The scope of this study was to estimate the hydrogen diffusion coefficient for real caprock samples from two natural gas storage reservoirs that are candidates for underground hydrogen storage. A significant number of adsorption/desorption tests were carried out using a Dynamic Gravimetric Vapor/Gas Sorption System. A total of 15 samples were tested at the reservoir temperature of 45 °C and using both hydrogen and methane. For each sample, two tests were performed with the same gas. Each test included four partial pressure steps of sorption alternated with desorption. After applying overshooting and buoyancy corrections, the data were then interpreted using the early time approximation of the solution to the diffusion equation. Each interpretable partial pressure step provided a value of the diffusion coefficient. In total, more than 90 estimations of the diffusion coefficient out of 120 partial pressure steps were available, allowing a thorough comparison between the diffusion of hydrogen and methane: hydrogen in the range of 1 × 10−10 m2/s to 6 × 10−8 m2/s and methane in the range of 9 × 10−10 m2/s to 2 × 10−8 m2/s. The diffusion coefficients measured on wet samples are 2 times lower compared to those measured on dry samples. Hysteresis in hydrogen adsorption/desorption was also observed.
