Summary Underground hydrogen storage (UHS) is a cost-effective and safer system vital for the growth of the hydrogen market and its role as an essential transitional fuel. Presently, depleted hydrocarbon reservoirs (DHR) account for more than 75% of all UHS sites due to their higher prevalence and readiness for use. However, hydrogen (H2) loss primarily due to abiotic interactions poses a significant challenge to the integrity of DHR sites, and while the underlying conditions have been investigated in some studies, the conclusions have been inconsistent, particularly for carbonate reservoirs. In this study, we analyzed the impact of reservoir physical and chemical parameters, (i.e., salinity, mineralogy, temperature, and pressure) on H2-brine-mineral interactions and the extent of H2 loss in carbonate formations. Static batch simulations were performed using PHREEQC and MATLAB® for a 1-year storage cycle period with three different brine and rock samples at 50–130°C and 15–30 MPa. The results showed that the dissociation of H2 and formation of CH4 and H2S increased with increasing temperature, at a two times higher rate compared to pressure. Also, markedly, in various brine compositions and reactive mineralogy, a 20% or less H2 loss could be attained in temperatures <50°C and 115–130°C, with pressure below 17 MPa; meanwhile, the pressure condition 18 MPa and greater (at 50°C) would risk at least 50% loss, with >86% from 19 MPa. Second, H2 loss increased to 80% after about 50 days for all the brines, and pressure and temperature conditions in the mineral sample with the largest composition of reactive minerals (i.e., pyrite, anhydrite, etc.) suggested a 50% loss risk in such mineralogy during the storage cycle period of about 1 month. Lastly, in the mineral sample with >90 wt% calcite and 0–2 wt% reactive minerals composition, H2 molality increased at least fourfold on average across the storage period and reservoir brine/temperature/pressure conditions. This result further indicates that reactive mineralogy has a more significant effect on the stability of hydrogen relative to temperature and pressure in a carbonate UHS formation. In summary, the findings suggest that a minimal reactive mineral composition, 100°C or higher, and 17 MPa or lower constitutes a set of reservoir physical and chemical conditions with the potential for a limited risk of H2 loss (<20%) in carbonate DHR. However, the extension of the present work to the dynamic UHS conditions is necessary to further ascertain these conclusions.
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