Underground hydrogen storage (UHS) in carbonate reservoirs
is a
suitable solution for safe storage and efficient hydrogen recovery
during the cycling process. The uncertainties associated with potential
geochemical reactions between hydrogen, rock, and brine may impact
the long-term containment of produced hydrogen in carbonate formations.
Despite the current interest in studying hydrogen-rock reactions,
only limited work is available in the literature. In this study, we
experimentally evaluate the reactivity of carbonate rocks to hydrogen
and address the potential of gas generation induced by geochemical
reactions. Limestone samples are treated with hydrogen under 1500
psi and 75 °C temperature for a duration between 6 and 13 months
using simple reaction cells. Scanning electron microscopy (SEM) analysis
is performed to examine the potential dissolution/precipitation reactions
induced by hydrogen. In contrast, gas chromatography (GC analyzer)
analysis and inductively coupled plasma optical emission spectroscopy
(ICP-OES) are conducted to detect gas generation and ion precipitation.
The experimental results indicate no significant impact of hydrogen
treatment on surface morphology and pore structure even after 6 months
of treatment, suggesting that abiotic reactions in carbonate rocks
are unlikely to occur during the first stages of UHS. Furthermore,
in the presence of brine, there are no apparent indications of geochemical
reactions occurring between hydrogen and calcite, and no traces of
any other gases are detected after 13 months of treatment. Besides,
the solutions’ pH remains almost unchanged, with a minor increase
in calcium (Ca2+) ions in the solution, which is attributed
to the presence of water, not hydrogen reactions. The results of this
work promisingly support the utilization of carbonate reservoirs for
long-term hydrogen storage.