Abstract

Geological storage has been proposed as a new technology to temporarily store significant amounts of hydrogen (H2) gas in depleted gas reservoirs, underground salt caverns, or saline aquifers. Often, such subsurface reservoirs naturally contain trace amounts of organic acids, and these compounds can considerably alter the wettability of reservoir rocks, causing them to become less water-wet. We carried out Molecular Dynamics (MD) simulations of contact angles in a quartz-brine-H2 system to evaluate wettability in realistic subsurface situations. MD simulations suggest that Humic acid makes quartz more hydrophobic, which can affect the overall behaviour of the storage reservoir. For the first time, this effect was experimentally investigated for a natural sandstone reservoir from the South West Hub Project, i.e., the Lesueur Sandstone (LS) formation. Multi-stage core flooding experiments were conducted on the same LS plug to investigate the impact of wettability alteration on initial and residual hydrogen saturation/trapping at depth. First, consecutive brine-H2 drainage-imbibition cycles were carried out on the natural sample; the result indicated that the rock-brine-H2 system was essentially water-wet. Then, the sample was aged in Humic acid with a molarity of 10−2 M for 42 days at 5 °C and 0.1 MPa. The wettability of the storage system shifted toward a less water-wet state, i.e., more hydrophobic. As a result of Humic acid ageing, the initial hydrogen saturation reduced from 29% to 15%, and the residual hydrogen trapping reduced from 23% to 11%. This is attributed to a change induced in the capillary force (i.e., snap-off) controlled by wettability and pore size. In addition, the wettability change induced by Humic acid increased the hydrogen recovery rate from 20.7% to 26.7%.

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