A simulation study and a series of autoclave experiments were performed, reproducing gas-rock-water systems under reservoir conditions, after injection of CO2 and the mixture of CO2 with H2S into rocks representing the Upper Silesian Coal Basin and the adjacent Małopolska Block (Central Europe). The water-rock-gas interactions were modeled in two stages: the first–aimed at simulating the short-term changes in system impacted by the gas injection, and the second–long-term effects of sequestration.
On the basis of the simulations, the reactions behind mineral transformations were identified. These phenomena are different for the injection of CO2 alone. and CO2+H2S mixtures, resulting in the formation of secondary minerals responsible for mineral sequestration. Depending on the original mineral composition of the rock, in the case of pure CO2, these are mainly carbonate minerals siderite, dawsonite, magnesite, dolomite and calcite, while in the case of mixture injection: elemental sulfur, sulfur sulfides–pyrite and pyrrhotite.
In experiments with the H2S+CO2 mixture, dissolution of skeletal grains was observed, which was most visible in the case of carbonates, feldspars, and chlorites. The analysis of rocks containing hematite revealed the formation of elemental sulfur surrounded by FeS2 crystals, which had not been previously reported.
The experiments generally confirmed the interactions in gas-rock-water systems identified by numerical simulation. This allowed to estimate the amount of mineral phases precipitated or dissolved in the analyzed reactions, and consequently the impact on changes in porosity and the amount of sequestered carbon dioxide and sulfur.
In samples abundant in carbonate minerals (the Dębowiec Formation psephites), the decomposition of ankerite, due to the injection of CO2+H2S, is not compensated for by the precipitation of sufficient amounts of other carbonates, which leads to the desequestration process–CO2 release.
Based on the calculations, it was found that the potentially most favorable conditions for the sequestration occur in the Paralic Series mudstones, rich in chlorites–a maximum of 22.36 kg CO2/m3 and 12.50 kg S/m3, trapping capacity after 10,000 years of storage.