Three hydrochemical types of CO2-rich water (i.e., Na-HCO3, Ca-Na-HCO3 and Ca-HCO3) occur together in the silicate bedrock (granite and gneiss) of Gangwon Province in South Korea. As a natural analogue of geological carbon storage (GCS), this can provide implications for the environmental impacts of the leakage of CO2 from deep GCS sites. By using hydrochemical and isotopic datasets that were collected for previous and current studies, this study aimed to carefully scrutinize the hydrochemical differences in the three water types with an emphasis on providing a better understanding of the impacts of long-term CO2 leakage on groundwater quality (especially the enrichments of minor and trace metals). As a result, the Na-HCO3 type CO2-rich water contained higher Li, Rb and Cs than the Ca-HCO3 type, whereas Fe, Mn and Sr were higher in the Ca-HCO3 type than in the Na-HCO3 type despite the similar geological setting, which indicate that the hydrochemical differences were caused during different geochemical evolutionary processes. The δ18O and δD values and tritium concentrations indicated that the Na-HCO3 type was circulated through a deep and long pathway for a relatively long residence time in the subsurface, while the Ca-HCO3 type was strongly influenced by mixing with recently recharged water. These results were supported by the results of principal component analysis (PCA), whose second component showed that the Na-HCO3 type had a significant relation with alkali metals such as Li, Rb and Cs as well as Na and K and also had a strong relationship with Al, F and U, indicating an extensive water-rock interaction, while the Ca-HCO3 type was highly correlated with Ca, Mg, Sr, Fe and Mn, indicating mixing and reverse cation exchange during its ascent with hydrogeochemical evolution. In particular, the concentrations of Fe, Mn, U and Al in the CO2-rich water, the result of long-term water-rock interaction and cation exchange that was enhanced by CO2 leakage into silicate bedrock, exceeded drinking water standards. The study results show that the leakage of CO2 gas and CO2-rich fluid into aquifers and the subsequent hydrogeochemical processes can degrade groundwater quality by mobilizing trace elements in rocks and consequently may pose a health risk.
Carbon Capture and Storage (CCS) is a valuable climate-mitigation technology, which offers the potential to costeffectively reduce the emissions associated with the burning of fossil fuels. However, there is a potential risk of a small portion of the stored CO2 unintentionally migrating from a storage site to a shallow groundwater aquifer which is the final retaining zone for any migrated CO2 before it escapes to the atmosphere. Hence, it is imperative to identify the physical retention mechanisms of CO2 within a shallow aquifer. In this study 1.70x102 kg of CO2 and noble gas tracers (He, Ar and Kr) were continuously injected into a groundwater aquifer over 28 days with the aim of identifying the mechanisms and amount of CO2 retention. Among the tracers, Kr was found to be the earliest indicator of CO2 migration. The other tracers -He and Ar -arrived later and exhibited diluted signals. The diluted signals were attributed to degassing of the plume mass (1.6% of CO2) during the early stages of CO2 migration. Diffusion accelerated the dilution of the lighter elements at the plume boundaries. Consequently, the clear relation of the noble gases with the CO2 proved that degassing and mixing primarily control the mass retention of CO2 in shallow groundwater, and the relative importance of these processes varies along the evolving path of migrating CO2.
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