Abstract: Geological storage of gases will be necessary in the push to net zero and the energy transition to reduce carbon emissions to atmosphere. These include CO2 geological storage in suitable sandstone reservoirs. Understanding groundwater flow, connectivity and hydrogeochemical processes in aquifer and storage systems is vital to prevent risk and protect important water resources, such as the Great Artesian Basin. Here, we provide a ‘tool-box’ of geochemical assessment methods to provide information on flow patterns through the basin’s aquifers (changes in chemistry along flow path), stagnant versus flowing conditions (cosmogenic isotopes and noble gases), inter-aquifer connectivity and seal properties (major ions, Sr and stable isotopes), water quality (major ions and metals) and general assessments on residence times of groundwater (cosmogenic isotopes and noble gases). This information can be used with reservoir and groundwater models to inform on possible changes in the above-mentioned processes and serve as input parameters for CO2 injection impact modelling. We demonstrate the use and interpretation on an example of a potential CO2 storage geological sequestration site in the Surat Basin, part of the Great Artesian Basin, and the aquifers that overly the reservoir. The stable water isotopes are depleted compared to average rainfall and most likely indicate greater contributions from monsoonal rain events from the northern monsoonal troughs, where amount and rainout effects lead to the depletion rather than colder recharge climates. This is supported by the modern recharge temperatures from noble gases. Inter-aquifer mixing between the Precipice Sandstone reservoir and the Hutton Sandstone aquifer seems unlikely as the Sr isotope ratios are distinctly different suggesting that the Evergreen Formation is a seal in the locations sampled. Mixing, however, occurs on the edges of the basin, especially in the south-east and east where the Surat Basin transitions into the Clarence-Moreton Basin. Groundwater flow appears to be to the south in the Precipice Sandstone, with a component of flow east to the Clarence-Morton Basin. The cosmogenic isotopes and noble gases strongly indicate very long residence times of groundwater in the central south Precipice Sandstone around a proposed storage site. 14C values below analytical uncertainty, R36Cl ratios at secular equilibrium as well as high He concentrations and high 40Ar/36Ar ratios support the argument that groundwater flow in this area is extremely slow or groundwater is stagnant. The results of this study reflect the geological and hydrogeological complexities of sedimentary basins and that baseline studies, such as this one, are paramount for management strategies.

Abstract: Groundwater abstracted from aquifers in the Vale of Pickering, North Yorkshire, UK and monitored over the period 2015–2022, shows evidence of variable but commonly high concentrations of dissolved CH4. Sampled groundwater from the Jurassic organic-rich Kimmeridge Clay Formation (boreholes up to 180 m depth) has concentrations up to 57 mg/L, and concentrations up to 59 mg/L are found in groundwater from underlying confined Corallian Group limestone (borehole depths 50–227 m). The high concentrations are mainly from boreholes in the central parts of the vale. Small concentrations of ethane (C2H6, up to 800 μg/L) have been found in the Kimmeridge Clay and confined Corallian groundwaters, and of propane (C3H8, up to 160 μg/L) in deeper boreholes (110–180 m) from these formations. The concentrations are typically higher in groundwater from the deeper boreholes and vary with hydrostatic pressure, reflecting the pressure control on CH4 solubility. The occurrences contrast with groundwater from shallow Quaternary superficial deposits which have low CH4 concentrations (up to 0.39 mg/L), and with the unconfined and semi-confined sections of the Corallian aquifer (up to 0.7 mg/L) around the margins of the vale. Groundwater from the Quaternary, Kimmeridge Clay formations and to a small extent the confined Corallian aquifer, supports local private-water supplies, that from the peripheral unconfined sections of Corallian also supports public supply for towns and villages across the region. Dissolved methane/ethane (C1/C2) ratios and stable-isotopic compositions (δ13C-CH4, δ2H-CH4 and δ13C-CO2) suggest that the high-CH4 groundwater from both the Kimmeridge Clay and confined Corallian formations derives overwhelmingly from biogenic reactions, the methanogenesis pathway by CO2 reduction. A small minority of groundwater samples shows a more enriched δ13C-CH4 composition (−50 to −44 ‰) which has been interpreted as due to anaerobic or aerobic methylotrophic oxidation in situ or post-sampling oxidation, rather than derivation by a thermogenic route. Few of the existing groundwater sites are proximal to abandoned or disused conventional hydrocarbon wells that exist in the region, and little evidence has been found for an influence on groundwater dissolved gases from these sites. The Vale of Pickering has also been under recent consideration for development of an unconventional hydrocarbon (shale-gas) resource. In this context, the monitoring of dissolved gases has been an important step in establishing the high-CH4 baseline of groundwaters from Jurassic deposits in the region and in apportioning their sources and mechanisms of genesis.

Abstract: Vietnam is a country with a long coastline and a high population density residing in the coastal plains. The largest dry area in Vietnam, the coastal plain of Ninh Thuan province, always lacks water in the first dry months of the year (Jan., Feb., Mar., and Apr.). Groundwater is an extremely valuable resource for supplies at this time. Therefore, the objective of this study is to establish a comprehensive approach to sustainable groundwater management in this semi-arid region. This approach is not only mitigating the negative impacts of factors such as climate change, sea level rise, and socio-economic development but also suggesting measures for management of aquifer recharge. A groundwater model for a 3-layer system with variable density flow SEAWAT is built to predict the impacts of climate change and sea level rise without a change in groundwater abstraction. This model helps to understand the trend of salt intrusion and lowering groundwater level in the study area. Afterwards, scenarios with different ground water abstraction and groundwater development such as ground dam, infiltration basin have been set up to meet the demands of socio-economic development in the future. Predicted results will show the impacts of the groundwater systems in the area such as groundwater level change, and saltwater intrusion. Controlled groundwater abstraction and some measures of groundwater development such as infiltration basin, underground dam would allow for an increase of up to 50000m3/day in the year 2050 without negative impacts on the aquifer system.

Abstract: A large number of radionuclides remain in uranium tailings, and U, 226Ra and 210Pb leach out with water chemistry, causing potential radioactive contamination to the surrounding environment. In this paper, uranium tailings from a uranium tailings pond in southern China were collected at different depths by means of borehole sampling, mixed and homogenised, and analysed for mineral and chemical composition, microscopic morphology, U, 226Ra and 210Pb fugacity, static leaching and dynamic leaching of U, 226Ra and 210Pb in uranium tailings at different pH conditions. The variation of U, 226Ra and 210Pb concentrations in the leachate under different pH conditions with time was obtained, and the leaching mechanism was analysed. The results showed that the uranium tailings were dominated by quartz, plagioclase and other minerals, of which SiO2 and Al2O3 accounted for 65.45% and 13.32% respectively, and U, 226Ra and 210Pb were mainly present in the residue form. The results of the static leaching experiments show that pH mainly influences the leaching of U, 226Ra and 210Pb by changing their chemical forms and the particle properties of the tailings, and that the lower the pH the more favourable the leaching. The results of dynamic leaching experiments during the experimental cycle showed that the leaching concentration and cumulative release of U, 226Ra and 210Pb in the leach solution were greater at lower pH conditions than at higher pH conditions, and the leaching of U, 226Ra and 210Pb at different pH conditions was mainly from the water-soluble and exchangeable states. The present research results are of great significance for the environmental risk management and control of radioactive contamination in existing uranium tailings ponds, and are conducive to ensuring the long-term safety, stability and sustainability of uranium mining sites.

Abstract: The complex behavior of uranium in recovery is mostly driven by water-rock interactions following lixiviant injection into ore-bearing aquifers. Significant challenges exist in exploring the geochemical processes responsible for uranium release and mobilization. Herein this study provides an illustration of a ten-year field scale CO2 and O2 in-situ leaching (ISL) process at a typical sandstone-hosted uranium deposit in northern China. We also conducte a three-dimensional (3-D) multicomponent reactive transport model to assess the effects of potential chemical reactions on uranium recovery, in particular, to focus on the role of sulfide mineral pyrite (FeS2). Numerical simulations are performed considering three potential ISL reaction pathways to determine the relative contributions to uranium release, and the results indicate that bicarbonate promotes the oxidative dissolution of uranium-bearing minerals and further accelerates the uranium leaching in a neutral geochemical system. Moreover, the presence of FeS2 exerts a strong competitive role in the uranium-bearing mineral dissolution by increasing oxygen consumption, favoring the formation of iron oxyhydroxide, and therefore causing an associated decrease in uranium recovery rates. The simulation model demonstrates that dissolution of carbonate neutralizes acidic water generated from pyrite oxidation and aqueous CO2 dissociation. In addition, the cation concentrations (i.e., Ca and Mg) are increasing in the pregnant solutions, showing that the recycling of lixiviants and kinetic dissolution of carbonate generates a larger number of dissolved Ca and Mg and inevitably triggers the secondary dolomite mineral precipitation. The findings improve our fundamental understanding of the geochemical processes in a long-term uranium ISL system and provide important environmental implications for the optimal design of uranium recovery, remediation, and risk exposure assessment.