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Hofmann, H.; Pearce, J.K.; Hayes, P.; Golding, S.D.; Hall, N.; Baublys, K.A.; Raiber, M.; Suckow, A. |
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Title |
Multi-tracer approach to constrain groundwater flow and geochemical baseline assessments for CO2 sequestration in deep sedimentary basins |
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Journal Article |
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Year |
2023 |
Publication |
International Journal of Coal Geology |
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104438 |
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CO geological storage, Great Artesian Basin, Groundwater chemistry, Isotopic tracer, Surat Basin |
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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. |
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0166-5162 |
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THL @ christoph.kuells @ hofmann_multi-tracer_2023 |
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165 |
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Boumaiza, L.; Ammar, S.B.; Chesnaux, R.; Stotler, R.L.; Mayer, B.; Huneau, F.; Johannesson, K.H.; Levison, J.; Knöller, K.; Stumpp, C. |
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Title |
Nitrate sources and transformation processes in groundwater of a coastal area experiencing various environmental stressors |
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Journal Article |
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Year |
2023 |
Publication |
Journal of Environmental Management |
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Volume |
345 |
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118803 |
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Keywords |
Aquifer, Denitrification, MixSIAR, Nitrate, Nitrification, Stable isotopes |
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Abstract |
In coastal salinized groundwater systems, contamination from various nitrate (NO3) inputs combined with complex hydrogeochemical processes make it difficult to distinguish NO3 sources and identify potential NO3 transformtation processes. Effective field-based NO3 studies in coastal areas are needed to improve the understanding of NO3 contamination dynamics in groundwater of such complex coastal systems. This study focuses on a typical Mediterranean coastal agricultural area, located in Tunisia, experiencing substantial NO3 contamination from multiple anthropogenic sources. Here, multiple isotopic tracers (δ18OH2O, δ2HH2O, δ15NNO3, δ18ONO3, and δ11B) combined with a Bayesian isotope MixSIAR model are used (i) to identify the major NO3 sources and their contributions, and (ii) to describe the potential NO3 transformation processes. The measured NO3 concentrations in groundwater are above the natural baseline threshold, suggesting anthropogenic influence. The measured isotopic composition of NO3 indicates that manure, soil organic matter, and sewage are the potential sources of NO3, while δ11B values constrain the NO3 contamination to manure; a finding that is supported by the results of MixSIAR model revealing that manure-derived NO3 dominates over other likely sources. Nitrate derived from manure in the study area is attributed to organic fertilizers used to promote crop growth, and livestock that deposit manure directly on the ground surface. Evidence for ongoing denitrification in groundwaters of the study area is supported by an enrichment in both 15N and 18O in the remaining NO3, although isotopic mass balances between the measured and the theoretical δ18ONO3 values also suggest the occurrence of nitrification. The simultaneous occurrence of these biogeochemical processes with heterogeneous distribution across the study area reflect the complexity of interactions within the investigated coastal aquifer. The multiple isotopic tracer approach used here can identify the effect of multiple NO3 anthropogenic activities in coastal environments, which is fundamental for sustainable groundwater resources management. |
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0301-4797 |
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THL @ christoph.kuells @ boumaiza_nitrate_2023 |
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170 |
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Smedley, P.L.; Bearcock, J.M.; Ward, R.S.; Crewdson, E.; Bowes, M.J.; Darling, W.G.; Smith, A.C. |
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Title |
Monitoring of methane in groundwater from the Vale of Pickering, UK: Temporal variability and source discrimination |
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Journal Article |
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Year |
2023 |
Publication |
Chemical Geology |
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636 |
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121640 |
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Keywords |
Aquifer, Biogenic, Ethane, Hydrocarbons, Methane, Shale gas |
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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. |
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0009-2541 |
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THL @ christoph.kuells @ smedley_monitoring_2023 |
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172 |
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Lima, G.F.C.; Filho, C.A. de C.; Ferreira, V.G.; Lima, J. da S.D.; Marques, E.D.; Minardi, P.S.P.; Dalmázio, I.; Moreira, R.M. |
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Establishing a water baseline for the unconventional gas industry: A multiple environmental isotopes assessment (18O, 2H, 3H, 13C, and 14C) of surface and groundwater in the São Francisco Basin, Brazil |
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Journal Article |
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Year |
2023 |
Publication |
Applied Geochemistry |
Abbreviated Journal |
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159 |
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105818 |
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Fracking, Groundwater dating, Indaiá river, Isotopes assessment, Shale gas, Unconventional hydrocarbons |
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Unconventional hydrocarbon production has become the target of an intensive environmental debate due to the risks it poses to water resources. Fracking, while enabling the extraction of oil and gas from ultra-low permeability reservoirs, also possesses the risk of polluting water systems through failures from hydraulic fracturing and its associated procedures. The need to foster national industrial development with a transitional energy matrix has led Brazil to discuss the environmental suitability before producing its large unconventional reserves. Many studies have highlighted the need for a robust environmental characterization before the development of the unconventional industry. In this sense, multiple environmental isotopes may work as a proxy for identifying water contamination right from the early stages. Environmental isotopes may also be applied to enhance the understanding of the natural geochemical processes intrinsic to a given area. This study presents an environmental isotopes baseline for the groundwater and riverine water systems within the São Francisco Basin, a proven tight gas reservoir in Brazil, in a pre-operational context. δ18O, δ2H, 3H, δ13C, and Δ14C were evaluated in three different seasons in groundwater and surface water samples, along with other auxiliary parameters such as physical-chemical parameters (in situ), major ions, and d-excess. The δ2H and δ18O in surface water shows an upstream → downstream enrichment trend, with some variations suggesting baseflow interactions in the surface water systems. An evaporation line for the study area was defined as δ2H = 4.6903 δ18O + 10.362. δ13C indicates a mutual dissolution of silicates and carbonates in the groundwater system and suggests a group of samples highly related to the recharge areas. Groundwater dating denotes the Serra da Saudade Formation as a modern fractured aquifer with a strong recharge capacity. These findings support stakeholders in environmental monitoring and management of the unconventional gas industry. |
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0883-2927 |
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THL @ christoph.kuells @ lima_establishing_2023 |
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173 |
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Pham, Q.-N.; Nguyen, T.-C.; Ta, T.-T.; Tran, T.-L. |
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Comprehensive approach to sustainable groundwater management in semi-arid Ninh Thuan plain, Vietnam |
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Journal Article |
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2023 |
Publication |
Groundwater for Sustainable Development |
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23 |
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101031 |
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Climate change, Groundwater, Managed aquifer recharge (MAR), Modeling, Sea level rise, Seawater intrusion, Sustainable groundwater management |
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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. |
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2352-801x |
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THL @ christoph.kuells @ pham_comprehensive_2023 |
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174 |
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Kurmanseiit, M.B.; Tungatarova, M.S.; Royer, J.-J.; Aizhulov, D.Y.; Shayakhmetov, N.M.; Kaltayev, A. |
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Streamline-based reactive transport modeling of uranium mining during in-situ leaching: Advantages and drawbacks |
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Journal Article |
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Year |
2023 |
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Hydrometallurgy |
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220 |
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106107 |
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3D modeling, In-situ leaching, Reactive transport model, Streamlines, Uranium recovery |
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Reactive transport modeling is known to be computationally intensive when applied to 3D problems. Transforming sequential computing on the computer processor units (CPU) into parallelized computation on the high-performance parallel graphic processor units (GPU) is a classical approach to increasing computational performance. Another complementary approach is to decompose a complex 3D modeling problem into a set of simpler 1D problems using streamline approaches which can be easily parallelized, therefore reducing computation time. This paper investigates solutions to the equations governing dissolution and transport using streamlines coupled with a parallelization approach. In addition, an analytical solution to the dissolution and transfer equations of uranium describing the In-Situ Leaching (ISL) mining recovery is found using an approximation series to the 2nd order. The analytical solution is compared to the 1D numerical resolution along the streamlines and to the 3D simulation results superimposed on the streamline. Both approaches give similar results with a relative error of \textless2 % (2%). The proposed methodology is then applied to a case study in which the classical 3D resolution is compared to the newly suggested streamline solution, demonstrating that the streamline approach increases computational performances by a factor ranging from hundred to thousand depending on the complexity of the grid-block model. |
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0304-386x |
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THL @ christoph.kuells @ kurmanseiit_streamline-based_2023 |
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190 |
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Xie, T.; Lian, B.; Chen, C.; Qian, T.; Liu, X.; Shang, Z.; Li, T.; Wang, R.; Wang, Z.; Zhang, A.; Zhu, J. |
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Leaching behaviour and mechanism of U, 226Ra and 210Pb from uranium tailings at different pH conditions |
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Journal Article |
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2023 |
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Journal of Environmental Radioactivity |
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270 |
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107300 |
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Leaching experiments, Pb, Ra, U, Uranium tailings |
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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. |
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0265-931x |
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THL @ christoph.kuells @ xie_leaching_2023 |
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200 |
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Shayakhmetov, N.M.; Alibayeva, K.A.; Kaltayev, A.; Panfilov, I. |
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Enhancing uranium in-situ leaching efficiency through the well reverse technique: A study of the effects of reversal time on production efficiency and cost |
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Journal Article |
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2023 |
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Hydrometallurgy |
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219 |
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106086 |
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Economic evaluation, Hydrodynamic enhancement of mineral production, In-situ leaching, Mineral recovery, Optimal reversal time, Well reversing technique |
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In this study, the application of the Well Reversal Technique (WRT) and the impact of reversal time on the efficiency of uranium mining via In-Situ Leaching (ISL) were investigated. A prevalent issue in ISL mineral extraction is the formation of stagnant zones caused by limited access of the lixiviant, which leads to increased operating expenditures. The WRT, which involves altering the function of some wells from injection to production or vice versa, is a potential solution to this problem. The efficiency of WRT is heavily dependent on the well pattern and reversal time. Two commonly used well patterns in ISL are the 9-spot (row arrangement) and 7-spot (hexagonal arrangement). The objective of this study was to determine the optimal reversal time for a 9-spot well pattern through mathematical modeling of hydrodynamic and physico-chemical processes and subsequent economic assessment. A mathematical model of uranium extraction processes was developed using the principles of mass conservation, Darcy’s, and mass action laws. The results obtained for a 9-spot well pattern without reversal, with two reversal options, and a 7-spot scheme were analyzed comparatively. The 7-spot scheme without reversal was found to be the most effective of the options examined. The application of WRT on a 9-spot well pattern allows to enhance production efficiency to a level comparable to that of a 7-spot well pattern. Additionally, the effect of reversal time on recovery was studied based on two well reversal options. The results from calculation revealed that the optimal scenario was when the well reversal is conducted immediately after the time point at which the average concentration of the pregnant solution in the production wells reaches its peak value. The overall efficiency of WRT application was determined through economic calculations of capital (CAPEX) and operating (OPEX) expenditures. Based on economic calculations, it was determined that the utilization of WRT results in a 3–18% increase in mineral production efficiency for a 9-point scheme, depending on the chosen reversal method. |
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0304-386x |
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THL @ christoph.kuells @ shayakhmetov_enhancing_2023 |
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203 |
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Qiu, W.; Yang, Y.; Song, J.; Que, W.; Liu, Z.; Weng, H.; Wu, J.; Wu, J. |
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What chemical reaction dominates the CO2 and O2 in-situ uranium leaching?: Insights from a three-dimensional multicomponent reactive transport model at the field scale |
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Journal Article |
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2023 |
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Applied Geochemistry |
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148 |
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105522 |
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Carbonate minerals, In-situ leaching (ISL) of uranium, Pyrite oxidation, Reactive transport modeling (RTM) |
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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. |
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THL @ christoph.kuells @ qiu_what_2023 |
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Wang, B.; Luo, Y.; Qian, J.-zhong; Liu, J.-hui; Li, X.; Zhang, Y.-hong; Chen, Q.-qian; Li, L.-yao; Liang, D.-ye; Huang, J. |
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Machine learning–based optimal design of the in-situ leaching process parameter (ISLPP) for the acid in-situ leaching of uranium |
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2023 |
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Journal of Hydrology |
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626 |
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130234 |
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In-situ leaching, Injection rate design, Lixiviant concentration design, Machine learning, Simulation-optimisation, Uncertainty |
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The migration process of leached uranium in the in-situ leaching of uranium is considered a typical reactive transport problem. During this process, the lixiviant concentration and injection rate are important in-situ leaching process parameters (ISLPP) to efficiently recover uranium. However, several uncertain factors affect the outcomes of the ISLPP design. In addition, the repeated use of the reactive transport model (RTM) for investigating the acid in-situ leaching of uranium with the application of the Monte Carlo method leads to a substantial computational load. For this reason, a machine learning (ML)–based surrogate model was developed with the backpropagation neural network (BPNN) method to replace the RTM under the condition of uncertain parameters. Moreover, the simulated annealing optimisation model for ISLPP was created based on the proposed surrogate model. The optimal ISLPP was achieved that generated maximum profits from uranium recovery under different lixiviant prices, uranium prices and exploitation times. The optimal design framework of ISLPP based on the proposed ML algorithm was then applied in the Bayan-Uul sandstone-type uranium deposit in Inner Mongolia, China. From our analysis, it was demonstrated that the ML-based surrogate model exhibited great fitness with the RTM. The optimal results of the ISLPP indicated that the lixiviant concentration and injection rate could be adjusted based on the fluctuations in lixiviant price, uranium price and exploitation time. If the prices of sulphuric acid were high, a specific concentration of hydrogen peroxide could be injected into the injection well to promote the oxidation and dissolution of the uranium ore to increase the income from the uranium recovery. The optimisation model can also use the ISLPP scheme to boost the revenues from different lixiviant prices, uranium prices and exploitation times under the uncertainty of porosity, illustrating the applicability of the ML-based optimal design method of ISLPP in ISL mining. A general framework for developing surrogate models, as well as for conducting uncertainty analyses for a wide range of groundwater models was proposed here yielding valuable insights. |
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0022-1694 |
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THL @ christoph.kuells @ wang_machine_2023 |
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210 |
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