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Qiu, W., Yang, Y., Song, J., Que, W., Liu, Z., Weng, H., et al. (2023). 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. Applied Geochemistry, 148, 105522.
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.
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Haque, N., & Norgate, T. (2014). The greenhouse gas footprint of in-situ leaching of uranium, gold and copper in Australia. Journal of Cleaner Production, 84, 382–390.
Abstract: In-situ leaching (ISL) is a chemical method for recovering useful minerals and metals directly from underground ore bodies which is also referred to as ‘solution mining’. ISL is commonly used for uranium mining, accounting for about 45% of global production. The main benefits are claimed to be a lower environmental impact in terms of visual disturbances, emissions, lower energy use, cost compared with conventional open-cut or underground mining methods, and potential utilisation of lower grade resources. However, there is a lack of reported studies on the assessment of the environmental impacts of ISL, particularly greenhouse gas (GHG) emissions using life cycle assessment (LCA) methodology. The SimaPro LCA software was used to estimate the GHG footprint of the ISL of uranium, gold and copper. The total GHG emissions were estimated to be 38.0 kg CO2-e/kg U3O8 concentrate (yellowcake), 29 t CO2-e/kg gold, and 4.78 kg CO2-e/kg Cu. The GHG footprint of ISL uranium was significantly lower than that of conventional mining, however, the footprints of copper and gold were not much less compared with conventional mining methods. This is due to the lower ore grade of ISL deposits and recovery compared with high ore grades and recovery of conventional technology. Additionally, the use of large amount of electricity for pumping in case of ISL contributes to this result. The electricity consumed in pumping leaching solutions was by far the greatest contributor to the well-field related activities associated with ISL of uranium, gold and copper. The main strategy to reduce the GHG footprint of ISL mining should be to use electricity derived from low emission sources. In particular, renewable sources such as solar would be suitable for ISL as these operations are typically in remote locations with smaller deposits compared with conventional mining sites.
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Jana, A., Unni, A., Ravuru, S. S., Das, A., Das, D., Biswas, S., et al. (2022). In-situ polymerization into the basal spacing of LDH for selective and enhanced uranium adsorption: A case study with real life uranium alkaline leach liquor. Chemical Engineering Journal, 428, 131180.
Abstract: Uranium is used as a fuel for nuclear power plant and can be extracted from different ores, mainly acidic (silicious ore) and alkaline (carbonate ore). Recovery of uranium through acid leaching from silicious ore is well established, whereas, alkaline leaching from carbonate ore is challenging due to the excessive salinity of leach liquor and high concentration of carbonate, bicarbonate and sulphate. Herein, two monomers, acrylic acid (AA) and N, N-methylene bisacrylamide (BAM), selective towards uranyl were intercalated in-situ into the interlayer, followed by their polymerization and cross-linking to form novel polymer intercalated hybrid layered double hydroxide (LDH). The LDH acts as a backbone to overcome coiling and swelling of polymer and anchors them as free-standing. Various parameters, like, the type of metal ions, monomer ratio (AA: BAM) and metal ion ratio (M2+:M3+), were studied to determine the optimum conditions for effective intercalation and polymerization of monomers. Magnesium aluminum (MgAl) LDH with a cross-linked polymer having a monomer ratio of 3:2 (AA: BAM) as intercalating species showed maximum efficiency of uranyl adsorption (1456 mg/g at 30 °C) with highest capacity so far. The distribution coefficient (Kd, l/mg) in the order of 105 suggested that the adsorbent was highly selective for uranyl in the presence of different cations, anions and humic acid. The adsorbent extracts uranium effectively and selectively from a real-life alkaline leach liquor with an efficiency of 96% at 5 g/l dose. Uranium can be recovered from the adsorbent in the form of sodium di-uranate using 2(M) NaOH and was reused for eight cycles.
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Wang, B., Luo, Y., Qian, J. -zhong, Liu, J. -hui, Li, X., Zhang, Y. -hong, et al. (2023). Machine learning–based optimal design of the in-situ leaching process parameter (ISLPP) for the acid in-situ leaching of uranium. Journal of Hydrology, 626, 130234.
Abstract: 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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Li, J., Pang, Z., Liu, Y., Hu, S., Jiang, W., Tian, L., et al. (2023). Changes in groundwater dynamics and geochemical evolution induced by drainage reorganization: Evidence from 81Kr and 36Cl dating of geothermal water in the Weihe Basin of China. Earth and Planetary Science Letters, 623, 118425.
Abstract: 81Kr and 36Cl can both be used to date groundwater beyond the dating range of 14C. 81Kr usually provides reliable groundwater ages because it has uniform initial distribution and negligible subsurface generation, while 36Cl is commonly influenced by subsurface sources or “dead” chloride dissolution. Therefore, the combined use of 81Kr and 36Cl could provide clues on the evolution history of groundwater. In the present study, we performed 36Cl and 81Kr dating of geothermal water in Weihe Basin of China and interpreted the possible cause of disagreement. Two distinct water masses were identified with distinctive isotopic signals: groundwater with significant δ18O shifts (up to −2.0‰), dissolved dead Cl and ages < 1.0 Ma (Cluster A), and older water with little δ18O shifts, negligible dissolved Cl and ages >1.0 Ma (Cluster B). The results confirm the eastward flow path of Cluster B to the Ancient Sanmen Lake with an increasing trend of Cl concentration and age. Modern recharge from the mountains flows to the basin center with intense interaction between water and carbonate under respective reservoir temperatures (100 ∼ 130 °C). These waters flow through the saline stratum emerging from the spillover of the Ancient Sanmen Lake, resulting in higher dead Cl dissolution. A significant linear relationship is observed with the older end-member of ∼1.3Ma under the topographically-driven faster circulation effect. 81Kr ages seem to support the hypothesis that the birth of the modern Yellow River was at about 1.0–1.3 Ma. We inferred the drainage reorganization from the Ancient Sanmen Lake to the modern Yellow River since the Mid-Pleistocene Transition induced the change in groundwater dynamics as well as its chemical evolution. The excavation of the Ancient Sanmen Lake and the accentuated incision of the Weihe River induced groundwater gradient, and therefore the recharge from precipitation from both slopes of the Qinling Mountains in the south and the Beishan Mountains in the north. Our results highlight the effects of dead Cl on 36Cl dating and demonstrate the significant impact of catchment reorganization on groundwater dynamics and its chemistry.
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