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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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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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Zeng, S., Song, J., Sun, B., Wang, F., Ye, W., Shen, Y., et al. (2023). Seepage characteristics of the leaching solution during in situ leaching of uranium. Nuclear Engineering and Technology, 55(2), 566–574.
Abstract: Investigating the seepage characteristics of the leaching solution in the ore-bearing layer during the in situ leaching process can be useful for designing the process parameters for the uranium mining well. We prepared leaching solutions of four different viscosities and conducted experiments using a self-developed multifunctional uranium ore seepage test device. The effects of different viscosities of leaching solutions on the seepage characteristics of uranium-bearing sandstones were examined using seepage mechanics, physicochemical seepage theory, and dissolution erosion mechanism. Results indicated that while the seepage characteristics of various viscosities of leaching solutions were the same in rock samples with similar internal pore architectures, there were regular differences between the saturated and the unsaturated stages. In addition, the time required for the specimen to reach saturation varied with the viscosity of the leaching solution. The higher the viscosity of the solution, the slower the seepage flow from the unsaturated stage to the saturated stage. Furthermore, during the saturation stage, the seepage pressure of a leaching solution with a high viscosity was greater than that of a leaching solution with a low viscosity. However, the permeability coefficient of the high viscosity leaching solution was less than that of a low viscosity leaching solution.
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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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Musy, S., & Purtschert, R. (2023). Reviewing 39Ar and 37Ar underground production in shallow depths with implications for groundwater dating. Science of The Total Environment, 884, 163868.
Abstract: Argon-37 (37Ar) and Argon-39 (39Ar) are used for groundwater dating on timescales from weeks to centuries. For both isotopes, the quantification of underground sources is essential to accurately infer water residence times from sampled dissolved activities. Subsurface production resulting from interactions with neutrons from the natural radioactivity in rocks and with primary cosmogenic neutrons has been known for a long time. More recently, the capture of slow negative muons and reactions with muon-induced neutrons were documented for 39Ar subsurface production in the context of underground particle detectors (e.g. for Dark Matter research). However, the contribution from these particles was never considered for groundwater dating applications. Here, we reevaluate the importance of all potential depth-related production channels at depth ranges relevant for 39Ar groundwater dating [0 − 200 meters below the surface (m.b.s)]. The production of radioargon by muon-induced processes is considered in this depth range for the first time. The uncertainty on the total depth-dependent production rate is estimated with Monte Carlo simulations assuming a uniform distribution of the parameter uncertainties. This work aims to provide a comprehensive framework for interpreting 39Ar activities in terms of groundwater residence times and for exposure age dating of rocks. The production of 37Ar is also addressed since this isotope is relevant as a proxy for 39Ar production, for the timing of river-groundwater exchanges, and in the context of on-site inspections (OSI) within the verification framework of the Comprehensive Nuclear-Test-Ban Treaty (CTBT). In this perspective, we provide an interactive web-based application for the calculation of 37Ar and 39Ar production rates in rocks.
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