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Gil-Márquez, J. M., Sültenfuß, J., Andreo, B., & Mudarra, M. (2020). Groundwater dating tools (3H, 3He, 4He, CFC-12, SF6) coupled with hydrochemistry to evaluate the hydrogeological functioning of complex evaporite-karst settings. Journal of Hydrology, 580, 124263.
Abstract: The hydrogeological functioning of four different areas in a complex evaporite-karst unit of predominantly aquitard behavior in S Spain was investigated. Environmental dating tracers (3H, 3He, 4He, CFC-12, SF6) and hydrochemical data were determined from spring samples to identify and characterize groundwater flow components of different residence times in the media. Results show a general geochemical evolution pattern, from higher (recharge areas) to lower positions (discharge areas), in which mineralization rises as well as the value of the rCl−/SO42−, evidencing longer water-rock interaction. Ne values show degassing of most of the samples, favored by the high salinity of groundwater and the development of karstification so that the concentration of all the considered gases were corrected according to the difference between the theoretical and the measured Ne. The presence of modern groundwater in every sample was proved by the detection of 3H and CFC-12. At the opposite, the higher amount of radiogenic 4He in most samples also indicates that they have an old component. The 3H/3He dating method does not give reliable ages as a consequence of degassing and the large uncertainty of the 3He/4He ratios of the sources for the radiogenic Helium. The large SF6 concentrations suggest terrigenic production related to halite and dolomite. Binary Mixing and Free Shape Models were created based on 3H and CFC-12 data to interpret the age distribution of the samples. Two parameters (GA50 and >70%) were proposed as an indicator of that distribution, as they provide further information than the mean age. Particularly, GA50 is derived from the median groundwater age and is presented as a new way of interpreting mixed groundwater age data. A greater fraction of old groundwater (3H and CFC-12 free) was identified in discharge areas, while the proportion and estimated infiltration date of the younger fractions in recharge areas were higher and more recent, respectively. The application of different approaches has been useful to corroborate previous theoretical conceptual model proposed for the study area and to test the applicability of the used environmental tracer in dating brine groundwater and karst springs.
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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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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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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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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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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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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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YI, Z. -ji, LIAN, B., YANG, Y. -qun, & ZOU, J. -ling. (2009). Treatment of simulated wastewater from in situ leaching uranium mining by zerovalent iron and sulfate reducing bacteria. Transactions of Nonferrous Metals Society of China, 19, 840.
Abstract: Batch and column experiments were conducted to determine whether zerovalent iron (ZVI) and sulfate reducing bacteria (SRB) can function synergistically and accelerate pollutant removal. Batch experiments suggest that combining ZVI with SRB can enhance the removal of U(?) synergistically. The removal rate of U(?) in the ZVI+SRB combining system is obviously higher than the total rate of ZVI system and SRB system with a difference of 13.4% at t=2 h and 29.9% at t=4 h. Column experiments indicate that the reactor filled with both ZVI and SRB biofilms is of better performance than the SRB bioreactor in wastewater basification, desulfurization and U(?) fixation. The results imply that the ZVI+SRB permeable reactive barrier may be a promising method for treating subsurface uranium contamination.
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Zhou, Y., Li, G., Xu, L., Liu, J., Sun, Z., & Shi, W. (2020). Uranium recovery from sandstone-type uranium deposit by acid in-situ leaching – an example from the Kujieertai. Hydrometallurgy, 191, 105209.
Abstract: The factors influencing uranium recovery in water-rock systems during acid in-situ leaching (ISL) were studied at the Kujieertai uranium deposit in Xinjiang. Using an ISL unit, a field leach trial (FLT) had been carried out to test the sequential effects of a leaching solution without oxidant (H2SO4 solution 4–8 g/L) and a leaching solution with oxidant (H2SO4 3–7 g/L, and Fe (III) 2–6 g/L). The observation of the leaching process revealed clearly defined stages of uranium release from the solid mineral to solution. Uranium mobilization from solid mineral into solution can be described in four stages. At the beginning of the acid ISL process, there was no oxidant to be added to the leaching solution and the desorption of hexavalent uranyl ions in the open pores, as well as dissolution of hexavalent uranium minerals, led to a short-term peak in the pregnant solution, which happened while pH decreased from about 5.3 to 2.62. Following the depletion of the adsorbed hexavalent uranium and a decline in uranium dissolution intensity, the addition of Fe(III) facilitated the oxidation of tetravalent uranium, which enabled intensive uranium mobilization again. During this process, the dissolution of uranium had a strong positive correlation with the reduction of Fe(III) and Eh in the leach solution. Beside hydrochemical factors, the deportment of uranium was also an important factor affecting uranium recovery. Uranium located in the open pores can be completely exposed to the solution and the mobilization intensity was significantly affected by hydrogeochemical conditions; but the uranium present in microfissures and in the ore matrix could not be fully exposed to the solution, so, their dissolution intensity was primarily controlled by corrosion and permeability of the ore. In general, the hydrogeochemical conditions and the deportment of uranium were the external and internal factors that significantly affected the dissolution and recovery of uranium in the early and middle stages of the FLT. However, in the latest stages, due to uranium depletion, enhancing the chemical potential of the leaching solution, specifically acidity and/or the amount of oxidant, had little improvement on uranium recovery.
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Pastukhov, A. M., Rychkov, V. N., Smirnov, A. L., Skripchenko, S. Y., & Poponin, N. A. (2014). Purification of in situ leaching solution for uranium mining by removing solids from suspension. Minerals Engineering, 55, 1–4.
Abstract: This study investigated the process of in situ leaching (ISL) method of uranium mining, and the removal of solid particles from the leaching solution. Investigations were carried out for 4months. The content of firm suspensions in the productive solutions arriving from the well field was up to standard of 3–5mg/l. After keeping in a settler of productive solutions within one hour concentration of suspensions decreases to 2–2.5mg/l. To increase the life of the wells requires more fine purification of the ISL solutions. The best results can be obtained but using filtration. Bag filters were used in experiments carried out at the extraction site. All samples of polypropylene bag filter was produced by the Tamfelt Corporation. The best results were obtained for fabrics S-51M03-L2K4 (pore size 3μm). After three month of trials following indicators of wells work were fixed: on the trial cell decrease in intake capacity did not occur; on the other cells of well field injectability of holes for the same period of time decreased for 15–40%. The results illustrated the high efficiency of this method, which allows injection wells to reach a constant intake capacity, making it possible for technological cells to achieve a constant productivity and balance. Purification of solutions allows to reduce acidulation term of new technological cells from 3–4 to 1.5–2months.
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