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Dutova, E. M., Nikitenkov, A. N., Pokrovskiy, V. D., Banks, D., Frengstad, B. S., & Parnachev, V. P. (2017). Modelling of the dissolution and reprecipitation of uranium under oxidising conditions in the zone of shallow groundwater circulation. Journal of Environmental Radioactivity, 178-179, 63–76.
Abstract: Generic hydrochemical modelling of a grantoid-groundwater system, using the Russian software “HydroGeo”, has been carried out with an emphasis on simulating the accumulation of uranium in the aqueous phase. The baseline model run simulates shallow granitoid aquifers (U content 5 ppm) under conditions broadly representative of southern Norway and southwestern Siberia: i.e. temperature 10 °C, equilibrated with a soil gas partial CO2 pressure (PCO2, open system) of 10−2.5 atm. and a mildly oxidising redox environment (Eh = +50 mV). Modelling indicates that aqueous uranium accumulates in parallel with total dissolved solids (or groundwater mineralisation M – regarded as an indicator of degree of hydrochemical evolution), accumulating most rapidly when M = 550–1000 mg L−1. Accumulation slows at the onset of saturation and precipitation of secondary uranium minerals at M = c. 1000 mg L−1 (which, under baseline modelling conditions, also corresponds approximately to calcite saturation and transition to Na-HCO3 hydrofacies). The secondary minerals are typically “black” uranium oxides of mixed oxidation state (e.g. U3O7 and U4O9). For rock U content of 5–50 ppm, it is possible to generate a wide variety of aqueous uranium concentrations, up to a maximum of just over 1 mg L−1, but with typical concentrations of up to 10 μg L−1 for modest degrees of hydrochemical maturity (as indicated by M). These observations correspond extremely well with real groundwater analyses from the Altai-Sayan region of Russia and Norwegian crystalline bedrock aquifers. The timing (with respect to M) and degree of aqueous uranium accumulation are also sensitive to Eh (greater mobilisation at higher Eh), uranium content of rocks (aqueous concentration increases as rock content increases) and PCO2 (low PCO2 favours higher pH, rapid accumulation of aqueous U and earlier saturation with respect to uranium minerals).
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Xie, T., Lian, B., Chen, C., Qian, T., Liu, X., Shang, Z., et al. (2023). Leaching behaviour and mechanism of U, 226Ra and 210Pb from uranium tailings at different pH conditions. Journal of Environmental Radioactivity, 270, 107300.
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.
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