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Liu, Z.; Li, C.; Tan, K.; Li, Y.; Tan, W.; Li, X.; Zhang, C.; Meng, S.; Liu, L. |
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Title |
Study of natural attenuation after acid in situ leaching of uranium mines using isotope fractionation and geochemical data |
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Journal Article |
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Year |
2023 |
Publication |
Science of The Total Environment |
Abbreviated Journal |
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Volume |
865 |
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Pages |
161033 |
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Keywords |
Acid in situ leaching, Geochemical and isotopic tracing, Groundwater contamination, Natural attenuation, Uranium post-mining |
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Abstract |
Acid in situ leaching (AISL) is a subsurface mining approach suitable for low-grade ores which does not generate tailings, and has been adopted widely in uranium mining. However, this technique causes an extremely high concentration of contaminants at post-mining sites and in the surroundings soon after the mining ceases. As a potential AISL remediation strategy, natural attenuation has not been studied in detail. To address this problem, groundwater collected from 26 wells located within, adjacent, upgradient, and downgradient of a post-mining site were chosen to analyze the fate of U(VI), SO42−, δ34S, and δ238U, to reveal the main mechanisms governing the migration and attenuation of the dominant contaminants and the spatio-temporal evolutions of contaminants in the confined aquifer of the post-mining site. The δ238U values vary from −0.07 ‰ to 0.09 ‰ in the post-mining site and from −1.43 ‰ to 0.03 ‰ around the post-mining site. The δ34S values were found to vary from 3.3 ‰ to 6.2 ‰ in the post-mining site and from 6.0 ‰ to 11.0 ‰ around the post-mining site. Detailed analysis suggests that there are large differences between the range of isotopic composition variation and the range of pollutants concentration distribution, and the estimated Rayleigh isotope fractionation factor is 0.9994–0.9997 for uranium and 1.0032–1.0061 for sulfur. The isotope ratio of uranium and sulfur can be used to deduce the migration history of the contaminants and the irreversibility of the natural attenuation process in the anoxic confined aquifer. Combining the isotopic fractionation data for U and S with the concentrations of uranium and sulfate improved the accuracy of understanding of reducing conditions along the flow path. The study also indicated that as long as the geological conditions are favorable for redox reactions, natural attenuation could be used as a cost-effective remediation scheme. |
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0048-9697 |
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THL @ christoph.kuells @ liu_study_2023 |
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155 |
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Liu, Z.; Tan, K.; Li, C.; Li, Y.; Zhang, C.; Song, J.; Liu, L. |
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Title |
Geochemical and S isotopic studies of pollutant evolution in groundwater after acid in situ leaching in a uranium mine area in Xinjiang |
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Journal Article |
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Year |
2023 |
Publication |
Nuclear Engineering and Technology |
Abbreviated Journal |
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55 |
Issue |
4 |
Pages |
1476-1484 |
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Keywords |
Acid in situ leaching of uranium, Pollution evolution, Sulfate elimination, Sulfur isotopes analysis |
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Abstract |
Laboratory experiments and point monitoring of reservoir sediments have proven that stable sulfate reduction (SSR) can lower the concentrations of toxic metals and sulfate in acidic groundwater for a long time. Here, we hypothesize that SSR occurred during in situ leaching after uranium mining, which can impact the fate of acid groundwater in an entire region. To test this, we applied a sulfur isotope fractionation method to analyze the mechanism for natural attenuation of contaminated groundwater produced by acid in situ leaching of uranium (Xinjiang, China). The results showed that δ34S increased over time after the cessation of uranium mining, and natural attenuation caused considerable, area-scale immobilization of sulfur corresponding to retention levels of 5.3%–48.3% while simultaneously decreasing the concentration of uranium. Isotopic evidence for SSR in the area, together with evidence for changes of pollutant concentrations, suggest that area-scale SSR is most likely also important at other acid mining sites for uranium, where retention of acid groundwater may be strengthened through natural attenuation. To recapitulate, the sulfur isotope fractionation method constitutes a relatively accurate tool for quantification of spatiotemporal trends for groundwater during migration and transformation resulting from acid in situ leaching of uranium in northern China. |
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1738-5733 |
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THL @ christoph.kuells @ liu_geochemical_2023 |
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192 |
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Qiu, W.; Yang, Y.; Song, J.; Que, W.; Liu, Z.; Weng, H.; Wu, J.; Wu, J. |
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Title |
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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0883-2927 |
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THL @ christoph.kuells @ qiu_what_2023 |
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207 |
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Author |
Su, X.; Liu, Z.; Yao, Y.; Du, Z. |
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Title |
Petrology, mineralogy, and ore leaching of sandstone-hosted uranium deposits in the Ordos Basin, North China |
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Journal Article |
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2020 |
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Ore Geology Reviews |
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127 |
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103768 |
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Geochemical composition, leach mining, Mineralogy, Ordos Basin, Sandstone-hosted uranium deposit |
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The Nalinggou–Daying uranium metallogenic belt is situated at the northern Ordos Basin, China. Petrographical, mineralogical and geochemical techniques were used to study the ore-bearing sandstones and host rocks in the Nalinggou–Daying uranium metallogenic belt. The present study shows that uranium minerals, i.e., coffinite, pitchblende, and brannerite, are mostly disseminated around pyrite and detrital particles. The ore-bearing sandstones are enriched in organic matter, with which this reductive environment influenced uranium leaching. The carbonate concentration of the uranium ores is markedly higher than that of the host rocks, and intense carbonatization occurs in the ore-bearing sandstones. In this case, the usage of the classical in-situ leach uranium mining technique by injecting H2SO4 + H2O2 solution produces calcium sulfate precipitate, which can lead to blocking of the ore-bearing strata. For this reason, laboratory and field uranium mining tests were conducted using CO2 + O2 in-situ leaching technology and were demonstrated to be successful, illustrating that this approach is technically feasible. Inhibiting ore bed blockage and increasing the amount of injected O2 are important for uranium leaching in this setting. |
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0169-1368 |
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THL @ christoph.kuells @ su_petrology_2020 |
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120 |
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