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Robin, V.; Beaufort, D.; Tertre, E.; Reinholdt, M.; Fromaget, M.; Forestier, S.; Boissezon, H. de; Descostes, M. |
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Title |
Fate of dioctahedral smectites in uranium roll front deposits exploited by acidic In Situ Recovery (ISR) solutions |
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Journal Article |
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Year  |
2020 |
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Applied Clay Science |
Abbreviated Journal |
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Volume |
187 |
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Pages |
105484 |
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Keywords |
Dissolution, In situ recovery, Ion exchange, Post mining, Remediation, Smectite |
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Abstract |
In Situ Recovery (ISR) is the most important process of uranium production in the world (50%). It consists of an injection of a leaching solution into a permeable mineralized aquifer (sandstone), pumping of the solution after dissolution of the ore minerals and recovery of the uranium from the pregnant solution in a surface plant. In this context, the fate of swelling clay minerals such as smectites is of main importance due to their role in the mobility of cationic elements by diverse geochemical processes such as ion-exchange reactions or dissolution. The present study details analysis of dioctahedral smectites before and after in-situ leaching by acidic (H2SO4) ISR solutions. Samples were collected from two sedimentary basins hosting some of the main uranium roll front deposits exploited by acidic ISR (Tortkuduk deposit, Shu-Saryssu basin, Kazakhstan, and Dulaan Uul and Zoovch Ovoo deposits, Sainshand basin, Mongolia). Scanning Electron Microscope and X-Ray Diffraction analysis revealed that dioctahedral smectite is a ubiquitous mineral in all analyzed samples, before and after acidification, and revealed a difference of crystal chemistry of the smectites between deposits of Kazakhstan (beidellite type) and Mongolia (montmorillonite type). Chemical analysis and semi-quantification of the smectites before and after acidification also revealed a difference in chemical reactivity, with a higher dissolution of montmorillonite layers compared to beidellite ones, and the importance of ion-exchange reactions. These findings are consistent with literature data obtained on model systems. The persistence of dioctahedral smectites after several years of acidification is crucial for the understanding of geochemical processes during uranium production or remediation of the aquifers. Finally, based on the analysis of samples from U-deposits hosted in both sedimentary basins, a schematic model of the impact of acid solutions on dioctahedral smectite was proposed. |
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0169-1317 |
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THL @ christoph.kuells @ robin_fate_2020 |
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179 |
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Bonnetti, C.; Zhou, L.; Riegler, T.; Brugger, J.; Fairclough, M. |
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Title |
Large S isotope and trace element fractionations in pyrite of uranium roll front systems result from internally-driven biogeochemical cycle |
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Journal Article |
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Year |
2020 |
Publication |
Geochimica et Cosmochimica Acta |
Abbreviated Journal |
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282 |
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113-132 |
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Keywords |
Activity cycle, Pyrite composition, Roll front uranium deposits, S isotope and trace element fractionation |
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Complex pyrite textures associated with large changes in isotopic and trace element compositions are routinely assumed to be indicative of multi-faceted processes involving multiple fluid and sulfur sources. We propose that the features of ore-stage pyrite from roll front deposits across the world, revealed in exquisite detail via high-resolution trace element mapping by LA-ICP-MS, reflect the dynamic internal evolution of the biogeochemical processes responsible for sulfate reduction, rather than externally driven changes in fluid or sulfur sources through time. Upon percolation of oxidizing fluids into the reduced host-sandstones, roll front systems become self-organized, with a systematic reset of their activity cycle after each translation stage of the redox interface down dip of the aquifer. Dominantly reducing conditions at the redox interface favor the formation of biogenic framboidal pyrite (δ34S from −30.5 to −12.5‰) by bacterial sulfate reduction and the genesis of the U mineralization. As the oxidation front advances, oxidation of reduced sulfur minerals induces an increased supply of sulfate and metals in solution to the bacterial sulfate reduction zone that has similarly advanced down the flow gradient. Hence, this stage is marked by increased rates of the bacterial sulfate reduction associated with the crystallization of variably As-Co-Ni-Mo-enriched concentric pyrite (up to 10,000′s of ppm total trace contents) with moderately negative δ34S values (from −13.7 to −7.5‰). A final stage of pyrite cement with low trace element contents and heavier δ34S signature (from −6.9 to +18.8‰) marks the end of the roll front activity cycle and the transition from an open to a predominantly closed system behavior (negligible advection of fresh sulfate). Blocky pyrite cement is formed using the remaining sulfate, which now becomes quickly heavy according to a Rayleigh isotope fractionation process. This ends the cycle by depleting the nutrient supplies for the sulfate-reducing bacteria and cementing pore spaces within the host sandstone, effectively restricting fluid infiltration. This internally-driven roll front activity cycle results in systematic, large S isotope and trace element fractionation. Ultimately, the long-time evolution of the basin and fluid sources control the metal endowment and evolution of the system; these events, however, are unlikely to be preserved by the roll front, as a direct result of its hydrodynamic nature. |
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0016-7037 |
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THL @ christoph.kuells @ bonnetti_large_2020 |
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185 |
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Zhou, Y.; Li, G.; Xu, L.; Liu, J.; Sun, Z.; Shi, W. |
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Title |
Uranium recovery from sandstone-type uranium deposit by acid in-situ leaching – an example from the Kujieertai |
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Journal Article |
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2020 |
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Hydrometallurgy |
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191 |
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105209 |
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Keywords |
Acid in-situ leaching, Sandstone-type uranium deposit, Uranium deportment in the ore, Uranium recovery, Water-rock interaction |
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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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0304-386x |
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THL @ christoph.kuells @ zhou_uranium_2020 |
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205 |
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Gil-Márquez, J.M.; Sültenfuß, J.; Andreo, B.; Mudarra, M. |
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Groundwater dating tools (3H, 3He, 4He, CFC-12, SF6) coupled with hydrochemistry to evaluate the hydrogeological functioning of complex evaporite-karst settings |
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Journal Article |
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2020 |
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Journal of Hydrology |
Abbreviated Journal |
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580 |
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124263 |
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Groundwater dating, Evaporite karst, Brine spring, Free-shape models |
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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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0022-1694 |
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THL @ christoph.kuells @ Gilmarquez2020124263 |
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213 |
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Jamali, B.; Bach, P.M.; Deletic, A. |
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Title |
Rainwater harvesting for urban flood management – An integrated modelling framework |
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Journal Article |
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2020 |
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Water Research |
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171 |
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115372 |
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Keywords |
Rainwater harvesting tanks, Urban flood simulation, Rapid flood inundation model, Urban flood risk mitigation |
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It is well known that rainwater harvesting (RWH) can augment water supply and reduce stormwater pollutant discharges. Due to the lack of continuous 2D modelling of urban flood coverage and its associated damage, the ability of RWH to reduce urban flood risks has not been fully evaluated. Literature suggests that small distributed storage spaces using RWH tanks will reduce flood damage only during small to medium flooding events and therefore cumulative assessment of their benefits is needed. In this study we developed a new integrated modelling framework that implements a semi-continuous simulation approach to investigate flood prevention and water supply benefits of RWH tanks. The framework includes a continuous mass balance simulation model that considers antecedent rainfall conditions and water demand/usage of tanks and predicts the available storage prior to each storm event. To do so, this model couples a rainfall-runoff tank storage model with a detailed stochastic end-use water demand model. The available storage capacity of tanks is then used as a boundary condition for the novel rapid flood simulation model. This flood model was developed by coupling the U.S. EPA Storm Water Management Model (SWMM) to the Cellular-Automata Fast Flood Evaluation (CA-ffé) model to predict the inundation depth caused by surcharges over the capacity of the drainage network. The stage-depth damage curves method was used to calculate time series of flood damage, which are then directly used for flood risk and cost-benefit analysis. The model was tested through a case study in Melbourne, using a recorded rainfall time series of 85 years (after validating the flood model against 1D-2D MIKE-FLOOD). Results showed that extensive implementation of RWH tanks in the study area is economically feasible and can reduce expected annual damage in the catchment by up to approximately 30 percent. Availability of storage space and temporal distribution of rainfall within an event were important factors affecting tank performance for flood reduction. |
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0043-1354 |
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THL @ christoph.kuells @ Jamali2020115372 |
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239 |
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