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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 |
Publication |
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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Petisco-Ferrero, S.; Idoeta, R.; Rozas, S.; Olondo, C.; Herranz, M. |
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Title |
Radiological environmental monitoring of groundwater around NPP: A proposal for its assessment |
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Journal Article |
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Year |
2023 |
Publication |
Heliyon |
Abbreviated Journal |
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9 |
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9 |
Pages |
19470 |
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Keywords |
Detection limit, Nuclear power plant dismantling and decommissioning, Radiological environmental monitoring, Radionuclides in groundwater |
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Abstract |
Whether a nuclear installation has radiological impact and, in that case, its extension, are the questions behind any environmental analysis of the installation along its operational life. This analysis is based on the detailed establishment of the radiological background of the area. Accordingly, the dismantling and decommissioning process (D&D) of a nuclear power plant starts with a radiological monitoring plan, which includes the radiological characterization of the area and of its surroundings. At the completion of the D&D, unrestricted use for the site will be permitted strictly in accordance with results of the radiological survey within the limits established by the local authorities. Groundwater quality is typically included in any radiological analysis since, among other reasons, a significant part of it is highly likely to end up being extracted for domestic use and hence, human consumption. While there is no regulation containing maximum activity concentration or radionuclide guidance values for water that may be destined for uses other than public consumption, if groundwater is considered a “part” of the land, dose criteria for site release can be applied. Therefore, together with the guidance levels to be established for the different radionuclides expected in the groundwater, the detection limits to be employed when performing routine radio analytical characterization procedures in the laboratory should also be provided. In this paper, we first propose a relation of the potential radionuclides to be analyzed in groundwater, together with their detection limits to be achieved when the determinations are performed in a laboratory, and subsequently, we discuss the most suitable analytical methodologies and resources that would be necessary to undertake radiological characterization plans from a practical point of view. |
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2405-8440 |
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THL @ christoph.kuells @ petisco-ferrero_radiological_2023 |
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133 |
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Paradis, C.J.; Hoss, K.N.; Meurer, C.E.; Hatami, J.L.; Dangelmayr, M.A.; Tigar, A.D.; Johnson, R.H. |
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Elucidating mobilization mechanisms of uranium during recharge of river water to contaminated groundwater |
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Journal Article |
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2022 |
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Journal of Contaminant Hydrology |
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251 |
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104076 |
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Keywords |
Desorption, Dissolution, Groundwater, Surface water, Tracer, Uranium |
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The recharge of stream water below the baseflow water table can mobilize groundwater contaminants, particularly redox-sensitive and sorptive metals such as uranium. However, in-situ tracer experiments that simulate the recharge of stream water to uranium-contaminated groundwater are lacking, thus limiting the understanding of the potential mechanisms that control the mobility of uranium at the field scale. In this study, a field tracer test was conducted by injecting 100 gal (379 l) of oxic river water into a nearby suboxic and uranium-contaminated aquifer. The traced river water was monitored for 18 days in the single injection well and in the twelve surrounding observation wells. Mobilization of uranium from the solid to the aqueous phase was not observed during the tracer test despite its pre-test presence being confirmed on the aquifer sediments from lab-based acid leaching. However, strong evidence of oxidative immobilization of iron and manganese was observed during the tracer test and suggested that immobile uranium was likely in its oxidized state as U(VI) on the aquifer sediments; these observations ruled out oxidation of U(IV) to U(VI) as a potential mobilization mechanism. Therefore, desorption of U(VI) appeared to be the predominant potential mobilization mechanism, yet it was clearly not solely dependent on concentration as evident when considering that uranium-poor river water (\textless0.015 mg/L) was recharged to uranium-rich groundwater (≈1 mg/L). It was possible that uranium desorption was limited by the relatively higher pH and lower alkalinity of the river water as compared to the groundwater; both factors favor immobilization. However, it was likely that the immobile uranium was associated with a mineral phase, as opposed to a sorbed phase, thus desorption may not have been possible. The results of this field tracer study successfully ruled out two common mobilization mechanisms of uranium: (1) oxidative dissolution and (2) concentration-dependent desorption and ruled in the importance of advection, dispersion, and the mineral phase of uranium. |
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0169-7722 |
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THL @ christoph.kuells @ paradis_elucidating_2022 |
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135 |
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Ammar, F.H.; Deschamps, P.; Chkir, N.; Zouari, K.; Agoune, A.; Hamelin, B. |
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Uranium isotopes as tracers of groundwater evolution in the Complexe Terminal aquifer of southern Tunisia |
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Journal Article |
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2020 |
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Quaternary International |
Abbreviated Journal |
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547 |
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33-49 |
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CT southern Tunisia, Holocene, Mixing, Radicarbon, Uranium isotopes, Water-rock interaction |
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The Complexe Terminal (CT) multi-layer aquifer is formed by Neogene/Paleogene sand deposits, Upper Senonian (Campanian-Maastrichtian limestones) and Turonian carbonates. The chemical composition and isotopes of carbon and uranium were investigated in groundwater sampled from the main hydrogeological units of the (CT) aquifer in southern Tunisia. We paid special attention to the variability of uranium contents and isotopes ratio (234U/238U) to provide a better understanding of the evolution of the groundwater system. Uranium concentrations range from 1.5 to 19.5 ppb, typical of oxic or mildly reducing conditions in groundwaters. The lowest concentrations are found southeast of the study area, where active recharge is supposed to take place. When looking at the isotope composition, it appears that all the samples, including those from carbonate levels, are in radioactive disequilibrium with significant 234U excess. A clear-cut distinction is observed between Turonian and Senonian carbonate aquifers on the one hand, with 234U/238U activity ratios between 1.1 and 1.8, and the sandy aquifer on the other hand, showing higher ratios from 1.8 to 3.2. The distribution of uranium in this complex aquifer system seems to be in agreement with the lithological variability and are ultimately a function of a number of physical and chemical factors including the uranium content of the hosting geological formation, water-rock interaction and mixing between waters having different isotopic signatures. Significant relationships also appear when comparing the uranium distribution with the major ions composition. It is noticeable that uranium is better correlated with sulfate, calcium and magnesium than with other major ions as chloride or bicarbonate. The 14C activities and δ13C values of DIC cover a wide range of values, from 1.1 pmc to 30.2 pmc and from −3.6‰ to −10.7‰, respectively. 14C model ages estimated by the Fontes and Garnier model are all younger than 22 Ka and indicate that the recharge of CT groundwater occurred mainly during the end of the last Glacial and throughout the Holocene. |
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1040-6182 |
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THL @ christoph.kuells @ ammar_uranium_2020 |
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119 |
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Gimeno, M.J.; Tullborg, E.-L.; Nilsson, A.-C.; Auqué, L.F.; Nilsson, L. |
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Hydrogeochemical characterisation of the groundwater in the crystalline basement of Forsmark, the selected area for the geological nuclear repositories in Sweden |
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Journal Article |
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2023 |
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Journal of Hydrology |
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624 |
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129818 |
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Crystalline bedrock, Deep geological repository, Glacial meltwater intrusion, Groundwater mixing, Hydrogeochemical model, Nuclear waste disposal |
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Numerous groundwater analyses from the crystalline bedrock in the Forsmark area have been performed between 2002 and 2019, together with thorough geological, geophysical, and hydrogeological studies, within the site investigations carried out by the Swedish Nuclear Fuel and Waste Management Company. The groundwater samples have been taken from boreholes down to ≈ 1000 m and the analysis include major- and trace-elements, stable and radiogenic isotopes, gases and microbes. The chemical and isotopic composition of these groundwaters evidences the presence of non-marine brackish to saline groundwaters with very long residence times (many hundreds of thousands of years) and a series of complex mixing events resulting from the recharge of different waters over time: glacial meltwaters, probably from different glaciations of which the latest culminated some 20,000 years ago, and marine waters from the Baltic starting some 7000 years ago. Later, meteoric water and present Baltic Sea water have recharged in different parts of the upper 100 m. These mixing events have also triggered chemical and microbial reactions that have conditioned some of the important groundwater parameters and, together with the structural complexity of the area, they have promoted a heterogeneous distribution of groundwater compositions in the bedrock. Due to these evident differences in chemistry, residence time and origin of the groundwater, several groundwater types were defined in order to facilitate the visualisation and communication. The differentiation (linked to the paleohydrological history of the area) was based on Cl concentration, Cl/Mg ratio (marine component), and δ18O value (glacial component). The work presented in this paper increases the understanding of the groundwater evolution in fractured and compartmentalised aquifers where mixing processes are the most important mechanisms. The model proposed to characterise the present groundwater system of the Forsmark area will also help to predict the future hydrogeochemical behaviour of the groundwater system after the construction of the repositories for the nuclear wastes. |
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0022-1694 |
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THL @ christoph.kuells @ gimeno_hydrogeochemical_2023 |
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137 |
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