Abstract: Uranium reserve estimates in ore deposits can be significantly impacted by 226Ra/238U disequilibria arising from the differential mobility of uranium and radium during groundwater transport. 1D reactive transport models were developed to investigate the long-term effects of retention processes (UO2(am) precipitation, U(VI) and Ra sorption on smectite, Ra co-precipitation with barite) on the repartitioning of 238U and 226Ra during formation of roll-front type deposits. Analytical solutions to radioactive decay chains were used in complement to examine the influence of geochemical parameters, including fluid 234U/238U activity ratios and α-recoil loss, on 226Ra/238U disequilibria in uranium ores. Model results demonstrate that smectite and barite can produce 226Ra/238U ratios \textgreater1 at low uranium contents and may explain 226Ra/238U disequilibria occurring in altered rock up- and downstream of roll-front deposits. The capacity of these phases to take up Ra and generate 226Ra/238U disequilibria depends on both mineral contents and groundwater compositions, and is thus expected to be site-specific. Simulations of ore deposits that advance downstream with time demonstrate the formation of stronger 226Ra/238U disequilibria, as expected, in the downgradient side or nose of the ore, reflecting both younger mineralization ages and the presence of active uranium precipitation. Whether disequilibria are positive or negative with respect to secular equilibrium, however, depends on the 234U/238U activity ratio in the fluid from which uranium minerals precipitate. Smaller hydraulic conductivities are shown to generate a narrower range in 226Ra/238U activity ratios with distance, and may explain the occurrence of disequilibria in the limb ore that are less pronounced than those in the nose. Furthermore, the ability of α-recoil loss to decrease 226Ra/238U activity ratios at secular equilibrium may account for negative disequilibria in high grade ores. The South Tortkuduk uranium deposits (Kazakhstan) are subsequently used as a case study to identify the processes and parameters that may contribute to 226Ra/238U disequilibria at this site. Variations in multiple parameters, including clay contents, barite contents, and mineralization ages, are found to reproduce measured 226Ra/238U activity ratios in the roll-front ore. Prioritization of these parameters will necessitate field measurements targeting both groundwater fluids and the host rock. Results from this study will ultimately aid geologists in building appropriate hydrogeochemical data sets to more efficiently locate and exploit uranium ore deposits.

Abstract: Uranium (U) roll-front deposits constitute a valuable source for an economical extraction by in situ recovery (ISR) mining. Such technology may induce changes in the subsurface microbiota, raising questions about the way their activities could build a functional ecosystem in such extreme environments (i.e.: oligotrophy and high SO4 concentration and salinity). Additionally, more information is needed to dissipate the doubts about the microbial role in the genesis of such U orebodies. A U roll-front deposit hosted in an aquifer driven system (in Zoovch Ovoo, Mongolia), intended for mining by acid ISR, was previously explored and showed to be governed by a complex bacterial diversity, linked to the redox zonation and the geochemical conditions. Here for the first time, transcriptional activities of microorganisms living in such U ore deposits are determined and their metabolic capabilities allocated in the three redox-inherited compartments, naturally defined by the roll-front system. Several genes encoding for crucial metabolic pathways demonstrated a strong biological role controlling the subsurface cycling of many elements including nitrate, sulfate, metals and radionuclides (e.g.: uranium), through oxidation-reduction reactions. Interestingly, the discovered transcriptional behaviour gives important insights into the good microbial adaptation to the geochemical conditions and their active contribution to the stabilization of the U ore deposits. Overall, evidences on the importance of these microbial metabolic activities in the aquifer system are discussed that may clarify the doubts on the microbial role in the genesis of low-temperature U roll-front deposits, along the Zoovch Ovoo mine.

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.