Abstract: Despite numerous studies, there are many knowledge gaps in our understanding of uranium (U) contamination in the alluvial aquifers of Punjab, India. In this study, a large hydrogeochemical dataset was compiled to better understand the major factors controlling the mobility and enrichment of uranium (U) in this groundwater system. The results showed that shallow groundwaters (\textless60 m) are more contaminated with U than from deeper depths (\textgreater60 m). This effect was predominant in the Southwest districts of the Malwa, facing significant risk due to chemical toxicity of U. Groundwaters are mostly oxidizing and alkaline (median pH: 7.25 to 7.33) in nature. Spearman correlation analysis showed that U concentrations are more closely related to total dissolved solids (TDS), salinity, Na, K, HCO3−, NO3− Cl−, and F− in shallow water than deep water, but TDS and salinity remained highly correlated (U-TDS: ρ = 0.5 to 0.6; U-salinity: ρ = 0.5). This correlation suggests that the salt effect due to high competition between ions is the principal cause of U mobilization. This effect is evident when the U level increased with increasing mixed water species (Na-Cl, Mg-Cl, and Na-HCO3). Speciation data showed that the most dominant U species are Ca2UO2(CO3)2− and CaUO2(CO3)3−, which are responsible for the U mobility. Based on the field parameters, TDS along with pH and oxidation-reduction potential (ORP) were better fitted to U concentration above the WHO guideline value (30 μg.L−1), thus this combination could be used as a quick indicator of U contamination. The strong positive correlation of U with F− (ρ = 0.5) in shallow waters indicates that their primary source is geogenic, while anthropogenic factors such as canal irrigation, groundwater table decline, and use of agrochemicals (mainly nitrate fertilizers) as well as climate-related factors i.e., high evaporation under arid/semi-arid climatic conditions, which result in higher redox and TDS/salinity levels, may greatly affect enrichment of U. The geochemical rationale of this study will provide Science-based-policy implications for U health risk assessment in this region and further extrapolate these findings to other arid/semi-arid areas worldwide.

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: The pore structure of uranium-bearing sandstone is one of the critical factors that affect the uranium leaching performance. In this article, uranium-bearing sandstone from the Yili Basin, Xinjiang, China, was taken as the research object. The fractal characteristics of the pore structure of the uranium-bearing sandstone were studied using mercury intrusion experiments and fractal theory, and the fractal dimension of the uranium-bearing sandstone was calculated. In addition, the effect of the fractal characteristics of the pore structure of the uranium-bearing sandstone on the uranium leaching kinetics was studied. Then, the kinetics was analyzed using a shrinking nuclear model, and it was determined that the rate of uranium leaching is mainly controlled by the diffusion reaction, and the dissolution rate constant (K) is linearly related to the pore specific surface fractal dimension (DS) and the pore volume fractal dimension (DV). Eventually, fractal kinetic models for predicting the in-situ leaching kinetics were established using the unreacted shrinking core model, and the linear relationship between the fractal dimension of the sample’s pore structure and the dissolution rate during the leaching was fitted.