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Ren, Y., Yang, X., Hu, X., Wei, J., & Tang, C. (2022). Mineralogical and geochemical evidence for biogenic uranium mineralization in northern Songliao Basin, NE China. Ore Geology Reviews, 141, 104556.
Abstract: The sandstone-hosted uranium mineralization areas in the Sanzhao Sag of the northern Songliao Basin have been newly identified. The target stratum is the Upper Cretaceous Sifangtai Formation and the uranium mineralization mainly occurs in the bottom of Sifangtai Formation, corresponding to channel sand bodies in meandering river system, characterized by medium to fine-grained sandstone. This study proposes the uranium metallogenic model through petrographic observation, whole rock geochemistry, mineralogical study of uranium occurrence form (SEM), organic matter rock–eval pyrolysis analysis (REP) and in-situ sulfur isotope determination of different generations of pyrite by LA-MC-ICP-MS. Compared with the sandstones collected in barren reduction and oxidization zones, the mineralized sandstones show obvious increase in the contents of TOC, total sulfur, Y and U. Petrographic observations indicate that organic matters are mainly inherited from land plants. REP data display that the organic matter (OM) disseminated in the sandstone has very low hydrogen index (HI) from around 0 to 21 mg HC/g TOC and varied oxygen index (OI) from 44 to 115 mg CO2/g TOC, corresponding to Type Ⅳ kerogen (degraded kerogen). There are two types of coffinite with different grain size, micro-particles (μm-sized) and large aggregates (generally up to 100 μm) respectively. The coffinite micro spherules exhibit short rod-like or worm-like morphology occurring in clay matrix and cell cavities in degradofusinite or around subidiomorphic-idiomorphic pyrite. The coarse-grained coffinite contains other mineral facies (e.g. pyrite, quartz) and some of large coffinite aggregates display thrombolite-type microbial structures. The irregular pyrite relict particles in coarse-grained colloidal coffinite have light sulfur isotope compositions characterized by δ34S values from –39.96‰ to –49.89‰. The δ34S values of colloidal pyrite in replacement of OM or of the sub-idiomorphic FeS2 cement filling in the cavities of OM range from –52.77‰ to –13.88‰. Some of sub-idiomorphic pyrite cement and idiomorphic crystal have the heavier signature from – 27.06‰ to + 14.23‰. The light sulfur isotope signature suggests that the sulfur originates from bacterial sulfate reduction (BSR). The OM replacement by pyrite and the highest OI values recorded by REP in uranium mineralized samples are lines of evidence of biodegradation. Bacteria use the organic matter as food source and produce isotopically light reduced sulfur species. Oxygenated uranium-bearing waters infiltrated through the denudated windows at Daqing placanticline into the porous reduced sandstones deposited in the Sanzhao Sag. Uranium was indirectly reduced by BSR-derived iron disulfides or directly reduced by sulfate-reducing bacteria.
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Sahoo, P. K., Virk, H. S., Powell, M. A., Kumar, R., Pattanaik, J. K., Salomão, G. N., et al. (2022). Meta-analysis of uranium contamination in groundwater of the alluvial plains of Punjab, northwest India: Status, health risk, and hydrogeochemical processes. Science of The Total Environment, 807, 151753.
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.
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Kumar, V., Setia, R., Pandita, S., Singh, S., & Mitran, T. (2022). Assessment of U and As in groundwater of India: A meta-analysis. Chemosphere, 303, 135199.
Abstract: More than 2.5 billion people depend upon groundwater worldwide for drinking, and giving quality water has become one of the great apprehensions of human culture. The contamination of Uranium (U) and Arsenic (As) in the groundwater of India is gaining global attention. The current review provides state-of-the-art groundwater contamination with U and As in different zones of India based on geology and soil texture. The average concentration of U in different zones of India was in the order: West Zone (41.07 μg/L) \textgreater North Zone (37.7 μg/L) \textgreater South Zone (13.5 μg/L)\textgreater Central Zone (7.4 μg/L) \textgreater East Zone (5.7 μg/L) \textgreaterSoutheast Zone (2.4 μg/L). The average concentration of As in groundwater of India is in the order: South Zone (369.7 μg/L)\textgreaterCentral Zone (260.4 μg/L)\textgreaterNorth Zone (67.7 μg/L)\textgreaterEast Zone (60.3 μg/L)\textgreaterNorth-east zone (9.78 μg/L)\textgreaterWest zone (4.14 μg/L). The highest concentration of U and As were found in quaternary sediments, but U in clay skeletal and As in loamy skeletal. Results of health risk assessment showed that the average health quotient of U in groundwater for children and adults was less than unity. In contrast, it was greater than unity for As posing a harmful impact on human health. This review provides the baseline data regarding the U and As contamination status in groundwater of India, and appropriate, effective control measures need to be taken to control this problem.
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Grozeva, N. G., Radwan, J., Beaucaire, C., & Descostes, M. (2022). Reactive transport modeling of U and Ra mobility in roll-front uranium deposits: Parameters influencing 226Ra/238U disequilibria. Journal of Geochemical Exploration, 236, 106961.
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.
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Zhang, H., Gao, J., Xu, L., & Zhang, X. (2022). Case studies of radioactivity of drilling mud for in situ leaching uranium mining in China. Journal of Environmental Radioactivity, 251-252, 106982.
Abstract: The drilling mud from in situ leaching uranium mining is a type of low-radioactivity waste that contains natural nuclides and other harmful substances. In order to determine whether the drilling mud can meet the requirements of radioactive exemption management standards, field investigations and data simulations were conducted in this study. Two typical uranium mines were selected for onsite investigations. Drilling mud from different layers (i.e., the upper covering layer and ore-bearing layer) and from different stages (e.g., logging stage mud, drilling expansion stage mud, and mixed mud) was sampled. For each sample, the 238U and 226Ra concentrations of the solid components and the U and 226Ra concentrations of the supernatant were analyzed. The results revealed that the highest 238U and 226Ra concentrations of the solid components were 4122 Bq/kg and 4077 Bq/kg, while the 238U and 226Ra concentrations of the mixed drilling mud were all less than 300 Bq/kg. A radioactivity estimation model was established for scenario analysis. Exemption management screening lines of waste drilling mud, which can be used to classify and treat the drilling project according to the deposit’s grade and conditions, were proposed for in situ leaching drilling projects.
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Zeng, S., Shen, Y., Sun, B., Tan, K., Zhang, S., & Ye, W. (2022). Fractal kinetic characteristics of uranium leaching from low permeability uranium-bearing sandstone. Nuclear Engineering and Technology, 54(4), 1175–1184.
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.
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Wang, B., Luo, Y., Liu, J. -hui, Li, X., Zheng, Z. -hong, Chen, Q. -qian, et al. (2022). Ion migration in in-situ leaching (ISL) of uranium: Field trial and reactive transport modelling. Journal of Hydrology, 615, 128634.
Abstract: Acid in-situ leaching (ISL) can be used as a mining technique for in situ uranium recover from underground. Acids and oxidants as lixiviants were continuously injected into a sandstone-type uranium deposit in Bayan-Uul (China). It was conducted to facilitate the dissolution of uranium minerals to generate uranyl ions, which could then be extracted for the recovery of uranium resources by the pumping cycle. A reactive transport model based on PHAST was developed to investigate the dynamic reactive migration process of uranium. The simulated results well reproduce the fluid dynamic evolution in the injecting and pumping units, as well as the dynamic release of uranium. The simulated leaching area indicates that the uranium ore leaching area was much larger than the acidification area. In addition, the pollution plume of uranium and acid water was larger than that of the leaching area, which can be used as a reference for uranium mining schemes. Furthermore, the parameter sensitivity analysis indicates the volume fraction of uranium ore and the reaction rate were the main factors affecting uranium leaching efficiency. Without considering the blockage of pores by precipitation, the Fe2+ in the reinjection fluid had a significant negative influence on uranium leaching.
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Jana, A., Unni, A., Ravuru, S. S., Das, A., Das, D., Biswas, S., et al. (2022). In-situ polymerization into the basal spacing of LDH for selective and enhanced uranium adsorption: A case study with real life uranium alkaline leach liquor. Chemical Engineering Journal, 428, 131180.
Abstract: Uranium is used as a fuel for nuclear power plant and can be extracted from different ores, mainly acidic (silicious ore) and alkaline (carbonate ore). Recovery of uranium through acid leaching from silicious ore is well established, whereas, alkaline leaching from carbonate ore is challenging due to the excessive salinity of leach liquor and high concentration of carbonate, bicarbonate and sulphate. Herein, two monomers, acrylic acid (AA) and N, N-methylene bisacrylamide (BAM), selective towards uranyl were intercalated in-situ into the interlayer, followed by their polymerization and cross-linking to form novel polymer intercalated hybrid layered double hydroxide (LDH). The LDH acts as a backbone to overcome coiling and swelling of polymer and anchors them as free-standing. Various parameters, like, the type of metal ions, monomer ratio (AA: BAM) and metal ion ratio (M2+:M3+), were studied to determine the optimum conditions for effective intercalation and polymerization of monomers. Magnesium aluminum (MgAl) LDH with a cross-linked polymer having a monomer ratio of 3:2 (AA: BAM) as intercalating species showed maximum efficiency of uranyl adsorption (1456 mg/g at 30 °C) with highest capacity so far. The distribution coefficient (Kd, l/mg) in the order of 105 suggested that the adsorbent was highly selective for uranyl in the presence of different cations, anions and humic acid. The adsorbent extracts uranium effectively and selectively from a real-life alkaline leach liquor with an efficiency of 96% at 5 g/l dose. Uranium can be recovered from the adsorbent in the form of sodium di-uranate using 2(M) NaOH and was reused for eight cycles.
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Romeo, N., Mabry, J., Hillegonds, D., Kainz, G., Jaklitsch, M., & Matsumoto, T. (2022). Developments of a field gas extraction device and krypton purification system for groundwater radio-krypton dating at the IAEA. Applied Radiation and Isotopes, 189, 110450.
Abstract: The long-lived radio-krypton isotope 81Kr (t1/2 = 2.29 × 105 yr) is an ideal tracer for old groundwater age dating in the range of 105–106 years which goes beyond the reach of radio-carbon (14C) age dating. Analytical breakthrough made over the last two decades in Atom Trap Trace Analysis (ATTA) has enabled the use of this isotope with extremely low abundance (81Kr/Kr = 6 × 10−13) to be used as a practical dating tool for very old groundwater. The International Atomic Energy Agency aims to provide this new isotope tool for better groundwater resource management of Member States and developed a field sampling device to collect dissolved gas samples from groundwater and a system to separate and purify trace amounts of krypton from the gas samples for the ATTA analysis. The design, setup and performances of our sampling and purification systems are described here. Our system can produce a high purity aliquot of about 5 μL of krypton from 5 L of air sample (recovery yield of >90%). The samples made by our system were confirmed to be acceptable for the ATTA analysis.
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Xu, W. D., Burns, M. J., Cherqui, F., Duchesne, S., Pelletier, G., & Fletcher, T. D. (2022). Real-time controlled rainwater harvesting systems can improve the performance of stormwater networks. Journal of Hydrology, 614, 128503.
Abstract: Real-Time Control (RTC) technology is increasingly applied in Rainwater Harvesting (RWH) systems to optimise their performance related to water supply and flood mitigation. However, most studies to date have focussed on testing the benefits at an individual site scale, leaving the potential benefits for downstream stormwater networks largely untested. In this study, we developed a methodology to predict how at-source RTC RWH systems influence the behaviour of a stormwater network. Simulation was enabled by coupling the drainage model in SWMM with an RTC RWH model coded using the R software. We modelled two different RTC strategies across a range of system settings (e.g. storage size for RWH and proportion of storage to which RTC is applied) under two different climate scenarios—current and future climates. The simulations showed that RTC reduced flooding volume and peak flow of the stormwater network, leading to a potential mitigation of urban flooding risks, while also providing a decentralised supplementary water supply. Implementing RTC in more of RWH storages yielded greater benefits than simply increasing storage capacity, in both current and future climates. More importantly, the RTC systems are capable of more precisely managing the resultant flow regime in reducing the erosion and restoring the pre-development conditions in sensitive receiving waters. Our study suggests that RTC RWH storages distributed throughout a catchment can substantially improve the performance of existing drainage systems, potentially avoiding or deferring expensive network upgrades. Investments in real-time control technology would appear to be more promising than investments in detention volume alone.
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