Retention Of Uranium Research Articles

Human exposure to uranium through drinking water and its detrimental impact on the human body organs.

Human exposure to high concentrations of uranium is a major concern due to the risk of developing numerous internal organ malignancies over time. In addition to the numerous attributes of uranium in the nuclear power industry, the radiological characteristics and chemical toxicity of uranium present a substantial risk to human health. This study aims to evaluate potential negative health impacts associated with the ingestion of uranium through drinking water in the Noida and Greater Noida region within the Gautam Buddha districts of Uttar Pradesh (India), due to extreme industrial revolution in this geological location. The mean concentration of uranium in drinking water of the examined area was estimated to range from 0.23 to 78.21µgl-1. The hair compartment biokinetic model is used to estimate the retention and radiological doses of uranium in distinct organs and tissues. Studies on time-dependent factors revealed variations in uranium retention, with lower levels observed in the Gastrointestinal Tract (GIT) region and higher levels on cortical bone surfaces causes the skeletal deformities. The kidney, liver, and other soft tissues (OST) exhibited a non-saturation pattern in the retention of uranium via exposure of drinking water. The age-wise non-carcinogenic and carcinogenic doses were estimated for the health hazards studies. The outcome of this study will be useful for water resource management authorities to supply safe potable water to the local residents.

Estimation of uranium retention, radiological and chemical doses from the exposure of uranium through drinking water

Estimation of uranium retention, radiological and chemical doses from the exposure of uranium through drinking water

The impact of uranium contamination in groundwater on human health: a toxicological risk assessment

ABSTRACT All living beings are exposed to naturally occurring radionuclides. Uranium, a primordial radionuclide forms compounds that are water soluble and enter the human body through food and drinking water. This study conducted a health risk assessment to evaluate the potential dangers associated with consuming uranium through groundwater in the Mansa district of Punjab, India. The uranium concentration varied from 43.43 µg/L to 449.79 µg/L. The biokinetic model of uranium including hair compartment as excretion pathway is used to calculate uranium retention in different organs of the human body. The Pearson correlation and principal component analysis are used for assessing the correlation of uranium with TDS, salinity, conductivity and pH. The high correlation is observed between TDS and uranium. The hazard quotient is 17.42 and excess cancer risk is higher than the permissible limit of 10−4. Owing to the high uranium concentration in Mansa district, periodic monitoring is advised along with clinical investigation of the population.

Machine learning surrogates for surface complexation model of uranium sorption to oxides

The safety assessments of the geological storage of spent nuclear fuel require understanding the underground radionuclide mobility in case of a leakage from multi-barrier canisters. Uranium, the most common radionuclide in non-reprocessed spent nuclear fuels, is immobile in reduced form (U(IV) and highly mobile in an oxidized state (U(VI)). The latter form is considered one of the most dangerous environmental threats in the safety assessments of spent nuclear fuel repositories. The sorption of uranium to mineral surfaces surrounding the repository limits their mobility. We quantify uranium sorption using surface complexation models (SCMs). Unfortunately, numerical SCM solvers often encounter convergence problems due to the complex nature of convoluted equations and correlations between model parameters. This study explored two machine learning surrogates for the 2-pK Triple Layer Model of uranium retention by oxide surfaces if released as U(IV) in the oxidizing conditions: random forest regressor and deep neural networks. Our surrogate models, particularly DNN, accurately reproduce SCM model predictions at a fraction of the computational cost without any convergence issues. The safety assessment of spent fuel repositories, specifically the migration of leaked radioactive waste, will benefit from having ultrafast AI/ML surrogates for the computationally expensive sorption models that can be easily incorporated into larger-scale contaminant migration models. One such model is presented here.

Shielding process for the effect of anions on uranium selective recovery and heavy metal removal from simulated mine effluents

The selective separation of uranium from uranium tailing wastewater is of great importance for environmental protection and nuclear energy development. The complexation of Cl−, SO42−, NO3–, and PO43− with UO22+ seriously hindered the achievement of this goal. Herein, a process for achieving it with the coexistence of anions and cations by shielding the influence of anions was designed. Thermodynamic calculations indicated that CO32– could enhance the retention of uranium in the solution by complexing with UO22+ and capturing UO22+ in UO2SO4 and UO2HPO4 to form water-soluble uranyl-carbonate. The capturing ability of CO32– was not diminished by the increase in anion concentration. And the electrochemical experiments revealed the high efficiency of uranium electrochemical extraction in the above system. In addition, the results showed that uranium could be separated from Co2+, Cd2+, and Ni2+ ions under the coexistence of Cl−, SO42−, NO3–, and PO43−, thus achieving the selective separation of uranium in the wastewater. And the retention ratio of impurity cations in the liquid phase after separation was less than 0.003. Overall, this method provides new insights into the selective separation of uranium and heavy metal removal in real uranium tailings wastewater.

Renal toxicity and biokinetics models after repeated uranium instillation

During nuclear fuel processing, workers can potentially be exposed to repeated inhalations of uranium compounds. Uranium nephrotoxicity is well documented after acute uranium intake, but it is controversial after long-term or protracted exposure. This study aims to analyze the nephrotoxicity threshold after repeated uranium exposure through upper airways and to investigate the resulting uranium biokinetics in comparison to reference models. Mice (C57BL/6J) were exposed to uranyl nitrate (0.03–3 mg/kg/day) via intranasal instillation four times a week for two weeks. Concentrations of uranium in urines and tissues were measured at regular time points (from day 1 to 91 post-exposure). At each exposure level, the amount of uranium retained in organs/tissues (kidney, lung, bone, nasal compartment, carcass) and excreta (urine, feces) reflected the two consecutive weeks of instillation except for renal uranium retention for the highest uranium dose. Nephrotoxicity biomarkers, KIM-1, clusterin and osteopontin, are induced from day 4 to day 21 and associated with changes in renal function (arterial fluxes) measured using non-invasive functional imaging (Doppler-ultrasonography) and confirmed by renal histopathological analysis. These results suggest that specific biokinetic models should be developed to consider altered uranium excretion and retention in kidney due to nephrotoxicity. The threshold is between 0.25 and 1 mg/kg/day after repeated exposure to uranium via upper airways.

Sorption properties of carbonized biopolymers of plant origin

Studies of carbon nanomaterials (CNM) synthesized from lignocellulosic biomass, and natural and technical lignins were carried out. For the first time, we suggested using stems of Sosnovsky hogweed, one of the most aggressive and poisonous invasive plant species, to produce CNM. The influence of the choice of raw materials and synthesis conditions on the sorption and surface-porous characteristics of the samples was evaluated. The main regularities of adsorption processes from aqueous media with a low concentration (0.625 μg/ml) of uranium were established. We found that strong retention of uranium characterizes carbonized biopolymers (CBP) samples, a significant amount of which (67–70%) is not desorbed either by water or aqueous solutions of CH3COONH4 and HCI (1 M). In addition, we found out that the carbon nanomaterials we synthesized can adsorb mycotoxin T-2. The obtained results indicated a high innovative potential of CNM.

U Migration during Weathering of Uraniferous Syenite on Tropical Climate: Case of Ngombas in the Southern Cameroon

The lolodorf syenite axis is known for its radiometric indices. In the Ngombas area the migration and retention of uranium in the regolith developed on syenite is studied using a combination of mineralogy and geochemistry in a bid to understand the processes involved in the dissolution and redistribution of uranium in the secondary environment. A trench dug in the area shows three horizons from the bottom to the top. They include the saprolite, B and Ah horizons. Petrographic and XRD investigations of the syenites reveals minerals such as plagioclase, potassic feldspar, amphibole, pyroxene, biotite, quartz, hematite, zircon coupled with uraninite, U-monazite. The regolith developed on the syenite shows relics of plagioclase, amphibole, quartz, hematite, goethite, chlorite, vermiculite, kaolinite. This is associated with U-bearing minerals such as uranothorite, U-monazite, U-zircon, U-florencite and U-rhadophane. The chemical alteration index (CIA), and gain and loss diagrams indicate that the horizons are more weathered from the top to the bottom. The presence of uranium bearing phases such as uranothorite indicates that U-minerals were dissolved, migrated and sorbed on thorite. The occurrences of U-florencite and U-rhabdophane in the weathering blanket indicate that uranyl is stabilized by phosphate minerals. Under oxidizing conditions the stability of hexavalent uranium is favored by the presence of clay minerals and Fe/Mn-oxyhydroxides. Thus, the migration of uranium in Ngombas is sequestrated by clay blended on Fe-oxides through the process of sorption. The U-bearing phases in the regolith that survived weathering include monazite and zircon. The presence of accessories minerals (U-zircon, U-monazite), sorption of uranium by phosphates, by Fe/Mn-oxyhydroxides, and clays minerals play important roles to reduce the U migration in environmental impact of Ngombas region.

Uranium retention in a Callovo-Oxfordian clay rock formation: From laboratory-based models to in natura conditions

For the performance assessment of radioactive waste disposal, it is critical to predict the mobility of radionuclides in the geological barrier that hosts it. A key challenge consists of assessing the transferability of current knowledge on the retention properties deduced from model systems to in natura situations. The case of the redox-sensitive element uranium in the Callovo-Oxfordian clay formation (COx) is presented herein. Extensive experimental work was carried out with respect to parameters affecting uranium speciation (pH, PCO2, [Ca] and redox potential) with illite, COx clay fraction and raw COx claystone. The “bottom-up” approach implemented, with illite and montmorillonite as reactive phases, quantitatively explains the adsorption results of U(VI) and U(IV) on COx. While retention is high for U(IV) (Rd∼104 L kg−1), it remains very low for U(VI) (Rd∼4 L kg−1) due to the formation of soluble ternary Ca(Mg)–U(VI)-carbonate complexes. The applicability of the sorption model was then assessed by comparing predictive analyses with data characterizing the behavior of naturally-occurring U (<3 mg kg−1). The COx clay phase is the largest reservoir of naturally-occurring U (∼65%) but only a small fraction appears to be adsorbed (∼1%). Under representative site conditions (especially with respect to reducing conditions), we have concluded that ternary U(VI) complexes control U speciation in solution while U(IV) surface species dominate U adsorption, with Rd values > 70 L kg−1.

Modeling Uranium Transport in Rough-Walled Fractures with Stress-Dependent Non-Darcy Fluid Flow

The reactive-transportation of radioactive elements in fractured rock mass is critical to the storage of radioactive elements. To describe the reactive-transportation and distribution morphology of a uranium-containing solution, a stress-dependent reactive transport model was developed, and the simulator of FLAC3D-CFD was employed. The uranium transport experiment subjected to the variation of confining stress of 5–19 MPa and hydraulic pressure of 0.5–3.5 MPa was conducted in fractured rock mass. The results show that the uranium-containing solution transport and distribution is significantly dependent on the evolution of the connected channel in rough-walled fracture, which is significantly influenced by the confining stress and hydraulic pressure. In more detail, the increase of confining stress resulted in the anisotropic of seepage channel in aperture, and corresponding turbulence flow and uranium retention were presented at the fracture aperture of 2–5 μm. As the increase of hydraulic pressure, flow regime evolved from the inertial flow to vortex flow, and the transformation region is 16 MPa confining stress and 1.5 MPa hydraulic pressure. The evolution of loading paths also dominates the flow and solute transport, and high seepage speed and strong solute transport were presented at the k = 1 (ratio of vertical stress loading to horizontal stress unloading), and a laminar flow and weak solute transport were presented at k = 0.

Synthesis and thermodynamics of uranium-incorporated α-Fe2O3 nanoparticles

• Uranium-incorporated hematite is thermodynamically metastable. • Increasing uranium incorporation within hematite increases its formation enthalpy. • Hydrothermal treatment can increase uranium concentrations in hematite. • U-Fe 2 O 3 coordination in radioactive waste environments may be process-dependent. Hematite nanoparticles were synthesized with U(VI) in circumneutral water through a coprecipitation and hydrothermal treatment process. XRD, TEM, and EXAFS analyses reveal that uranium may aggregate along grain boundaries and occupy Fe sites within hematite. The described synthesis method produces crystalline, single-phase iron oxide nanoparticles absent of surface-bound uranyl complexes. EXAFS data were comparable to spectra from existing studies whose syntheses were more representative of naturally occurring, extended aging processes. This work provides and validates an accelerated method of synthesizing uranium-immobilized iron oxide nanoparticles for further mechanistic studies. High temperature oxide melt solution calorimetry measurements were performed to calculate the thermodynamic stability of uranium-incorporated iron oxide nanoparticles. Increasing uranium content within hematite resulted in more positive formation enthalpies. Standard formation enthalpies of U x Fe 2–2x O 3 were as high as 76.88 ± 2.83 kJ/mol relative to their binary oxides, or -764.04 ± 3.74 kJ/mol relative to their constituent elements, at x = 0.037. Data on the thermodynamic stability of uranium retention pathways may assist in predicting waste uranyl remobilization, as well as in developing more effective methods to retain uranium captured from aqueous environments.

Hydrolytic degradation of tri-iso-amyl phosphate-dodecane system

A solution of 1.1 M tri-iso-amyl phosphate (TiAP) in n-dodecane (n-DD) has been proposed as a candidate solvent for reprocessing of spent nuclear fuel arising from fast reactors. Significant amounts of radioruthenium are produced as a fission product in fast reactors. To minimize the extraction of radioruthenium during the separation of uranium and plutonium, it was proposed to carry out the solvent extraction process at nitric acid concentration ranging from 4 to 5 M. Under these process conditions, it is quite likely that the solvent phase can undergo hydrolytic degradation, which can cause significant changes in the physicochemical properties of the solvent phase and hamper the recovery of uranium and plutonium. In view of this, the hydrolytic degradation of 1.1 M TiAP/n-DD was studied as a function of nitric acid concentration, duration of degradation and process temperature. The physicochemical properties of the hydrolytically degraded organic phase such as density, viscosity, interfacial tension, phase disengagement time was studied and compared with those obtained for thermally degraded solvent (in the absence of nitric acid) and neat solvent phase. The degree of damage was assessed by the uranium retention test in the hydrolytically degraded solvent phase and the procedure for the removal of degradation products from the organic phase was reported. The results revealed that hydrolytic degradation resulted in the formation of acidic degradation products of both TiAP and n-DD. While most of the acidic degradation products arising from TiAP appears to be washable by sodium carbonate during clean-up, a small amount of hydrocarbon degradation products, e.g. nitrolic acid, sparingly soluble in sodium carbonate seems to retain uranium in organic phase during recovery. The formation of nitration degradation products was confirmed by FT-IR spectroscopy. The recovery of uranium was more that 95% after the clean-up of degraded solvent.

A systematic study of uranium retention in human organs and quantification of radiological and chemical doses from uranium ingestion

The Industrial revolution introduced umpteen radionuclides in the environment and their long-term exposure from ingestion and inhalation is a potential threat to the human race. In numerous developing countries, uranium and other radionuclide concentrations are higher than their recommended limits and cause adverse health effects to inhabitants. The present study depicts the uranium concentration in water samples of Nawanshahr and Rupnagar districts of Punjab (India). The uranium concentration in the studied region ranged from 13.23 μg l−1 to 38.61 μg l−1, and some samples reported to be have higher concentration than their recommended limits. An attempt has been made to quantify the uranium retention in different organs using ICRP’s age-specific biokinetic model with a specific update of urine, faeces, and hairs. The dosimetric models were used to estimate the radiological doses for particular organs and chemical toxicity for overall health risk assessment. Time dependence studies of uranium in distinct organs and tissues claimed that the kidney, liver, non-exchangeable bone volume and soft tissues are the vital target organs for uranium depository.

Evaluation of thermodynamic data for aqueous Ca-U(VI)-CO3 species under conditions characteristic of geological clay formation

Uranium(VI) forms stable Ca-U(VI)-CO3 ternary complexes, which are highly mobile in the environment. This characteristic can be critical as regards radioactive waste disposal in deep geological formations. While the formation of aqueous ternary Ca-U(VI)-CO3 complexes has been clearly established and identified under room temperature conditions, the effect of temperature on their formation has barely been investigated. An experimental study was thus designed to evaluate the stability of these complexes with temperature (20–80 °C) under well-controlled physicochemical conditions typical of clay rock formation (especially CO2 pressure). This method is based on a study of the competition between the processes of complex formation and uranium retention on an anion-exchange resin. A modelling approach with PhreeqC code, using the Davies equation for the calculation of the activity coefficients, was carried out to derive the thermodynamic data for the formation of these complexes. The Van't Hoff Equation can be applied to explain the variation in stability constant values as a function of temperature. This work suggests: log10β113o= 27.27 ± 0.04 and log10β213o= 29.8 ± 0.2 for CaUO2(CO3)32- and Ca2UO2(CO3)3(aq) complexes, respectively, hence in good agreement with the literature data. The enthalpy of reaction determined here from experiments suggests that temperature does not facilitate the formation of CaUO2(CO3)32- (ΔrHmo = −24.4 ± 2.2 kJ mol−1), whereas it has very little effect on the stability of Ca2UO2(CO3)3(aq) (ΔrHmo = −3 ± 10 kJ mol−1).

Understanding the mobility and retention of uranium and its daughter products

Knowledge of the behavior of technologically enhanced naturally occurring radioactive materials derived through the decay of U and its daughter products, and their subsequent fractionation, mobilization and retention, is essential to develop effective mitigation strategies and long-term radiological risk prediction. In the present study, multiple state-of-the-art, spatially resolved micro-analytical characterization techniques were combined to systematically track the liberation and migration of radionuclides (RN) from U-bearing phases in an Olympic Dam Cu flotation concentrate following sulfuric-acid-leach processing. The results highlighted the progressive dissolution of U-bearing minerals (mainly uraninite) leading to the release, disequilibrium and ultimately upgrade of daughter RN from the parent U. This occurred in conjunction with primary Cu-Fe-sulfide minerals undergoing coupled-dissolution reprecipitation to the porous secondary Cu-mineral, covellite. The budget of RN remaining in the leached concentrate was split between RN still hosted in the original U-bearing minerals, and RN that were mobilized and subsequently sorbed/precipitated onto porous covellite and auxiliary gangue mineral phases (e.g. barite). Further grinding of the flotation concentrate prior to sulfuric-acid-leach led to dissolution of U-bearing minerals previously encapsulated within Cu-Fe-sulfide minerals, resulting in increased release and disequilibrium of daughter RN, and causing further RN upgrade. The various processes that affect RN (mobility, sorption, precipitation) and sulfide minerals (coupled-dissolution reprecipitation and associated porosity generation) occur continuously within the hydrometallurgical circuit, and their interplay controls the rapid and highly localized enrichment of RN. The innovative combination of tools developed here reveal the heterogeneous distribution and fractionation of the RN in the ores following hydrometallurgical treatment at nm to cm-scales in exquisite detail. This approach provides an effective blueprint for understanding of the mobility and retention of U and its daughter products in complex anthropogenic and natural processes in the mining and energy industries.

Uranium retention on iron oxyhydroxides in post-mining environmental conditions

Investigating uranium migration mechanisms related to the weathering of waste rocks is essential for developing strategies that can address the potential environmental issues caused by uranium mining.This work is based on environmental samples containing 2 L ferrihydrite, lepidocrocite and goethite collected in the technosols from granitic waste rock piles, mine drainage conduits and mine waters. The results show the important role of iron oxyhydroxide in U immobilization and re-concentration.EXAFS spectroscopy combined with mineralogical and geochemical studies (Scanning electronic microscopy, Wavelength-dispersive X-ray spectroscopy microprobe, inductively coupled plasma - optical emission spectrometry/mass spectrometry and X-ray diffraction) allowed for the identification of uranyl ternary surface complexes at the ferrihydrite surface that were either composed of phosphate groups or organic matter. Moreover, goethite and lepidocrocite were also identified as a secondary trap for U immobilization. U(VI) is known to be mobile in oxidizing conditions. This study highlights the control of the uranyl mobility by various iron oxyhydroxides in supergene conditions.

Uranium and neptunium retention mechanisms in Gallionella ferruginea/ferrihydrite systems for remediation purposes

The ubiquitous β-Proteobacterium Gallionella ferruginea is known as stalk-forming, microaerophilic iron(II) oxidizer, which rapidly produces iron oxyhydroxide precipitates. Uranium and neptunium sorption on the resulting intermixes of G. ferruginea cells, stalks, extracellular exudates, and precipitated iron oxyhydroxides (BIOS) was compared to sorption to abiotically formed iron oxides and oxyhydroxides. The results show a high sorption capacity of BIOS towards radionuclides at circumneutral pH values with an apparent bulk distribution coefficient (Kd) of 1.23 × 104 L kg−1 for uranium and 3.07 × 105 L kg−1 for neptunium. The spectroscopic approach by X-ray absorption spectroscopy (XAS) and ATR FT-IR spectroscopy, which was applied on BIOS samples, showed the formation of inner-sphere complexes. The structural data obtained at the uranium LIII-edge and the neptunium LIII-edge indicate the formation of bidentate edge-sharing surface complexes, which are known as the main sorption species on abiotic ferrihydrite. Since the rate of iron precipitation in G. ferruginea-dominated systems is 60 times faster than in abiotic systems, more ferrihydrite will be available for immobilization processes of heavy metals and radionuclides in contaminated environments and even in the far-field of high-level nuclear waste repositories.

Measurement of uranium distribution coefficient and 235U/238U ratio in soils affected by Fukushima dai-ichi nuclear power plant accident

Fukushima Daiichi Nuclear Power Plant (FDNPP) accident resulted radioactive contamination in soil due to deposition of mainly radiocesium as well as many long-lived radionuclides surrounding a large area around FDNPP. Depending upon environmental conditions, radionuclides in soil can be mobilized in aquatic systems. Therefore, the fate and transfer of these radionuclides in the soil water system is very important for radiation protection and dose assessment. In the present study, soil and water samples were collected from contaminated areas around FDNPP. Inductively coupled plasma mass spectrometry (ICP-MS) is used for total uranium concentration. Emphasis has been given on isotope ratio measurement of 235U/238U ratio using thermal ionization mass spectrometry (TIMS) that gives us the idea about its contamination during accident. For the migration behavior, its distribution coefficient (Kd) has been determined using laboratory batch method. Chemical characterization of soil with respect to different parameters has been carried out. The effect of these soil parameters on distribution coefficient of uranium has been studied in order to explain the radionuclide mobility in this particular area. The distribution coefficient values for uranium are found to vary from 30 to 36000 L/kg. A large variation in the distribution coefficient values shows the retention or mobility of uranium is highly dependent on soil characteristics in the particular area. This variation is explained with respect to soil pH, Fe, Mn, CaCO3 and organic content. There is a very good correlation of uranium Kd obtained with Fe content. There is no enrichment of 235U has been noticed in the studied area.

Retention of uranium in cement systems: effects of cement degradation and complexing ligands

Retention of uranium in cement systems: effects of cement degradation and complexing ligands

Uranium Retention in a Bioreduced Region of an Alluvial Aquifer Induced by the Influx of Dissolved Oxygen.

Reduced zones in the subsurface represent biogeochemically active hotspots enriched in buried organic matter and reduced metals. Within a shallow alluvial aquifer located near Rifle, CO, reduced zones control the fate and transport of uranium (U). Though an influx of dissolved oxygen (DO) would be expected to mobilize U, we report U immobilization. Groundwater U concentrations decreased following delivery of DO (21.6 mg O2/well/h). After 23 days of DO delivery, injection of oxygenated groundwater was paused and resulted in the rebound of groundwater U concentrations to preinjection levels. When DO delivery resumed (day 51), groundwater U concentrations again decreased. The injection was halted on day 82 again and resulted in a rebound of groundwater U concentrations. DO delivery rate was increased to 54 mg O2/well/h (day 95) whereby groundwater U concentrations increased. Planktonic cell abundance remained stable throughout the experiment, but virus-to-microbial cell ratio increased 1.8-3.4-fold with initial DO delivery, indicative of microbial activity in response to DO injection. Together, these results indicate that the redox-buffering capacity of reduced sediments can prevent U mobilization, but could be overcome as delivery rate or oxidant concentration increases, mobilizing U.