Geotechnical behavior of uranium mill tailings from Saskatchewan,Canada

This paper investigates the geotechnical behavior of uranium mill tailings from Saskatchewan, Canada.The 4% tailings were well-graded with 29% fines whereas the 5% and 6% tailings were gap-graded with 49% fines. All samples exhibited a negligible strength(0.4 k Pa) up to 60% solids, followed by a rapid increase. The 4% tailings exhibited a lower rate and amount of settlement than 5% and 6% tailings. The kidecreased from 10^(-2)to 10^(-4)m/s with a decrease in eifrom 16 to 4 and a decrease in ef from 8 to 4 such that 4% tailings showed one order of magnitude lower values than the 5% and 6%tailings. The settling potential decreased ten times(50%–5%) for 4% tailings and four times(60%–15%)for 5% and 6% tailings. The effective stress increased from 80 to 260 Pa in the settling tests. The 4%tailings were less prone to segregation when compared with 5% and 6% tailings. The average solids content after settling was 35% for 4% tailings, 40% for 5% tailings and 39% for 6% tailings with a solids content deviation of ±3%, ±8%, ±6%, respectively. All materials were essentially non-segregating at 40%initial solids.

Pyrite Oxidation in Leaching Process ofRadionuclides and Heavy Metals fromUranium Mill Tailings

Pyrite is a sensitive mineral in the geological environment, and its oxidation produces an important geochemical and environmental effect on the control of the redox and pH conditions. Column experiment results were used for modeling the geochemical processes in uranium mill tailings under leaching conditions. Oxidation of pyrite dominates the control of the tailings leaching process. The experimental and modeling results show that the leachate chemistry changes substantially with the decrease in pyrite consumption. In the initial stage of the leaching experiment, the pyrite is consumed several hundred times greater than that in the later stages, for much more oxygen is present in the tailings in the initial stage. As the experiment continues, the tailings is gradually saturated with water and the oxygen concentration greatly decreases and so does pyrite consumption. The experimental and modeling results are useful for the design of mill tailing decommissioning: oxidation process and transport of radioactive nuclides and heavy metals can be constrained by controlling the oxygen concentration of tailings and the infiltration of meteoric water.

Efficient and rapid capture of uranium(Ⅵ) in wastewater via multiamine modified β-cyclodextrin porous polymer

It is quite important to ensure the safety and sustainable development of nuclear energy for the treatment of radioactive wastewater. To treat radioactive wastewater efficiently and rapidly, two multi-amine β-cyclodextrin polymers(diethylenetriamine β-cyclodextrin polymer(DETA-TFCDP) and triethylenetetramine β-cyclodextrin polymer(TETA-TFCDP)) were prepared and applied to capture uranium. Results exhibited that DETA-TFCDP and TETA-TFCDP displayed the advantages of high adsorption amounts(612.2and 628.2 mg·g-1, respectively) and rapid adsorption rates, which can reach(88 ± 1)% of their equilibrium adsorption amounts in 10 min. Moreover, the adsorbent processes of DETA-TFCDP and TETATFCDP on uranium(Ⅵ) followed the Langmuir model and pseudo-second-order model, stating they were mainly chemisorption and self-endothermic. Besides, TETA-TFCDP also showed excellent selectivity in the presence of seven competing cations and could be effectively reused five times via Na2CO3as the desorption reagent. Meanwhile, X-ray photoelectron spectroscopy and Fourier transform infrared spectroscopy illustrated that the enriched multi-amine groups and oxygen-containing functional groups on the surface of TETA-TFCDP were the main active sites for capturing uranium(Ⅵ). Hence, multi-amine β-cyclodextrin polymers are a highly efficient, rapid, and promising adsorbent for capturing uranium(Ⅵ)from radioactive wastewater.

Apatite Fission Track Thermochronology of Granite from the Xiazhuang Uranium Ore Field,South China:Implications for Exhumation History and Ore Preservation

Xiazhuang uranium ore field,located in the southern part of the Nanling Metallogenic Belt,is considered one of the largest granite-related U regions in South China.In this paper,we contribute new apatite fission track data and thermal history modeling to constrain the exhumation history and evaluate preservation potential of the Xiazhuang Uranium ore field.Nine Triassic outcrop granite samples collected from different locations of Xiazhuang Uranium ore field yield AFT ages ranging from 43 to 24 Ma with similar mean confined fission track lengths ranging from 11.8±2.0 to 12.9±1.9μm and Dpar values between 1.01 and 1.51μm.The robustness time-temperature reconstructions of samples from the hanging wall of Huangpi fault show that the Xiazhuang Uranium ore field experienced a time of monotonous and slow cooling starting from middle Paleocene to middle Miocene(~60-10 Ma),followed by relatively rapid exhumation in the late Miocene(~10-5 Ma)and nearly thermal stability in the Pliocene-Quaternary(~5-0 Ma).The amount of exhumation after U mineralization since the Middle Paleogene was estimated as~4.3±1.8 km according to the integrated thermal history model.Previous studies indicate that the ore-forming ages of U deposits in the Xiazhuang ore field are mainly before Middle Paleocene and the mineralization depths are more than 4.4±1.2 km.Therefore,the exhumation history since middle Paleocene plays important roles in the preservation of the Xiazhuang Uranium ore field.

Efficient extraction of uranium(VI)from aqueous solution by Zr/Ce-UiO-66-NH_(2) modified by dual strategies of bimetallization and amination

We modified Zr/Ce-UiO-66-NH_(2) using dual bimetallization and amination strategies to efficiently extract uranium from water resources.XRD,FTIR,and XPS indicated the successful alteration of material amination.Moreover,the metal Zr was partially replaced by Ce in Zr-oxygen atom clusters in Zr/Ce-UiO-66-NH_(2).It possessed commendable structural stability in acidic and alkaline solutions.Irrespective of whether it was submerged in a 6 M strong acid or in a 0.5M strong base solution,the structural integrity of Zr/Ce-UiO-66-NH_(2) remained unaffected.Batch experiments at pH=6.0 revealed that uranium adsorption by Zr/Ce-UiO-66-NH_(2) reached 376.8 mg g^(−1) and 611.33 mg g^(−1) at 298 K and 328 K,respectively.These values are much better than those obtained using bimetallic-modified Zr/Ce-UiO-66 or amine-functionalized UiO-66-NH_(2).After five consecutive sorption and desorption cycles,the material retained a uranium removal rate of more than 80%,proving its excellent regenerative properties.Kinetic modeling of U(VI)adsorption on Zr/Ce-UiO-66-NH_(2) implied that chemisorption dominated the rapid uranium sorption rate.We propose potential adsorption mechanisms involving three interactions:inner-sphere surface complexation,chemisorption,and electrostatic interactions.This study shows that the dual strategies of bimetallization and amination can effectively enhance U(VI)extraction from water.This approach has potential applications for the structural design of uranium adsorbents.

High-performance ZIF-8 membranes:preparation and their uranium adsorption performance

In this study,the ZIF-8 membrane(ZIF-8/PP-g-MAH)is prepared by in situ synthesis of ZIF-8 on irradiation-pretreated polymer substrates to improve the uranium adsorption performance and address the recycling problems of ZIF-8 powder.The effects of pH,contact time,and uranium concentration on the adsorption of ZIF-8/PP-g-MAH were investigated.Adsorption isotherm and kinetics analysis show that ZIF-8/PP-g-MAH has a high adsorption capacity of 478.5 mg/g,which is 1.26 times higher than that of ZIF-8,and a rapid adsorption equilibrium of 120 min,which is shortened to one-third of that required for ZIF-8(360 min).The adsorption process of ZIF-8/PP-g-MAH is consistent with that of the Langmuir isotherm and pseudo-second-order dynamic model.ZIF-8/PP-g-MAH also exhibits good selectivity for uranium in simulated seawater.The high adsorption performance of ZIF-8/PP-g-MAH is attributed to its membrane structure,which improves the utilization of coordination sites,including Zn-OH,C-N,and C=N.This study provides an efficient adsorption material for rapid uranium extraction,thus promoting the development of uranium extraction technologies.

Estimating Radon Flux and Environmental Radiation Dose from Decommisioning Uranium Mill Tailings and Mining Debris

Based on a case study on uranium mine No.765 of China National Nuclear Corporation (CNNC), the paper briefly describes disposal program and effect of decommissioning uranium mine/mill facilities and quantitatively evaluates radon fluxes and doses to man of gaseous airborne pathway from mill tailings and mining debris before and after decommissioning, including annual individual effective dose to critical groups and annual collective effective dose to the population within 80 km region of the facilities.

Efficient and selective extraction of uranium from seawater based on a novel pulsed liquid chromatography radionuclide separation method

The novel pulsed liquid chromatography radionuclide separation method presented here provides a new and promising strategy for the extraction of uranium from seawater.In this study,a new chromatographic separation method was proposed,and a pulsed nuclide automated separation device was developed,alongside a new chromatographic column.The length of this chromatographic column was 10 m,with an internal warp of 3 mm and a packing size of 1 mm,while the total separation units of the column reached 12,250.The most favorable conditions for the separation of nuclides were then obtained through optimizing the separation conditions of the device:Sample pH in the column=2,sample injection flow rate=5.698 mL/min,chromatographic column heating temperature=60℃.Separation experiments were also carried out for uranium,europium,and sodium ions in mixed solutions;uranium and sodium ions in water samples from the Ganjiang River;and uranium,sodium,and magnesium ions from seawater samples.The separation factors between the different nuclei were then calculated based on the experimental data,and a formula for the separation level was derived.The experimental results showed that the separation factor in the mixed solution of uranium and europium(1:1)was 1.088,while achieving the initial separation of uranium and europium theoretically required a 47-stage separation.Considering the separation factor of 1.50for the uranium and sodium ions in water samples from the Ganjiang River,achieving the initial separation of uranium and sodium ions would have theoretically required at least a 21-stage separation.Furthermore,for the seawater sample separation experiments,the separation factor of uranium and sodium ions was 1.2885;therefore,more than 28 stages of sample separation would be required to achieve uranium extraction from seawater.The novel pulsed liquid chromatography method proposed in this study was innovative in terms of uranium separation and enrichment,while expanding the possibilities of extracting uranium from seawater through chromatography.

Depleted uranium oxide supported nickel catalyst for autothermal CO_(2)methanation in non-adiabatic reactor under induction heating

Undoped nickel-based catalysts supported on depleted uranium oxide allow one to carry out CO_(2)methanation process under extremely low reaction temperature under atmospheric pressure and powered by a contactless induction heating.By adjusting the reaction conditions,the catalyst is able to perform CO_(2)methanation reaction under autothermal process operated inside a non-adiabatic reactor,without any external energy supply.Such autothermal process is possible thanks to the high apparent density of the UO_x which allows one to confine the reaction heat in a small catalyst volume in order to confine the exothermicity of the reaction inside the catalyst and to operate the reaction at equilibrium heat in-heat out.Such autothermal operation mode allows one to significantly reduce the complexity of the process compared to that operated using adiabatic reactor,where complete insulation is required to prevent heat disequilibrium,in order to reduce as much as possible,the heat exchange with the external medium.The catalyst displays an extremely high stability as a function of time on stream as no apparent deactivation.It is expected that such new catalyst with unprecedented catalytic performance could open new era in the field of heterogeneous catalysis where traditional supports show their limitations to operate catalytic processes under severe reaction conditions.

Branched fibrous amidoxime adsorbent with ultrafast adsorption rate and high amidoxime utilization for uranium extraction from seawater

Direct collection of uranium from low uranium systems via adsorption remains challenging.Fibrous sorbent materials with amidoxime(AO)groups are promising adsorbents for uranium extraction from seawater.However,low AO adsorption group utilization remains an issue.We herein fabricated a branched structure containing AO groups on polypropylene/polyethylene spun-laced nonwoven(PP/PE SNW)fibers using grafting polymerization induced by radiation(RIGP)to improve AO utilization.The chemical structures,thermal properties,and surface morphologies of the raw and treated PP/PE SNW fibers were studied.The results show that an adsorptive functional layer with a branching structure was successfully anchored to the fiber surface.The adsorption properties were investigated using batch adsorption experiments in simulated seawater with an initial uranium concentration of 500μg·L^(−1)(pH 4,25℃).The maximum adsorption capacity of the adsorbent material was 137.3 mg·g^(−1)within 24 h;moreover,the uranyl removal reached 96%within 240 min.The adsorbent had an AO utilization rate of 1/3.5 and was stable over a pH range of 4–10,with good selectivity and reusability,demonstrating its potential for seawater uranium extraction.

Application of sequential extraction for analyzing source and sink of uranium in Huanghe River sediments,China

Geochemical behaviors of heavy metals are closely related to their chemical state that can be divided by sequential extraction into exchangeable(F1),bound to carbonates(F2),bound to Fe-Mn oxides(F3),bound to organic matter or sulfide(F4),and residual(F5).Uranium in sediment of the Huanghe(Yellow)River,China,in different chemical states was extracted using the five-step procedure of Tessier and the source and sink were analyzed.Results show that more than 70%of the total uranium was immobile residual F5 in abundance,followed in order of F4>F3>F2>F1,indicating that the main source of uranium in the sediments was from weathered rock in the drainage basin.In addition,the uranium in the sediments presents potential exogenous input in the Lanzhou,Baotou,and Tongguan reach.Fe-Mn oxides are main carriers of unstable uranium,especially those of F1 and F3.Calcite and illite are secondary adsorption minerals of unstable uranium in sediments under natural conditions.Human activities can also produce an obvious impact on uranium speciation.This study provides a reference for the application of sequential extraction in analyzing the source and sink of uranium in river sediments.

Site selective 5f electronic correlations inβ-uranium

We investigate the electronic structure ofβ-uranium,which has five nonequivalent atomic sites in its unit cell,by means of the density functional theory plus Hubbard-U correction with U from linear response calculation.It is found that the 5f electronic correlations inβ-uranium are moderate.More interestingly,their strengths are site selective,depending on the local atomic environment of the present uranium atom.As a consequence,the occupation matrices and partial 5f density of states ofβ-uranium manifest site dependence.In addition,the complicate experimental structure ofβ-uranium could be well reproduced within this theoretical framework.

Effect of Natural Zeolite on Pore Structure of Cemented Uranium Tailings Backfill

The use of some environmental functional minerals as backfill-modified materials may improve the leaching resistance of cemented uranium tailings backfill created from alkali-activated slag(CUTB),but these materials may participate in the hydration reaction of the cementitious materials,which could have a certain impact on the pore structure of the CUTB,thus affecting its mechanical properties and leaching resistance.In this paper,natural zeolite is selected as the backfill-modified material,and it is added to alkali-activated slag paste(AASP)and CUTB in cementitious material proportions of 4%,8%,12%,and 16%to prepare AASP mixtures and CUTB mixtures containing environmental functional minerals.After the addition of natural zeolite,the porosity of the CUTB generally increases,but when the content is 4%,the porosity decreases to 22.30%.The uniaxial compressive strength(UCS)of the CUTB generally decreases,but the decrease is the smallest when the content is 4%,and the UCS is 12.37 MPa.The addition of natural zeolite mainly reduces the number of fine pores in the CUTB,but the pores with relaxation times T_(2)of greater than 10 ms account for about 10%of the total pores,and there are a certain number of large pores in the CUTB.The main product of alkali-activated slag is calcium(alumino)silicate hydrate(C-(A)-S-H gel).When natural zeolite is added,the hydration products develop towards denser products with a high degree of polymerization and the formation of low polymerization products is reduced.This affects the internal fracture pores of the hydration products and the interface pores of the CUTB,has an irregular effect on the pore characteristics of the CUTB,and influences the UCS.

Permeability evolution mechanism and the optimum permeability determination of uranium leaching from low-permeability sandstone treated with low-frequency vibration

Low-frequency vibrations can effectively improve natural sandstone permeability,and higher vibration frequency is associated with larger permeability.However,the optimum permeability and permeability evolution mechanism for uranium leaching and the relationship between permeability and the change of chemical reactive rate affecting uranium leaching have not been determined.To solve the above problems,in this study,identical homogeneous sandstone samples were selected to simulate lowpermeability sandstone;a permeability evolution model considering the combined action of vibration stress,pore water pressure,water flow impact force,and chemical erosion was established;and vibration leaching experiments were performed to test the model accuracy.Both the permeability and chemical reactions were found to simultaneously restrict U6þleaching,and the vibration treatment increased the permeability,causing the U6þleaching reaction to no longer be diffusion-constrained but to be primarily controlled by the reaction rate.Changes of the model calculation parameters were further analyzed to determine the permeability evolution mechanism under the influence of vibration and chemical erosion,to prove the correctness of the mechanism according to the experimental results,and to develop a new method for determining the optimum permeability in uranium leaching.The uranium leaching was found to primarily follow a process consisting of(1)a permeability control stage,(2)achieving the optimum permeability,(3)a chemical reactive rate control stage,and(4)a channel flow stage.The resolution of these problems is of great significance for facilitating the application and promotion of lowfrequency vibration in the CO_(2)+O_(2) leaching process.

An artificial neural network potential for uranium metal at low pressures

Based on machine learning,the high-dimensional fitting of potential energy surfaces under the framework of first principles provides density-functional accuracy of atomic interaction potential for high-precision and large-scale simulation of alloy materials.In this paper,we obtained the high-dimensional neural network(NN)potential function of uranium metal by training a large amount of first-principles calculated data.The lattice constants of uranium metal with different crystal structures,the elastic constants,and the anisotropy of lattice expansion of alpha-uranium obtained based on this potential function are highly consistent with first-principles calculation or experimental data.In addition,the calculated formation energy of vacancies in alpha-and beta-uranium also matches the first-principles calculation.The calculated site of the most stable self-interstitial and its formation energy is in good agreement with the findings from density functional theory(DFT)calculations.These results show that our potential function can be used for further large-scale molecular dynamics simulation studies of uranium metal at low pressures,and provides the basis for further construction of potential model suitable for a wide range of pressures.

Assessment of the Greenhouse Gas Footprint and Environmental Impact of CO_(2)and O_(2)in situ Uranium Leaching

Under the new development philosophy of carbon peaking and carbon neutrality,CO_(2)and O_(2)in situ leaching(ISL)has been identified as a promising technique for uranium mining in China,not only because it solves carbon dioxide utilization and sequestration,but it also alleviates the environmental burden.However,significant challenges exist in assessment of CO_(2)footprint and water-rock interactions,due to complex geochemical processes.Herein this study conducts a three-dimensional,multicomponent reactive transport model(RTM)of a field-scale CO_(2)and O_(2)ISL process at a typical sandstone-hosted uranium deposit in Songliao Basin,China.Numerical simulations are performed to provide new insight into quantitative interpretation of the greenhouse gas(CO_(2))footprint and environmental impact(SO_(4)^(2–))of the CO_(2)and O_(2)ISL,considering the potential chemical reaction network for uranium recovery at the field scale.RTM results demonstrate that the fate of the CO_(2)could be summarized as injected CO_(2)dissolution,dissolved CO_(2)mineralization and storage of CO_(2)as a gas phase during the CO_(2)and O_(2)ISL process.Furthermore,compared to acid ISL,CO_(2)and O_(2)ISL has a potentially smaller environmental footprint,with 20%of SO_(4)^(2–)concentration in the aquifer.The findings improve our fundamental understanding of carbon utilization in a long-term CO_(2)and O_(2)ISL system and provide important environmental implications when considering complex geochemical processes.

Assessment of Modeling Collimator Designs for Gamma-Ray Transmission of Uranium Oxide Spectrometry Using HPGe Detectors

Many scientific domains use gamma-ray spectrometry, but non-destructive gamma scanning and gamma emission tomography of radioactive fuel in particular. In the experimental setting, a collimator is frequently employed to focus on a particular location of interest in the fuel. Predictive models for the transmitted gamma-ray intensity through the collimator are required for both the optimization of instrument design and the planning of measurement campaigns. Gamma-ray transport accuracy is frequently predicted using Monte Carlo radiation transport methods, but using these tools in low-efficiency experimental setups is challenging due to the lengthy computation times needed. This study focused on the full-energy peak intensity that was transmitted through several collimator designs, including rectangle and cylinder. The rate of photons arriving at a detector on the other side of the collimator was calculated for anisotropic source of SNM (U3O8). Some geometrical assumptions that depended on the source-to-collimator distance and collimator dimensions (length, radius or length, height, and width) were applied to achieve precise findings.

Benchmark experiment on slab^(238)U with D-T neutrons for validation of evaluated nuclear data

A benchmark experiment on^(238)U slab samples was conducted using a deuterium-tritium neutron source at the China Institute of Atomic Energy.The leakage neutron spectra within energy levels of 0.8-16 MeV at 60°and 120°were measured using the time-of-flight method.The samples were prepared as rectangular slabs with a 30 cm square base and thicknesses of 3,6,and 9 cm.The leakage neutron spectra were also calculated using the MCNP-4C program based on the latest evaluated files of^(238)U evaluated neutron data from CENDL-3.2,ENDF/B-Ⅷ.0,JENDL-5.0,and JEFF-3.3.Based on the comparison,the deficiencies and improvements in^(238)U evaluated nuclear data were analyzed.The results showed the following.(1)The calculated results for CENDL-3.2 significantly overestimated the measurements in the energy interval of elastic scattering at 60°and 120°.(2)The calculated results of CENDL-3.2 overestimated the measurements in the energy interval of inelastic scattering at 120°.(3)The calculated results for CENDL-3.2 significantly overestimated the measurements in the 3-8.5 MeV energy interval at 60°and 120°.(4)The calculated results with JENDL-5.0 were generally consistent with the measurement results.

Efficient removal of U(VI) from wastewater by a sponge-like 3D porous architecture with hybrid electrospun nanofibers

Removal of uranium(VI)from nuclear wastewater is urgent due to the global nuclear energy exploitation.This study synthesized novel sponge-like 3D porous materials for enhanced uranium adsorption by combining electrospinning and fibrous freeze-shaping techniques.The materials possessed an organic-inorganic hybrid architecture based on the electrospun fibers of polyacrylonitrile(PAN)and SiO_(2).As a sup-porting material,the surface of fibrous SiO_(2) could be further functionalized by cyano groups via(3-cyanopropyl)triethoxysilane.All the cyano groups were turned into amidoxime(AO)groups to obtain a amidoxime-functionalized sponge(PAO/SiO_(2)-AO)through the subsequent ami-doximation process.The proposed sponge exhibited enhanced uranium adsorption performance with a high removal capacity of 367.12 mg/g,a large adsorption coefficient of 4.0×10^(4)mL/g,and a high removal efficiency of 97.59%.The UO_(2)^(2+)adsorption kinetics perfectly conformed to the pseudo-second-order reaction.The sorbent also exhibited an excellent selectivity for UO_(2)^(2+) with other interfering metal ions.2023 Hohai University.Production and hosting by Elsevier B.V.

Nondestructive and active interrogation system for special nuclear material:proof of principle and initial results

Herein,we employ the threshold energy neutron analysis(TENA)technique to introduce the world's first active interrogation system to detect special nuclear materials(SNMs),including U-235 and Pu-239.The system utilizes a DD neutron generator based on inertial electrostatic confinement(IEC)to interrogate suspicious objects.To detect secondary neutrons produced during fission reactions induced in SNMs,a tensioned metastable fluid detector(TMFD)is employed.The current status of the system's development is reported in this paper,accompanied by the results from experiments conducted to detect 10 g of highly enriched uranium(HEU).Notably,the experimental findings demonstrate a distinct difference in the count rates of measurements with and without HEU.This difference in count rates surpasses two times the standard deviation,indicating a confidence level of more than 96% for identifying the presence of HEU.The paper presents and extensively discusses the proof-of-principle experimental results,along with the system's planned trajectory.