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All sourcesNASA NTRSDOE OSTI
DOE OSTI2015

Laboratory Enrichment of Radioactive Assemblages and Estimation of Thorium and Uranium Radioactivity in Fractions Separated from Placer Sands in Southeast Bangladesh

The present study reports the likely first attempt of separating radioactive minerals for estimation of activity concentration in the beach placer sands of Bangladesh. Several sand samples from heavy mineral deposits located at the south-eastern coastal belt of Bangladesh were processed to physically upgrade their radioactivity concentrations using plant and laboratory equipment. Following some modified flow procedure, individual fractions were separated and investigated using gamma-ray spectrometry and powder-XRD analysis. The radioactivity measurements indicated contributions of the thorium and uranium radioactive series and of {sup 40}K. The maximum values of {sup 232}Th and {sup 238}U, estimated from the radioactivity of {sup 208}Tl and {sup 234}Th in secular equilibrium, were found to be 152,000 and 63,300 Bq/kg, respectively. The fraction of the moderately conductive part in electric separation contained thorium predominantly, while that of the non-conductive part was found to be uranium rich. The present arrangement of the pilot plant cascade and the fine tuning of setting parameters were found to be effective and economic separation process of the radioactive minerals from placer sands in Bangladesh. Probable radiological impacts and extraction potentiality of such radioactive materials are also discussed.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2017

Monte Carlo modeling of recrystallization processes in α-uranium

In this study, starting with electron backscattered diffraction (EBSD) data obtained from a warm clock-rolled α-uranium deformation microstructure, a Potts Monte Carlo model was used to simulate static site-saturated recrystallization while testing a number of different conditions for the assignment of recrystallized nuclei within the microstructure. The simulations support observations that recrystallized nuclei within α-uranium form preferentially on non-twin high-angle grain boundary sites at 450 °C, and demonstrate that the most likely nucleation sites on these boundaries can be identified by the surrounding degree of Kernel Average Misorientation (KAM), which may be considered as a proxy for the local geometrically necessary dislocation (GND) density.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Determining local thermal transport in a composite uranium-nitride/silicide nuclear fuel using square-pulse transient thermoreflectance technique

Laser-based techniques have become an appealing option for determining the thermal diffusivities (D) and conductivities (k) of nuclear materials that would otherwise prove too hazardous or difficult to measure otherwise. These techniques have enabled non-destructive and non-contact thermal transport measurements with micron-level spatial resolution. In this study, a new time-domain technique known as square-wave pulse thermoreflectance (SPTR) is described and used to determine D values of both uranium sesquisilicide (U 3 Si 2 ) and uranium nitride (UN) phases in a composite fuel. An extensive sensitivity analysis was conducted that identified the optimal measurement parameters of standard materials with a range of thermal transport properties comparable to those of various fuel types. The standards were measured using both SPTR as well as a spatial-domain thermoreflectance technique (SDTR). Several U 3 Si 2 and UN phase regions of polished UN/U 3 Si 2 (70/30 vol.%) samples were measured using both methods, and the resulting calculated D and k values are reported, with both techniques showing excellent agreement between samples. Finally, the ability to use the technique for local diffusivity mapping was demonstrated over a multiphase region, and could be used to determine thermal transport properties in precipitates, secondary phases, and irradiation-damaged regions of post-irradiated fuel samples.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2015

Comparative XRPD and XAS study of the impact of the synthesis process on the electronic and structural environments of uranium–americium mixed oxides

Uranium–americium mixed oxides are potential compounds to reduce americium inventory in nuclear waste via a partitioning and transmutation strategy. A thorough assessment of the oxygen-to-metal ratio is paramount in such materials as it determines the important underlying electronic structure and phase relations, affecting both thermal conductivity of the material and its interaction with the cladding and coolant. In 2011, various XAS experiments on U{sub 1−x}Am{sub x}O{sub 2±δ} samples prepared by different synthesis methods have reported contradictory results on the charge distribution of U and Am. This work alleviates this discrepancy. The XAS results confirm that, independently of the synthesis process, the reductive sintering of U{sub 1−x}Am{sub x}O{sub 2±δ} leads to the formation of similar fluorite solid solution indicating the presence of Am{sup +III} and U{sup +V} in equimolar proportions. - Graphical abstract: Formation of (U{sup IV/V},Am{sup III})O{sup 2} solid solution by sol–gel and by powder metallurgy. - Highlights: • Uranium–americium mixed oxides were synthesized by sol–gel and powder metallurgy. • Fluorite solid solutions with similar local environment have been obtained. • U{sup V} and Am{sup III} are formed in equimolar proportions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2014

Uranium Bioreduction Rates across Scales: Biogeochemical Hot Moments and Hot Spots during a Biostimulation Experiment at Rifle, Colorado

We aim to understand the scale-dependent evolution of uranium bioreduction during a field experiment at a former uranium mill site near Rifle, Colorado. Acetate was injected to stimulate Fe-reducing bacteria (FeRB) and to immobilize aqueous U(VI) to insoluble U(IV). Bicarbonate was coinjected in half of the domain to mobilize sorbed U(VI). We used reactive transport modeling to integrate hydraulic and geochemical data and to quantify rates at the grid block (0.25 m) and experimental field scale (tens of meters). Although local rates varied by orders of magnitude in conjunction with biostimulation fronts propagating downstream, field-scale rates were dominated by those orders of magnitude higher rates at a few selected hot spots where Fe(III), U(VI), and FeRB were at their maxima in the vicinity of the injection wells. At particular locations, the hot moments with maximum rates negatively corresponded to their distance from the injection wells. Although bicarbonate injection enhanced local rates near the injection wells by a maximum of 39.4%, its effect at the field scale was limited to a maximum of 10.0%. We propose a rate-versus-measurement-length relationship (log R' = -0.63

FEED MATERIALS PLANTS↗
DOE OSTI2014

Mathematical simulation of the amplification of 1790-nm laser radiation in a nuclear-excited He – Ar plasma containing nanoclusters of uranium compounds

The possibility of applying dusty active media in nuclearpumped lasers has been considered. The amplification of 1790-nm radiation in a nuclear-excited dusty He – Ar plasma is studied by mathematical simulation. The influence of nanoclusters on the component composition of the medium and the kinetics of the processes occurring in it is analysed using a specially developed kinetic model, including 72 components and more than 400 reactions. An analysis of the results indicates that amplification can in principle be implemented in an active laser He – Ar medium containing 10-nm nanoclusters of metallic uranium and uranium dioxide. (lasers)

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2017

Crystallographic texture of straight-rolled ?-uranium foils via neutron and X-ray diffraction

The texture of recrystallized straight-rolled ?-uranium foils, a component in prospective irradiation target designs for medical isotope production, has been measured by neutron diffraction, as well as X-ray diffraction using both Cu and Mo sources. Variations in the penetration depth of neutron and X-ray radiation allow for determination of both the bulk and surface textures. The bulk ?-uranium foil texture is similar to the warm straight-rolled plate texture, with the addition of a notable splitting of the (001) poles along the transverse direction. The surface texture of the foils is similar to the bulk, with an additional (001) texture component that is oriented between the rolling and normal directions. Differences between the surface and bulk textures are expected to arise from shear forces during the rolling process and the influence that distinct strain histories have on subsequent texture evolution during recrystallization.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Utilization of non-weapons-grade plutonium and highly enriched uranium with breeding of the {sup 233}U isotope in the VVER reactors using thorium and heavy water

A method for joint utilization of non-weapons-grade plutonium and highly enriched uranium in the thorium–uranium—plutonium oxide fuel of a water-moderated reactor with a varying water composition (D{sub 2}O, H{sub 2}O) is proposed. The method is characterized by efficient breeding of the {sup 233}U isotope and safe reactor operation and is comparatively simple to implement.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗
DOE OSTI2017

Fission barriers and other characteristics of nuclei from the uranium region

Fission barriers in nuclei belonging to the uranium region and their other characteristics are calculated on the basis of the FaNDF{sup 0} energy density functional. In particular, the neutron-separation energies S{sub n} and S{sub 2n}, the proton-separation energies S{sub p}, and the beta-transition energiesQ{sub β} are calculated for uranium, neptunium, and plutonium isotopes. In addition, the deformation energies and parameters of these nuclei are presented along with their radii. A comparison with the predictions of the Skyrme–Hartree–Fock method implemented with several versions of the Skyrme energy density functionals is performed. The role of the octupole deformation β{sub 3} is studied for the {sup 238}U nucleus. It is shown that this deformation does not have any significant effect on the first-barrier height B{sup (1)}{sub f} or ground-state properties. At the same time, the second-barrier height B(2) f decreases by a factor of about two upon taking into account β{sub 3}. A phase transition at A ~ 260 is found for the three isotopic chains being considered: this point is a bifurcation point at which B{sup (1)}{sub f} (A) forks into two curves. Of these, the curve B{sup (2)}{sub f} (A) splits from it, prolonging the former curve for B{sup (1)}{sub f} (A) almost continuously, whereas the curve for B{sup (1)}{sub f} (A) itself goes down sharply.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2017

Natural Transmutation of Actinides via the Fission Reaction in the Closed Thorium–Uranium–Plutonium Fuel Cycle

It is shown for a closed thorium–uranium–plutonium fuel cycle that, upon processing of one metric ton of irradiated fuel after each four-year campaign, the radioactive wastes contain ~54 kg of fission products, ~0.8 kg of thorium, ~0.10 kg of uranium isotopes, ~0.005 kg of plutonium isotopes, ~0.002 kg of neptunium, and “trace” amounts of americium and curium isotopes. This qualitatively simplifies the handling of high-level wastes in nuclear power engineering.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2014

An Overview of Process Monitoring Related to the Production of Uranium Ore Concentrate

Uranium ore concentrate (UOC) in various chemical forms, is a high-value commodity in the commercial nuclear market, is a potential target for illicit acquisition, by both State and non-State actors. With the global expansion of uranium production capacity, control of UOC is emerging as a potentially weak link in the nuclear supply chain. Its protection, control and management thus pose a key challenge for the international community, including States, regulatory authorities and industry. This report evaluates current process monitoring practice and makes recommendations for utilization of existing or new techniques for managing the inventory and tracking this material.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2015

Research and Development of Multiphysics Models in Support of the Conversion of the High Flux Isotope Reactor to Low Enriched Uranium Fuel

The findings presented in this report are results of a five year effort led by the RRD Division of the ORNL, which is focused on research and development toward the conversion of the High Flux Isotope Reactor (HFIR) fuel from high-enriched uranium (HEU) to low-enriched uranium (LEU). This report focuses on the tasks accomplished by the University of Tennessee Knoxville (UTK) team from the Department of Mechanical, Aerospace, and Biomedical Engineering (MABE) that provided expert support in multiphysics modeling of complex problems associated with the LEU conversion of the HFIR reactor. The COMSOL software was used as the main computational modeling tool, whereas Solidworks was also used in support of computer-aided-design (CAD) modeling of the proposed LEU fuel design. The UTK research has been governed by a statement of work (SOW), which was updated annually to clearly define the specific tasks reported herein. Ph.D. student Isaac T. Bodey has focused on heat transfer and fluid flow modeling issues and has been aided by his major professor Dr. Rao V. Arimilli. Ph.D. student Franklin G. Curtis has been focusing on modeling the fluid-structure interaction (FSI) phenomena caused by the mechanical forces acting on the fuel plates, which in turn affect the fluid flow in between the fuel plates, and ultimately the heat transfer, is also affected by the FSI changes. Franklin Curtis has been aided by his major professor Dr. Kivanc Ekici. M.Sc. student Adam R. Travis has focused two major areas of research: (1) on accurate CAD modeling of the proposed LEU plate design, and (2) reduction of the model complexity and dimensionality through interdimensional coupling of the fluid flow and heat transfer for the HFIR plate geometry. Adam Travis is also aided by his major professor, Dr. Kivanc Ekici. We must note that the UTK team, and particularly the graduate students, have been in very close collaboration with Dr. James D. Freels (ORNL technical monitor and mentor) and have benefited greatly from his leadership and expertise in COMSOL modeling of complex physical phenomena. Both UTK and ORNL teams have used COMSOL releases 3.4 through 5.0 inclusive (with particular emphasis on 3.5a, 4.3a, 4.3b, and 4.4) for most of the work described in this report, except where stated otherwise. Just as in the performance of the research, each of the respective sections has been originally authored by respective authors. Therefore, the reader will observe a contrast in writing style throughout this document.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2017

Characterization of the Environmentally Induced Chemical Transformations of Uranium Tetrafluoride

A key challenge with nuclear safeguards environmental sampling is identification of the materials post release due to subsequent chemical reactions with ambient water and oxygen. Uranium Tetrafluoride (UF4) is of interest as an intermediate in both the upstream and downstream portions of uranium feedstock and metal production processes used in nuclear fuel production; however minimal published research exists relating to UF4 hydrolysis. FY16 efforts were dedicated to in-situ Raman spectroscopy and X-ray diffraction characterization of UF4 during exposure to various relative humidity conditions. This effort mapped several hydrolysis reaction pathways and identified both intermediate, and terminal progeny species.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2018

Biota dose assessment of small mammals sampled near uranium mines in northern Arizona

In 2015, the U. S. Geological Survey (USGS) collected approximately 50 small mammal carcasses from Northern Arizona uranium mines and other background locations. Based on the highest gross alpha results, 11 small mammal samples were selected for radioisotopic analyses. None of the background samples had significant gross alpha results. The 11 small mammals were identified relative to the three ‘indicator’ mines located south of Fredonia, AZ on the Kanab Plateau (Kanab North Mine, Pinenut Mine, and Arizona 1 Mine) (Figure 1-1) and are operated by Energy Fuels Resources Inc. (EFRI). EFRI annually reports soil analysis for uranium and radium-226 using Arizona Department of Environmental Quality (ADEQ)-approved Standard Operating Procedures for Soil Sampling (EFRI 2016a, 2016b, 2017). In combination with the USGS small mammal radioiosotopic tissue analyses, a biota dose assessment was completed by Savannah River National Laboratory (SRNL) using the RESidual RADioactivity-BIOTA (RESRAD-BIOTA, V. 1.8) dose assessment tool provided by the Argonne National Laboratory (ANL 2017).

63 RADIATION, THERMAL, AND OTHER ENVIRON. POLLUTAN↗
DOE OSTI2016

Development of molecular dynamics potential for uranium silicide fuels

The use of uranium-silicide (U-Si) in place of uranium dioxide (UO{sub 2}) is one of the promising concepts being proposed to increase the accident tolerance of nuclear fuels for light water reactors. First-principles based density functional theory (DFT) electronic structure calculations may provide the most reliable information. However, it is probably not possible to obtain kinetic information such as amorphization under irradiation directly from DFT simulations due to size and time limitations. Thus, a more feasible way may be to employ molecular dynamics (MD) simulation. Unfortunately, so far no MD potential is available for U-Si to discover the underlying mechanisms. Here, we present our recent progress in developing a U-Si potential. The development is based on the Tersoff type potentials for single element U and Si. The Si potential is taken from the literature and a Tersoff type U potential is developed in this project. With the primary focus on the U{sub 3}Si{sub 2} phase, some other U-Si systems such as U{sub 3}Si are also included as a test of the transferability of the potentials for binary U-Si phases. Based on the potentials for unary U and Si, two sets of parameters for the binary U-Si system are developed using the Tersoff mixing rules and the cross-term fitting, respectively. The cross-term potential is found to give better results on the enthalpy of formation, lattice constants and elastic constants than those produced by the Tersoff mixing potential, with the reference data taken from either experiments or DFT calculations. In particular, the results on the formation enthalpy and lattice constants for the U{sub 3}Si{sub 2} phase and lattice constants for the high temperature U{sub 3}Si (h-U{sub 3}Si) phase generated by the cross-term potential agree well with experimental data. Reasonable agreements are also reached on the elastic constants of U{sub 3}Si{sub 2}, on the formation enthalpy for the low temperature U{sub 3}Si (m-U{sub 3}Si) and h-U{sub 3}Si phases, and on the lattice constants of m-U{sub 3}Si phase. All these phases are predicted to be mechanically stable. The unary U potential is also tested for three metallic U phases (α, β, γ). The potential is found capable to predict the cohesive energies well against experimental data for all three phases. It matches reasonably with previous experiments on the lattice constants and elastic constants of αU. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2017

Use of spectral shift to greatly improve uranium utilisation in FHR designs

Fluoride-salt-cooled high-temperature reactors (FHRs) are thermal-spectrum nuclear reactors defined by their use of liquid-fluoride-salt coolants, together with tri-isotropic (TRISO)-coated particle fuels and graphite moderator materials (Forsberg, 2004). FHRs are also characterized by their improved thermodynamic efficiency relative to gas-cooled reactors. The liquid salt coolant is designed to operate with high core outlet temperature and nearly atmosphere pressure. These features allow the FHR to possess higher core power density compared to gas-cooled TRISO-based systems. However, industry fabrication limitations result in a low volumetric fraction of fuel kernel in TRISO particles. In order to obtain reasonable operation periods, the enrichment needs to be in the high LEU (low enriched uranium) range as was proposed in the original design (Greene, 2010). Recent studies (Ilas, 2014) presented newly repurposed SmAHTR-CTC reactor concept that relies on prior experience obtained from the 2010 initial SmAHTR design (Greene, 2010). This design consists of 19 hexagonal fuel assemblies arranged in a 3-ring hexagonal geometry with 18 fuel plates each. The active length of fuel plates in each fuel assembly is 4 meters. The proposed SmAHTR-CTC achieves substantial improvements from the neutronic performance standpoint over the original concept. The results indicate that a fuel cycle length of over two years with discharged fuel burnup of 40 gigawatt-day per metric ton of initial heavy metal (HM) is possible with an 8% fuel enrichment in a once-through fuel cycle. However, the lower uranium enrichment loading requires a more frequent refueling strategy and hence considerably reduces the cycle length. It is necessary to achieve reasonable cycle length values but at the same time to extend the residence time of the fuel, especially since the costs associated with TRISO-fuel are substantially higher (Shropshire et al., 2008) than traditional UO{sub 2} fuel ($10,000/kg for TRISO vs $200/kg for UO{sub 2}). This paper presents an approach to extend the operational time and improve fuel utilization of FHR by means of spectral shift control. This is achieved by incorporating movable graphite structures into the design, instead of the static graphite blocks presently envisaged. At beginning of life (BOL), the graphite structures are withdrawn. The reactor is under-moderated, with excess neutrons being primarily captured in {sup 238}U, breeding {sup 239}Pu. Towards the end of life (EOL), the graphite structures are inserted, thermalizing the neutron spectrum and increasing reactivity. The extra {sup 239}Pu bred during the cycle is then burned, allowing the cycle and discharge burnup to be extended. Such movable structures regime should be feasible from an engineering point of view, given that it is broadly equivalent to inserting and withdrawing control rods. The preliminary results indicate that such a design may considerably improve the fuel utilization.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2026

Uranium Doped Gallium Nitride Epitaxial Thin Films

Gallium nitride (GaN) is near ubiquitous in modern day technologies, forming the backbone of solid-state lighting and high-power electronics. Engineering the physical properties of GaN has been investigated to some degree by the incorporation or doping of most of the elements of the periodic table, but the actinides remain unexplored. Molecular beam epitaxy is used to demonstrate uranium doping of GaN single crystals. High structural quality of the host matrix is maintained despite partial elemental segregation of the uranium dopant into 1D structures at the levels presented here. Electronic transport measurements reveal relatively high conductivity, which persists down to cryogenic temperature and is characterized by the formation of narrow gaps in the electronic band structures very close to the Fermi level. Photoluminescence measurements reveal that the U-doped GaN exhibits optical behavior similar to that of the GaN substrate. The addition of actinide materials to a non-centrosymmetric, optically active, radiation-hard, and electronically tunable host matrix opens a world of possibilities for investigating and leveraging elements with high electron correlations in the pursuit of novel devices.

36 - MATERIALS SCIENCE↗
DOE OSTI2016

Facile Reductive Silylation of UO 2 2+ to Uranium(IV) Chloride

General reductive silylation of the UO 2 2+ cation occurs readily in a one-pot, two-step stoichiometric reaction at room temperature to form uranium(IV) siloxides. Addition of two equivalents of an alkylating reagent to UO 2 X 2 (L) 2 (X=Cl, Br, I, OTf; L=triphenylphosphine oxide, 2,2'-bipyridyl) followed by two equivalents of a silyl (pseudo)halide, R 3 Si-X (R=aryl, alkyl, H; X=Cl, Br, I, OTf, SPh), cleanly affords (R 3 SiO) 2 UX 2 (L) 2 in high yields. Support is included for the key step in the process, reduction of UVI to UV. This procedure is applicable to a wide range of commercially available uranyl salts, silyl halides, and alkylating reagents. Under this protocol, one equivalent of SiCl 4 or two equivalents of Me 2 SiCl 2 results in direct conversion of the uranyl to uranium(IV) tetrachloride. Full spectroscopic and structural characterization of the siloxide products is reported.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗