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At least 145 records · Page 8
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

U(VI) binding onto electrospun polymers functionalized with phosphonate surfactants

We previously observed that phosphonate functionalized electrospun nanofibers can uptake U(VI), making them promising materials for sensing and water treatment applications. Here, we investigate the optimal fabrication of these materials and their mechanism of U(VI) binding under the influence of environmentally relevant ions (e.g., Ca 2+ and CO 3 2- ). We found that U(VI) uptake was greatest on polyacrylonitrile (PAN) functionalized with longer-chain phosphonate surfactants (e.g., hexa- and octadecyl phosphonate; HDPA and ODPA, respectively), which were better retained in the nanofiber after surface segregation. Subsequent uptake experiments to better understand specific solid-liquid interfacial interactions were carried out using 5 mg of HDPA-functionalized PAN mats with 10 μM U at pH 6.8 in four systems with different combinations of solutions containing 5 mM calcium (Ca 2+ ) and 5 mM bicarbonate (HCO 3 -). U uptake was similar in control solutions containing no Ca 2+ and HCO 3 - (resulting in 19 ± 3% U uptake), and in those containing only 5 mM Ca2+ (resulting in 20 ± 3% U uptake). A decrease in U uptake (10 ± 4% U uptake) was observed in experiments with HCO 3 -, indicating that UO 2 -CO 3 complexes may increase uranium solubility. Results from shell-by-shell EXAFS fitting, aqueous extractions, and surface-enhanced Raman scattering (SERS) indicate that U is bound to phosphonate as a monodentate inner sphere surface complex to one of the hydroxyls in the phosphonate functional groups. New knowledge derived from this study on material fabrication and solid-liquid interfacial interactions will help to advance technologies for use in the in-situ detection and treatment of U in water.

42 ENGINEERING↗
DOE OSTI2023

Polymorphism and phase transitions in Na 2 U 2 O 7 from density functional perturbation theory

Polymorphism and phase transitions in sodium diuranate, Na 2 U 2 O 7 , are investigated with density functional perturbation theory (DFPT). Thermal properties of crystalline α-, β- and γ-Na 2 U 2 O 7 polymorphs are predicted from DFPT phonon calculations, i.e., the first time for the high-temperature γ-Na 2 U 2 O 7 phase (R$\bar{3}$ with combining macron]m symmetry). The standard molar isochoric heat capacities predicted within the quasi-harmonic approximation are C p (298.15K)= 219.4 and 220.9 J K -1 mol -1 mfor P21/a α-Na 2 U 2 O 7 and C2/m β-Na 2 U 2 O 7 , respectively. Gibbs free energy calculations reveal that α-Na 2 U 2 O 7 (P2 1 /a) and β-Na 2 U 2 O 7 (C2/m) are almost energetically degenerate at low temperature, with β-Na 2 U 2 O 7 becoming slightly more stable than α-Na 2 U 2 O 7 as temperature increases. Here these findings are consistent with XRD data showing a mixture of α and β phases after cooling of γ-Na 2 U 2 O 7 to room temperature and the observation of a sluggish α → β phase transition above ca. 600 K. A recently observed α-Na 2 U 2 O 7 structure with P21 symmetry is also shown to be metastable at low temperature. Based on Gibbs free energy, no direct β → γ solid-solid phase transition is predicted at high temperature, although some experiments reported the existence of such phase transition around 1348 K. This, along with recent experiments, suggests the occurrence of a multi-step process consisting of initial β-phase decomposition, followed by recrystallization into γ-phase as temperature increases.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Coupling and recoupling coefficients for Wigner’s U(4) supermultiplet symmetry

A novel procedure for evaluating Wigner coupling coefficients and Racah recoupling coefficients for U(4) in two group–subgroup chains is presented. The canonical U(4) > U(3) > U(2) > U(1) coupling and recoupling coefficients are applicable to any system that possesses U(4) symmetry, while the physical U(4) coupling coefficients are more specific to nuclear structure studies that utilize Wigner’s supermultiplet symmetry concept. The procedure that is proposed sidesteps the use of binomial coefficients and alternating sum series and consequently enables fast and accurate computation of any and all U(4)-underpinned features. The inner multiplicity of a (S, T) pair within a single U(4) > SU S (2) Ⓧ SU T (2) irreducible representation is obtained from the dimension of the null space of the SU(2) raising generators, while the resolution for the outer multiplicity follows from the work of Alex et al. on U(N) . It is anticipated that a C++ library will ultimately be available for determining generic coupling and recoupling coefficients associated with both the canonical and the physical group–subgroup chains of U(4).

Cross-Coupling Reaction↗
DOE OSTI2022

Orders of vanishing and U(1) charges in F-theory

Many interesting questions about F-theory models, including several concerning the F-theory swampland, involve massless matter charged under U(1) gauge symmetries. It is therefore important to better understand the geometric properties of F-theory models realizing various U(1) charges. We propose that, for F-theory models described by elliptic fibrations in Weierstrass form, the U(1) charge of light matter is encoded in the orders of vanishing of the section components corresponding to the U(1) gauge symmetry. We give specific equations relating the U(1) charges to the orders of vanishing that seem to hold for both U(1)-charged singlets and for matter additionally charged under a simply-laced nonabelian gauge algebra. Our formulas correctly describe properties of F-theory models in the prior literature, and we give an argument that they should describe the orders of vanishing for arbitrarily high U(1) charges. They also resemble formulas for the p-adic valuations of elliptic divisibility sequences developed by Stange. These proposals could serve as a U(1) analogue of the Katz-Vafa method, allowing one to determine U(1) charges without resolution. Additionally, they predict geometric information about F-theory models with general U(1) charges, which may be useful for exploring the F-theory landscape and swampland.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2024

Exploring constituent redistribution in irradiated U-19Pu-14Zr fuel via electron probe microanalysis

Here, the phenomena of constituent redistribution, wherein a previously homogeneous metallic fuel forms discrete, radially concentric compositional zones upon irradiation was investigated by examining an irradiated U-19Pu-14Zr fuel (where numbers represent wt. %) with a burnup of 11.5 at.% with electron probe microanalysis (EPMA) and quadruple inductively coupled plasma mass spectroscopy (Q-ICP-MS). EPMA-generated U, Pu, and Zr compositional data obtained from a diameter traverse of the sample was converted to mass and was used to: 1) compare the overall fuel element analysis results between the two methods, 2) determine the number of compositionally distinct zones forming as a result of constituent redistribution; and 3) quantify the post-irradiation loss or gain of U, Pu, and Zr atoms in each distinct compositional zone. Weight percent concentrations of U, Pu, and Zr for the overall cross section compare favorably between the two analytical methods, suggesting that the spatially resolved EPMA analysis complements bulk chemical analysis. Among the four identified compositional zones, post-irradiation quantification of U, Pu, and Zr elemental atom content changes shows that the quantity of U atoms lost from the innermost zone is slightly less than the quantity of U atoms gained by the middle two zones, and the quantity of Zr atoms lost from the high-U third zone is slightly less than is gained by the two innermost zones. Pu is lost from all four zones, although the innermost zone and the high-U third zone lose a significantly higher percentage (> 22 %) of their initial Pu atoms than the other two zones. For all three elements, EPMA cannot distinguish between atoms lost due to transport to a different zone from atoms lost due to nuclear processes; however, the insight gained from using this process can be used to experiment with new modeling techniques to predict constituent redistribution in U-Pu-Zr fuels.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2023

U–C Bond Insertion, Ring-Opening, and C–H Activation in a Uranium Bis(diisopropylamino)cyclopropenylidene (BAC) Adduct

Reaction of [U(NR 2 ) 3 ] (R = SiMe 3 ) with 1 equiv of bis(diisopropylamino)cyclopropenylidene (BAC) in Et 2 O results in the formation of [(NR 2 ) 3 U(BAC)] (1), which can be isolated in modest yields. Thermolysis of 1 in C 6 D 6 at 85 °C results in the formation of the ring-opened U(IV) product, [(NR 2 ) 2 U{N(R)(SiMe 2 CH=C(NiPr 2 )C(NiPr 2 )=CH)}] (2), which can be isolated in low yields. Mechanistic studies suggest that the formation of 2 proceeds via dissociation of BAC from 1 to regenerate [U(NR 2 ) 3 ], which converts into [U{N(R)(SiMe 2 CH 2 )}(NR 2 ) 2 ] at the elevated temperatures. BAC then inserts into the U–C bond of [U{N(R)(SiMe 2 CH 2 )}(NR 2 ) 2 ] to generate a cyclopropenyl intermediate, which undergoes ring opening and C–H activation to afford the final product, 2. We hypothesize that the ring-opening generates an unobserved carbene intermediate. Notably, thermolysis of a 1:1 mixture of independently prepared [U{N(R)(SiMe 2 CH 2 )}(NR 2 ) 2 ] and BAC results in clean formation of 2, providing strong support for the proposed mechanism. The formulations of both 1 and 2 were confirmed by X-ray crystallography. Finally, theoretical calculations indicate that the hypothesized uranium carbene intermediate features strong U–C bonding, potentially with some carbyne character in the electronic structure.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2020

Supramolecular Assembly of U(IV) Clusters and Superatoms with Unconventional Countercations

Superatoms are nanometer-sized molecules or particles that form ordered lattices, mimicking their atomic counterparts. Hierarchical assembly of superatoms gives rise to emergent properties in lattices of quantum dots, p-block clusters, and fullerenes. In this report, we introduce a family of uranium-oxysulfate cluster anions whose hierarchical assembly in water is controlled by two parameters: acidity and the lanthanide or transition-metal countercation. In acid, larger Ln III (Ln = La–Ho) link hexamer (U 6 ) oxoclusters into body-centered cubic frameworks, while smaller Ln III (Ln = Er–Lu and Y) promote linking of 14 U 6 clusters into hollow superclusters (U 84 superatoms). U 84 assembles into superlattices including cubic-closest packed, body-centered cubic, and interpenetrating networks, bridged by interstitial countercations and U 6 clusters. Divalent transition metals (TM = Mn II and Zn II ) charge-balance and promote the fusion of 10 U 6 and 10 U monomers into a wheel-shaped cluster (U 70 ). Dissolution of U 70 in organic media shows (by small-angle X-ray scattering) that differing supramolecular assemblies are accessed, controlled by TM II -linking of U 70 clusters. Magnetic measurements of these assemblies reveal Curie–Weiss behavior at high temperatures, without pairing of the 5f 2 -electrons down to 2 K.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Passive and active neutron signatures of 233 U for nondestructive assay

The thorium fuel cycle is emerging as an attractive alternative to conventional nuclear fuel cycles, as it does not require the enrichment of uranium for long-term sustainability. The operating principle of this fuel cycle is the irradiation of 232 Th to produce 233 U, which is fissile and sustains the fission chain reaction. 233 U poses unique challenges for nuclear safeguards, as it is associated with a uniquely extreme γ-ray environment from 232 U contamination, which limits the feasibility of the γ-ray-based assay, as well as more conservative accountability requirements than for 235 U set by the International Atomic Energy Agency. Consequently, instrumentation used for safeguarding 235 U in traditional fuel cycles may be inapplicable. It is essential that the nondestructive signatures of 233 U be characterized so that nuclear safeguards can be applied to thorium fuel-cycle facilities as they come online. In this work, a set of 233 U 3 O 8 plates, containing 984 g 233 U, was measured at the National Criticality Experiments Research Center. A high-pressure 4 He gaseous scintillation detector, which is insensitive to γ-rays, was used to perform a passive fast neutron spectral signature measurement of 233 U 3 O 8 , and was used in conjunction with a pulsed deuterium-tritium neutron generator to demonstrate the differential die-away signature of this material. Furthermore, an array of 3 He detectors was used in conjunction with the same neutron generator to measure the delayed neutron time profile of 233 U, which is unique to this nuclide. These measurements provide a benchmark for future nondestructive assay instrumentation development, and demonstrate a set of key neutron signatures to be leveraged for nuclear safeguards in the thorium fuel cycle.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2020

Microstructure, Thermal, and Mechanical Properties Relationships in U and UZr Alloys (Final Report)

Uranium-zirconium (U-Zr) alloys are candidate fuel systems for transmutation based reactors that can be used to burn long-lived minor actinides and fission products in fast spectrum reactors. Metallic fuels have also been gaining more recent attention for applications as accident tolerant fuels, as well as for use in small modular reactors. This research focused on a “science-based” approach to capture the connections between U and U-Zr alloys’ three-dimensional (3-D) microstructure, thermal properties, and mechanical properties through closely coordinated experiments and modeling efforts from the unirradiated to the irradiated fuels. Advanced characterization and modeling techniques were used to understand irradiation-induced microstructural evolution and its direct impact on the thermal and mechanical properties of U and U-Zr fuel. Closely coordinated experiments and modeling were performed to provide crucial data that does not currently exist. Overall, this research spanned multiple length and time scales within the models and experiments. The scope of the research encompassed the understanding of the irradiation effects in U and various U-Zr alloys with particular attention paid to three task areas: (1) microstructural evolution, (2) in-situ/ex-situ thermal and mechanical properties, and (3) multiscale modeling connections to microstructure, thermal, and mechanical properties. This research resulted in (1) the 3-D characterization of neutron irradiated U-Zr fuel in multiple phase regions to better understand fission gas swelling and constituent redistribution, (2) development of a microstructural model linking thermal and mechanical properties via in situ Raman and nanoindentation, (3) and mesoscale phase field modeling was coupled with the AEH method in the MOOSE framework was used to calculate the effective thermal conductivities of U-Zr fuels consisting of α-U and δ-UZr 2 heterogeneous microstructures.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2022

Evaluated 238 U(n,f) Average Prompt Fission Neutron Multiplicities Including the CGMF Model

This report documents an evaluation of the average prompt fission neutron multiplicity, $\overline{v}_p$, of 238 U from 800 keV to MeV. This evaluation had to be re-done from “scratch” as the input to previous $\overline{v}_p$ evaluations, specifically ENDF/B-VIII.0, was not found. That means that all available experimental data were re-analyzed and uncertainties were re-estimated. The new evaluated 238 U $\overline{v}_p$ based on only experimental data differs distinctly from ENDF/B-VIII.0 $\overline{v}_p$ from 2 to 4.5 MeV, and from 6 to 7 MeV, and is otherwise similar. The difference from 2 to 4.5 MeV stems from the fact that ENDF/B-VIII.0 was tweaked in this energy range to data of Frehaut, while two other, equally trustworthy, data sets would indicate an evaluated 238 U $\overline{v}_p$ that is up to 2% higher. Also, second chance fission in ENDF/B-VIII.0 was smoothed over from 6–7 MeV. Another major difference to ENDF/B-VIII.0 is that one of the evaluations presented here includes model information from the Hauser-Feshbach fission fragment decay code CGMF, while ENDF/B-VIII.0 is based purely on experimental data. CGMF links several fission quantities with each other; $\overline{v}_p$ is predicted by assumptions made on, e.g., pre-neutron emission yields as a function of mass, the total kinetic energy, or spin and parity of fission fragments. This allows to validate the new 238 U $\overline{v}_p$ by using CGMF parameters obtained from fitting to experimental 238 U $\overline{v}_p$ to predict yields as a function of mass, the average total kinetic energy, or the mean energy of the prompt fission neutron spectrum. These model-predicted values can then be compared to experimental and evaluated data. The model-predicted fission-observable values using evaluated parameters obtained here are reasonably close to experimental data for some observables, but are farther away from experimental data related to TKE observables. In addition to that, the evaluated 238 U(n,f) $\overline{v}_p$ shows similar deviations from ENDF/B-VIII.0 as for the evaluation with only experimental data. This difference is expected to lead to changes in simulated effective neutron multiplication factor, $k_{eff}$ of ICSBEP critical assemblies that are sensitive to 238 U in the fast range (BigTen, Flattop, Flattop-Pu). These changes in $k_{eff}$ need to be counter-balanced. Chi-Nu PFNS experimental data are expected to be released in the next few months that might lead to the needed changes in the PFNS. Until then, we hold off in benchmarking the new 238 U(n,f) $\overline{v}_p$ as well as submitting it to ENDF/B-VIII.1. Also, new high-precision 238 U $\overline{v}_p$ are expected to be measured by the CEA in the next two years that will shed further light on question on 238 U $\overline{v}_p$ from 2–4.5 and 6–7 MeV.

238U↗
DOE OSTI2024

NSTX-U liquid metal core-edge facility (LMCE)

NSTX-U/LMCE will provide a unique and world-leading research facility to address the primary challenge to delivering economic and timely magnetic fusion energy, namely the need to develop a power and particle exhaust and first-wall system that can withstand very high edge heat fluxes, maximize energy confinement, and avoid the production of large masses of solid eroded first-wall material. The NSTX-U/LMCE facility will assess the ability of liquid metals (LMs) – especially liquid lithium – to provide a new boundary condition for magnetic fusion systems, to extend the lifetime of the plasma facing components (PFCs) and improve core plasma confinement. Such capability is needed to establish the basis for next-step fusion facilities including fusion pilot plants, and to maintain U.S. world leadership in core-edge integration research. NSTX-U/LMCE will leverage the ability to generate very high divertor perpendicular heat flux q⊥ ~ 100MW/m 2 , extensive diagnostics, and liquid-metal-applicable infrastructure of NSTX-U. NSTX-U/LMCE will provide access to a high-confinement plasma core with majority self-driven plasma current, the flexibility to test a range of liquid metal divertor concepts, access to a range of separatrix collisionalities (from high to very low), and the ability to controllably vary the first-wall temperature to vary the plasma- wall interaction physics on liquid lithium components. Further, NSTX-U/LMCE will utilize more reactor-relevant high-Z refractory-metal PFC substrates. With these capabilities the NSTX-U/LMCE facility will explore the full continuum of core-edge solutions ranging from high core radiated power, to conditions with radiative losses concentrated in the scrape-off layer (SOL), and ultimately low recycling conditions. The low collisionality SOL that may be accessible in the low recycling regime is relatively unexplored and will require a kinetic treatment of the edge, which can be addressed theoretically, and with experiments in LTX-β. Additional smaller-scale preparatory R&D facilities will be required to reduce the risk of premature technical/engineering failure of liquid metal systems implemented in NSTX-U. The NSTX-U/LMCE facility aligns very well with recommendations in the FESAC Long-Range Plan and NASEM Pilot Plant reports and the Bold Decadal Vision, will be unique in the world program throughout the next decade, and is garnering private company interest in utilizing NSTX-U/LMCE for development of LM PFCs.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
NASA NTRS1993

Th-230 - U-238 series disequilibrium of the Olkaria rhyolites Gregory Rift Valley, Kenya: Petrogenesis

Positive correlations of (U-238/Th-230) versus Th show the rhyolites to be products of partial melting. Positive correlations of U and Cl and U and F show that the U enrichment in the rhyolites is associated with the halogen contents which may be related to the minor phenocryst phase fractionation. Instantaneous Th/U ratios exceed time integrated Th/U ratios providing further evidence of the hydrous nature of the Olkaria rhyolite source. Excess (U-238/Th-230) in the subduction related rocks has been associated to the preferential incorporation of uranium in slab derived fluids, but no evaluation of the size of this flux has been made. The majority of the Naivasha samples show a (U-238/Th-230) less than 1 and plot close to the subduction related samples indicating the Naivasha rhyolites may also have been influenced by fluids during their formation. In general samples with high (U-238/Th-230) ratios reflecting recent enrichment of uranium relative to thorium have high thorium contents, thereby the high (U-238/Th-230) ratios are restricted to the most incompatible element enriched magmas and, hence, are a good indication that the rhyolites were formed by partial melting. If a fluid phase had some influence on the formation of the rhyolites then the uranium and thorium may have some correlation with F and Cl contents which can be mirrored by the peralkalinity. Plots of uranium against F and Cl contents are shown. The positive correlation indicates that the uranium enrichments are associated with the halogen contents. There seems to be a greater correlation for U against Cl than F indicating that the U may be transported preferentially as Cl complexes.

Black, S.↗
DOE OSTI2022

Minimizing thickness variation in monolithic U-10Mo fuel foil and Zr interlayer during hot rolling: A microstructure-based finite element method analysis

Low-enriched uranium alloyed with 10 wt. % molybdenum (U-10Mo) has been identified as a promising alternative to highly enriched uranium fuel for the United States’ high performance research reactors. The monolithic U-10Mo fuel plate consists of a metallic U-10Mo fuel foil with a 25 µm Zr interlayer and a relatively thick cladding of aluminum alloy 6061. The Zr interlayer is typically applied during the hot co-rolling process, and this process dictates the uniformity of the Zr interlayer. Thickness variation observed in the U-10Mo and Zr interlayer has been attributed to several sources: the initial grain size of the U-10Mo castings, can materials, rolling temperature, inhomogeneous molybdenum content, and porosity in the cast U-10Mo. This thickness variation limits the ability to meet the dimensional specification; thus, a better understanding of the factors causing the nonuniform thickness is needed. In this work, we used a novel, microstructure-based finite element method to model the hot rolling process to address these concerns. Grain microstructures in U-10Mo were tessellated and explicitly considered in the finite element model. Each grain was assigned a random material property to mimic the grain strength variations induced by different grain orientations. Simulations were performed using six steel can thicknesses, four grain sizes, and with or without a Zr interlayer to investigate the influences of those variables on the thickness nonuniformity. The simulation results showed that a thinner steel can and finer U-10Mo grain size reduce thickness variations in both the U-10Mo fuel foil and Zr interlayer. The direct findings from the simulations and analysis can be used to optimize the hot rolling schedule, reduce fabrication defects, and meet the dimensional specifications. The proposed microstructure-based finite element model can be also coupled with experimental microstructure characterization data, images, and models to simulate multi-pass hot rolling.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Materials Data on U(Al5Fe)2 by Materials Project

UFe2Al10 crystallizes in the orthorhombic Cmcm space group. The structure is three-dimensional. U is bonded in a 8-coordinate geometry to four equivalent Fe and sixteen Al atoms. All U–Fe bond lengths are 3.41 Å. There are a spread of U–Al bond distances ranging from 3.10–3.60 Å. Fe is bonded in a 10-coordinate geometry to two equivalent U and ten Al atoms. There are a spread of Fe–Al bond distances ranging from 2.52–2.70 Å. There are five inequivalent Al sites. In the first Al site, Al is bonded in a 12-coordinate geometry to one U, two equivalent Fe, and nine Al atoms. There are a spread of Al–Al bond distances ranging from 2.61–3.00 Å. In the second Al site, Al is bonded in a 2-coordinate geometry to one U, two equivalent Fe, and eight Al atoms. There are a spread of Al–Al bond distances ranging from 2.58–2.80 Å. In the third Al site, Al is bonded in a 2-coordinate geometry to two equivalent U, two equivalent Fe, and eight Al atoms. There are a spread of Al–Al bond distances ranging from 2.71–2.79 Å. In the fourth Al site, Al is bonded in a 2-coordinate geometry to two equivalent U, two equivalent Fe, and eight Al atoms. Both Al–Al bond lengths are 2.68 Å. In the fifth Al site, Al is bonded in a 2-coordinate geometry to two equivalent U, two equivalent Fe, and eight Al atoms.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Materials Data on U(Al5Ru)2 by Materials Project

URu2Al10 crystallizes in the orthorhombic Cmcm space group. The structure is three-dimensional. U is bonded in a 10-coordinate geometry to four equivalent Ru and sixteen Al atoms. All U–Ru bond lengths are 3.45 Å. There are a spread of U–Al bond distances ranging from 3.15–3.63 Å. Ru is bonded in a 10-coordinate geometry to two equivalent U and ten Al atoms. There are a spread of Ru–Al bond distances ranging from 2.58–2.74 Å. There are five inequivalent Al sites. In the first Al site, Al is bonded in a distorted linear geometry to two equivalent U and two equivalent Ru atoms. In the second Al site, Al is bonded in a 2-coordinate geometry to one U and two equivalent Ru atoms. In the third Al site, Al is bonded in a distorted bent 120 degrees geometry to two equivalent U and two equivalent Ru atoms. In the fourth Al site, Al is bonded in a distorted bent 120 degrees geometry to two equivalent U and two equivalent Ru atoms. In the fifth Al site, Al is bonded in a 12-coordinate geometry to one U and two equivalent Ru atoms.

36 MATERIALS SCIENCE↗
DOE OSTI2021

ZrN coating as diffusion barrier in U(Mo) dispersion fuel systems

The control of the interaction between the U(Mo) fuel phase and the Al matrix is one of the challenges of dispersion fuel plate development for research reactors. Given the specific properties of this interaction layer, larger amounts of it in the meat could lead to a reduction of the plate mechanical integrity and thermal conductivity, eventually leading to pillowing. The SELENIUM project showed that by depositing a ZrN coating on the surface of the U(Mo) fuel particles, the amount of formed U(Mo)-Al interaction layer is limited but still present. Microstructural analysis performed on the as fabricated coating and fresh fuel plates containing ZrN coated U(Mo) dispersed in an Al matrix, revealed that the coating gets damaged during plate production. The post irradiation examinations (PIE) of the ZrN coated U(Mo) fuel plates, from the SELENIUM and SEMPER FIDELIS experiments, show how the U(Mo)-Al interaction layer is formed -only at those locations where the coating is missing or damaged -and the evolution of coating microstructure during irradiation. Finally, as a remedy, to further reduce the amount of interaction layer formed, the use of an Al-Si matrix was proposed based on the higher affinity of Si for U compared to the affinity of Al for U. PIE of a fuel plate consisting of ZrN coated U(Mo) dispersed in an Al-Si matrix irradiated in the SEMPER FIDELIS experiment, clearly demonstrates the benefit of adding Si to the matrix.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Fuel-cladding chemical interaction of a prototype annular U-10Zr fuel with Fe-12Cr ferritic/martensitic HT-9 cladding

As an alternative fuel form, the annular metallic fuel design eliminates the liquid sodium bond between the fuel and the cladding, providing back-end fuel cycle and other benefits. The fuel-cladding chemical interaction (FCCI) of annular fuel also presents new features. In this work, state-of-the-art electron microscopy and spectroscopy techniques were used to study the FCCI of a prototype annular U-10wt%Zr (U-10Zr) fuel with ferritic/martensitic HT-9 cladding irradiated to 3.3% fission per initial heavy atom. Compared with sodium-bonded solid fuels, negligible amounts of lanthanides were found in the FCCI layer in the investigated helium-bonded annular fuel. Instead, most lanthanides were retained in the newly formed UZr 2 phase in the fuel center region. The interdiffusion of iron and uranium resulted in tetragonal ( U ,Zr) 6 Fe phase (space group I4/mcm) and cubic ( U ,Zr)( Fe ,Cr) 2 phase (space group Fd 3 ¯ m). The ( U ,Zr)( Fe ,Cr) 2 phase contains a high density of voids and intergranular uranium monocarbides of NaCl-type crystal structure (space group Fm 3 ¯ m). At the interdiffusion zone and inner cladding interface, a porous lamellar structure composed of alternating Cr-rich layers and U-rich layers was observed. Next to the lamellar region, the unexpected phase transformation from body-centered cubic ferrite (α-Fe) to tetragonal binary Fe-Cr σ phase (space group P4 2 /mnm) occurred, and tetragonal Fe-Cr-U-Si phase (space group I4/mmm) was identified. Due to the diffusion of carbon into the interdiffusion zone, carbon depletion inside the HT-9 led to the disappearance of the martensite lath structure, and intergranular U-rich carbides formed as a result of the diffusion of uranium into the cladding. These detailed new findings reveal the unique features of the FCCI behavior of annular U-Zr fuels, which could be a promising alternative fuel form for high burnup fast reactor applications.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2025

Producing 236 U reference standards for Accelerator Mass Spectrometry at the University of Notre Dame

36 U is a rare isotope of uranium, naturally occurring in ores with an abundance of 236 U/ 238 U$<$ 1 x 10 -9 . The ability to detect it and make isotopic ratio measurements has applications ranging from nuclear forensics and nonproliferation to energy production and environmental protection. Currently, Accelerator Mass Spectrometry (AMS) is the only technique sensitive enough to accurately measure 236 U/ 238 U isotopic ratios as they exist in naturally occurring ores in the range of 236 U/ 238 U = 10 -12 $-$ 10 -9 . Some AMS facilities have demonstrated their capabilities to make these measurements. Historically, the lack of commercially available reference standards covering the range of naturally occurring 236 U/ 238 U abundances has necessitated the use of absolute measurements, notoriously difficult to do using AMS, resulting in increased uncertainties in measurements and a reliance on knowledge of systematic effects. To mitigate these issues, various AMS facilities have sought to develop their own reference standards. Using a reference standard prepared for other forms of mass spectrometry, a series of AMS suitable standards was created through dilution with low-background natural uranium. The techniques used to produce and characterize these materials as well as analysis of them using AMS will be discussed.

236U↗