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At least 127 records · Page 7
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Investigation of constituent redistribution in U-Pu-Zr fuels and its dependence on varying Zr content

This contribution investigates fuel constituent segregation and fuel-cladding chemical interactions (FCCI) in three U-Pu-Zr fuel pins irradiated to ~11% burnup in Experimental Breeder Reactor-II as part of the X441 DP-1 experiment. In examined pins, Zr content ranged from 6 to 10 and 14 wt.%, while Pu concentration was constant at 19 wt.% Pu. The primary goal of the investigation was to determine the role Zr content plays in fuel performance and this manuscript provides assessment of both constituent redistribution and FCCI as a function of axial position. FCCI was observed in all pins, though no cladding failure was noted. Optical and scanning electron microscopy (SEM) results show that variation in Zr content alters the number and relative size of constituent redistribution zones in the fuel. For example, larger Zr-rich central regions and smaller U-rich intermediate regions were observed in 14 wt.% Zr fuels. More importantly, all examined fuels have four or more discrete constituent redistribution regions, where each region has dissimilar morphological features. The existence of four to six distinctive regions deviates from traditionally accepted three region redistribution model, highlights complexity of constituent redistribution in this metal fuel, and identifies the need to conduct additional studies using state-of-the-art instrumentation.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2025

Elucidating the effect of minor-actinide addition on fuel-cladding chemical interaction in an HT-9 clad U-Pu-Zr metallic fuel irradiated to 6.15 at.% burnup in EBR-II

Scanning and transmission electron microscopy (S/TEM) were used to characterize the local fuel-cladding chemical interaction (FCCI) in one cross-section taken from a HT-9 clad U-20.3Pu-10Zr-1.2Am-1.3Np (in wt.%) fuel irradiated to 6.15 at.% burnup with inner cladding temperatures ranging between 460–490 °C. Results showed that the total interaction thickness between fuel and cladding was <10 µm. Fe infiltrated the fuel to form U-Zr-Fe phases while fuel elements or lanthanides did not infiltrate into the cladding. Np was not involved in the formation of any phases in the examined locations; however, Am played a role by forming a ∼2 µm thick homogeneous Fe-Pu-Am planar front at the inner cladding wall. An oxidized Na layer existed in the fuel-cladding gap with Fe and lanthanide particles dispersed within, suggesting Na could facilitate the transport of fuel and cladding constituents. Secondary phases, including an FCC Zr-rich phase, lanthanide phases, and α’-Cr(Fe) were identified in the outer fuel and FCCI regions. Furthermore, this study suggests that, for the irradiation conditions specific to this cross-section, minor actinides have little impact on FCCI behavior beyond what would be observed in typical HT-9 clad U-Pu-Zr fuel pins systems.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2021

Quasi-differential neutron induced neutron emissions from 235 U, and 239 Pu

Uncertainty in nuclear reaction cross sections, angular distributions, and other nuclear data directly impact how well simulations of nuclear systems represent physical observations. Here, to determine how well the nuclear data in ENDF/B-VIII.0, JEFF-3.3, and JENDL-4.0 evaluations describe the physical behaviour of 235 U, and 239 Pu when subjected to a neutron flux, the neutron emission spectrum was measured for carbon, 93.0% 235 U, and 93.9% 239 Pu samples, and compared against detailed MCNP6 simulations. The measurements were performed at the Los Alamos Neutron Science Center using a quasi-differential method previously developed at Rensselaer Polytechnic Institute. The measurement spanned 0.82–20 MeV and 30–150 degrees. The measurements show there are a significant number of discrepancies between library predictions of the neutron yield and physical observation. A few of the main discrepancies found are described in this paper. Based on these results a new evaluation utilizing these results for carbon, 235 U, and 239 Pu is recommended.

235U↗
DOE OSTI2022

Computational insights into the lattice dynamics of Pu(IV) oxalates

Despite its use in PuO 2 production, the structure of anhydrous Pu(C 2 O 4 ) 2 is still not completely understood. Recently, two candidate structures for Pu(C 2 O 4 ) 2 were proposed via density functional theory (DFT), after which the first experimental optical vibrational spectra were reported. Here, in this study, we calculated the lattice dynamics of the candidate structures using DFT and found that the primary difference between them is the presence of a vibrational mode near 1380 cm -1 in one structure. The frequency and optical activity of this mode agree well with the published experimental results, providing strong support for this calculated structure as that of anhydrous Pu(C 2 O 4 ) 2 .

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2025

Remeasurement of the 239 Pu(n,f)/ 235 U(n,f) Cross-Section Ratio with the NIFFTE fission Time Projection Chamber Using Vapor-deposited Targets

The NIFFTE fission Time Projection Chamber (fissionTPC) has been used to measure the 239 Pu(n,f)/ 235 U(n,f) cross-section ratio for neutron-induced fission in the range of 0.1–100 MeV, with high precision. A white neutron source was provided by the Los Alamos Neutron Science Center, where the experiment was conducted as a remeasurement to evaluate a roughly 2% discrepancy of the previous fissionTPC results with ENDF/B-VIII.0. Further, a detailed accounting of measurement uncertainties was performed, based on the fissionTPC's novel ability to provide three-dimensional reconstruction of fission-fragment ionization profiles. Current results obtained using a vapor-deposited, highly uniform 239 Pu target, in comparison to the measurement published in 2021, where a 239 Pu electroplated target was used, are presented and discussed. The remeasurement presented here is in agreement with the previous fissionTPC result within measurement uncertainties.

235U↗
DOE OSTI2022

Structural and Bonding Analysis in Monomeric Actinide(IV) Oxalate from Th(IV) to Pu(IV): Comparison with the An(IV) Nitrate Series

In this work, single-crystal X-ray diffraction (SC-XRD) structures and Raman spectra of a series of new isomorphous molecular An(IV)-oxalate compounds (Th, U, Np, and Pu) are reported. These complexes are crystallized with cobalt(III) hexamine ([Co(NH 3 ) 6 ] 3+ ) as the counter cations, [Co(NH 3 ) 6 ] 2 [An(C 2 O 4 ) 5 ]·4H 2 O, revealing five bidentate nonbridging oxalate ligands in the first coordination sphere (CN = 10). The nonbridging oxalate is rather uncommon for An(IV)-oxalate systems, which are widely characterized as polymeric compounds. Density functional theory (DFT) calculations were performed to examine the bonding between An(IV) cations and oxalate ligands. For comparison, we also report results obtained for the An(IV)-hexanitrate series, [(C 2 H 5 ) 4 N] 2 [An(NO 3 ) 6 ] (with An = Th, U, Np, Pu, and Ce), which consists of O-donor ligands as well but with a larger coordination number (CN = 12). The bonding analysis confirms that the actinide–oxygen bond is predominantly ionic with a minor increase in covalency from Th to U and slight variations from U to Pu. Further comparison showed that the charge transfer increases slightly when increasing the number of anions in the coordination sphere (C 2 O$_4^{2–}$: CN = 10; NO$_3^–$: CN = 12), but covalent effects as indicated by the amount of internuclear electron density accumulation are small and similar for oxalate and nitrate.

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

Magnetic Properties of Tetravalent Pu in the Perovskites BaPuO 3 and SrPuO 3

BaPuO 3 and SrPuO 3 were synthesized, and their structures were refined in the orthorhombic space group Pbnm , a common distortion from the classic $Pm\bar{3}$m over barm cubic perovskite. Magnetic-susceptibility measurements, obtained as a function of temperature over the range of 1.8-320 K, exhibit temperature-dependent behavior, with evidence of long-range magnetic order at temperatures higher than their lanthanide and actinide analogues: BaPuO 3 below 164(1) K and SrPuO 3 below 76(1) K. Effective moments of 1.66(10)μ B for BaPuO 3 and 1.84(8)μ B for SrPuO 3 were obtained by fitting their paramagnetic susceptibilities using the Curie-Weiss law. Further, both are below the free-ion value of 2.68 μ B expected for a Pu 4+ 5 $\mid$ 4 ground level. Ab initio wave function calculations, performed at the relativistic complete active space level including spin-orbit coupling and with an embedded cluster approach that neglects interactions between Pu centers, were used to generate embedded-cluster Pu 4+ magnetic susceptibilities. The calculations agree well with experimental data at higher temperatures, providing evidence that a single-ion representation is sufficient to account for the observed paramagnetic behavior without the need to invoke charge transfer, disproportionation, strong covalent bonding, or other more complex electronic behavior.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Temperature Dependence of 239 Pu NMR Parameters in PuO 2

Solid-state 239 Pu NMR spectra of crystalline PuO 2 have been recorded over temperatures from 11 to 295 K with better than part per thousand resolution. These experiments represent the first independent detection of 239 Pu NMR in PuO 2 since the original report by Yasuoka and co-workers and extend the NMR observations to higher temperatures where recent theoretical explanations of the enigmatic magnetism and electronic structure of PuO 2 may be evaluated. The sensitivity achieved in these experiments was sufficient to measure the sinusoidal dependence of the NMR signal amplitude on the radiofrequency pulse length, which allows the determination of the nuclear g factor and magnetic moment of 239 Pu. These results demonstrate the use of NMR with an open-shell f element to explore subtle magnetic effects in plutonium materials of both technological and scientific significance.

Actinides↗
DOE OSTI2026

An–imidophosphorane (An = U–Pu) bond covalency and proton-coupled electron transfer thermodynamics driven by orbital energy matching

A series of mid-actinide (An = U–Pu) tetrahomoleptic complexes supported by highly electron-donating imidophosphorane ligands, NPC ([NP t Bu(pyrr) 2 ] − , where t Bu = C(CH 3 ) 3 ; pyrr = pyrrolidinyl = N(C 4 H 8 )), are systematically investigated computationally and experimentally to elucidate the nature of actinide–ligand (An–L) covalency across the An 3+/4+/5+ oxidation states. Trends in An–L bonding and redox properties for these complexes, together with their protonated counterparts, are examined using orbital-, electron density-, and energy-decomposition-based methods. This integrated approach reveals progressively improved energy matching between α-spin An 5f and N im 2p orbitals with increasing atomic number and oxidation state, becoming particularly pronounced in the ligand-dominant π-bonding orbitals of An 4+ and An 5+ . In contrast to the An 3+ species, the enhanced An 5f π contributions in the higher-valent counterparts drive the increase in An–N im covalency for later An, thereby inverting the covalency trend to U < Np < Pu. Redistribution of electron density towards the An and N im atomic basins due to the growing energy-matching assisted covalency correlates with higher pKa values and increased N im –H bond dissociation free energies in protonated An 4+ complexes. Electron density at Nim in An 4+ shows a linear correlation with the p K a values calculated via the Bordwell equation. Calculations predict a cathodic shift of 0.84–1.00 V in the redox couples upon protonation, a trend validated when experimentally accessible. These findings demonstrate an increasing role of covalency driven by orbital energy matching from U to Pu in tuning the thermodynamic driving force for proton-coupled electron transfer in the An 5+ species.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2024

Predicted thermophysical properties of UN, PuN, and (U,Pu)N

Molecular dynamics and density functional theory simulations are used to predict the lattice and electronic contributions of thermophysical properties for UN, PuN, and mixed (U,Pu)N systems. The properties predicted include the lattice parameter, linear thermal expansion, enthalpy, and specific heat capacity, as a function of temperature. The simulation predictions for high temperature specific heat capacity are compared against experimental measurements to understand the behavior, and why differences in the experimental measurements are observed. The influence of adding U vacancies, N interstitials, and Pu to UN is also examined. For this, a new PuN potential parameter set is developed and used with the Kocevski UN potential, enabling the dynamics of mixed (U,Pu)N systems to be studied. How defects impact the thermophysical properties is important for understanding fuel behavior under different reactor conditions, and these mechanistic predictions can be used to support fuel performance codes where data is scarce.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2024

Anderson impurity mechanism for a multi-level model in δ-Pu

Abstract Electronic correlations and spin–orbit interactions in plutonium create variations in the bonding behavior of each of its allotropes. In δ -Pu, the 5f electrons lie at the tipping point between itinerant and localized behavior which has made the use of mixed-level models successful in describing its mechanical properties. The mechanism for the emergence of a mixed-level model has not yet been understood. We use a series of density functional theory approximations to understand the interactions that create a mixed-level description of δ -Pu which leads to accurate physical properties. With the intersite interactions present in the hybrid functional, we show that a single 5f electron engages in orbital-selective bonding that can be understood with an Anderson impurity picture. The Anderson model gives us a mechanism to understand how the bonding in δ -Pu evolves as a function of the interactions in the material such that we obtain both the accuracy and physics of the multi-level models from ab initio theory.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2026

Investigation of the 244 Pu ⁢( 48 Ca,𝑥⁢𝑛) 292−𝑥 Fl reaction with the LBNL SHREC detector: Investigation of decay chains of isotopes of flerovium (𝑍=114)

The 244 Pu ⁢( 48 Ca,𝑥⁢𝑛)⁢ 292−𝑥 Fl reaction was investigated at Lawrence Berkeley National Laboratory’s 88 Inch Cyclotron using the Berkeley Gas-filled Separator (BGS), the newly installed Superheavy Recoil detector, along with an upgraded digital electronics and data acquisition system. Seven decay chains were observed starting with an evaporation residue, followed by a single 𝛼 decay and a spontaneous fission. The decay characteristics of these seven decay chains led to an assignment to 288 Fl , the product of the 4⁢𝑛 reaction channel. Two additional chains were (tentatively) assigned to the decay of the 3⁢𝑛 exit channel, 289 Fl . Cross sections for the 4⁢𝑛 and 3⁢𝑛 exit channels were 𝜎 prod =6.7⁢($^{36}_{25}$) pb and 𝜎 prod =1.6⁢($^{22}_{11}$) pb, respectively. Another decay chain, tentatively assigned to the 5⁢𝑛 exit channel through the 48 Ca + 244 Pu reaction or the 3⁢𝑛 exit channel of the 48 Ca + 242 Pu reaction, was also detected. Detailed information regarding the observed decay chains and their nuclear structure aspects is discussed, along with the performance of the BGS and the new detection system.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2024

Constraints on 5 f -electron magnetism in Ga-stabilized $δ$-Pu from x-ray magnetic circular dichroism

Density-functional theory models of δ-Pu accurately predict crystal structure, phonon density of states, and unit cell volumes but require magnetic degrees of freedom which have never been experimentally verified. Some models invoke an on-site cancellation of spin and orbital moments, engendering a near-zero bulk magnetization, undetectable by most probes. Here, we employ x-ray magnetic circular dichroism at the Pu M 4,5 edges to directly probe spin and orbital moments using the magneto-optical sum rules. The data show no dichroism within experimental error, constraining polarized moments at 6 T and 3 K to μ L,S <0.1⁢μ B . Finally, these experiments point to the absence of even unconventional spin-orbit compensated order in δ-Pu.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Ab initio prediction of rapid kinetics of Fe impurities in δ -Pu

Here, we study the formation energies of iron impurities in δ-Pu within spin–orbital-polarized density functional theory (SOP-DFT). The thermodynamic solubility limit of iron in δ-Pu is calculated, indicating low miscibility. We show that surprisingly, Fe impurities at equilibrium are almost equally likely to occupy octahedral interstitial sites or substitutional sites, with slight preference for the former. In contrast, we find the energy of the tetrahedral interstitial Fe to be nearly 1 eV higher than the octahedral one. We explore the energy landscape for Fe impurity hopping diffusion and conclude that Fe impurities in δ-Pu are divided into two populations: (i) Immobile substitutional Fe impurities and (ii) highly mobile interstitial Fe impurities. The latter, (ii), migrate between octahedral interstitial sites with an energy barrier of around 0.2 eV. The energy barrier for exchange between the two populations is calculated to exceed 0.7 eV. Finally, we discuss the role of magnetic order on the impurity energetics.

Atomic structure↗
DOE OSTI2025

AmeriFlux FLUXNET-1F US-xPU NEON Pu'u Maka'ala Natural Area Reserve (PUUM)

This is the AmeriFlux Management Project (AMP) created FLUXNET-1F version of the carbon flux data for the site US-xPU NEON Pu'u Maka'ala Natural Area Reserve (PUUM). This is the FLUXNET version of the carbon flux data for the site US-xPU NEON Pu'u Maka'ala Natural Area Reserve (PUUM) produced by applying the standard ONEFlux (1F) software. Site Description - NEON's PUUM field site is located in the Pu'u Maka'ala Natural Area Reserve (NAR) on the eastern side of Hawaii’s “Big Island,” managed by the Hawaii Division of Forestry and Wildlife (DOFAW). More than 18,000 acres in size, the NAR is home to a rainforest with many native species, some of them endangered. It was established to protect some of the Big Island’s best wet native forest and unique geologic features.

Network), NEON (National Ecological Observatory [N↗
DOE OSTI2020

NBL Pu CRM (Phase 1 Progress Report)

Several 100 μg aliquots of NBL CRM 137 Pu sulfate tetrahydrate were prepared in 20 mL glass vials at some time in the past and are expected to have similar chemical composition and similar concentrations of contaminants as the bulk 250 mg CRM 137 Pu sulfate tetrahydrate units. Thus, these units were characterized and used to test Pu purification chemistry to be employed on the larger unit. For preliminary characterization, the residue of bottle 6 was dissolved in 4 M HNO3/0.01 M HF and transferred quantitatively to a pre-weighed 30 mL Savillex Teflon vial with a total solution mass of approximately 18 g. A gravimetric aliquot was removed from this solution for characterization and the remaining solution was dried down and reconstituted in 8 M HNO 3 to test the anion exchange purification column.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2022

Modeling and evaluating 239 Pu and 235 U PFNS and average prompt-neutron multiplicity [Slides]

The following are currently in VIII.1 LANL and IAEA test files: 239 Pu nu-bar including CGMF modeling and CEA data, 239 Pu PFNS including Chi-Nu & CEA data, 239 Pu(n,f) cross section including fission TPC data. The following are currently being tested: 235 U nu-bar including CGMF modeling and 235 U PFNS including Chi-Nu data. Upcoming tasks include the correction of 235 U Chi-Nu PFNS at higher E inc , benchmarking 235 U PFNS and nu-bar evaluations, and getting 238 U nu-bar.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2022

Measurement of the 240 Pu(n,f) Prompt Fission Neutron Spectra with Chi-Nu

The DOE Nuclear Criticality Safety Program has funded a multi-year effort to measure the 240 Pu(n,f) Prompt Fission Neutron Spectrum at Chi-Nu. This project is a joint LANL-LLNL effort, involving the preparation of 12 240 Pu foils and construction of a Parallel-Plate Avalanche Counter at LLNL, with subsequent measurements of the 240 Pu(n,f) PFNS at the Chi-Nu beamline at the Los Alamos Neutron Science Center’s Weapons Neutron Research facility (LANSCE/WNR). We expect the PPAC to be ready in time to perform the measurements this run cycle.

240Pu Foils↗