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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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8 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

How novel is protactinium: Insights into the structure and properties of (PaO) 2 (SO 4 ) 3 (H 2 O) 2

Because of the scarcity of protactinium and the challenges associated with its separation and crystallization, even in sulfuric acid media where protactinium is relatively stable, there has been an incomplete understanding of the structural features of protactinium complexes. The characterization of protactinium sulfate complexes has been limited to those in solution, which have left key details unaddressed since the 1960s. This report describes a synthetic strategy to crystallize a protactinium complex using boric acid and sulfuric acid. Herein, the authors detail the results of hydrothermal synthesis and the single-crystal analysis of a novel protactinium sulfate complex, (PaO) 2 (SO 4 ) 3 (H 2 O) 2 . This work has elucidated structural features, providing groundwork for accurate computational analysis and clarifying previously unknown details on the coordination, denticity, and binding properties of protactinium sulfate complexes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS2021

On the Cycling of 231 Pa and 230 Th in Benthic Nepheloid Layers

The naturally-occurring radionuclides protactinium-231 ( 231 Pa) and thorium-230 ( 230 Th) are produced at approximately uniform rates in the ocean and thought to be removed from the water column through a reversible exchange with settling particles. Recent measurements along the U.S. GEOTRACES North Atlantic transect (GA03) revealed two features which are at odds with current understanding about 231 Pa and 230 Th cycling in the ocean: (i) a sharp decrease in dissolved 231 Pa ( 231 Pa d ) and 230 Th ( 230 Th d ) activities with depth below 2000-4000 m and (ii) very high particulate 231 Pa ( 231 Pa p ) and 230 Th ( 230 Th p ) activities near the bottom, at a number of stations between the New England continental shelf and Bermuda. Concomitant measurements of light attenuation from beam transmissometry showed that both features occur in benthic nepheloid layers (BNLs), which suggests that these features may stem, at least partly, from the presence of resuspended sediment in the deep water column. Here we explore the behaviour of 231 Pa and 230 Th in BNLs by using (i) radionuclide, optical, and hydrographic data from the western segment of GA03 (west of Bermuda) and (ii) a simplified model of particle and radionuclide cycling that includes a lateral particle source. First, the BNLs observed at GA03 stations are characterized from measurements of the beam attenuation coefficient converted to particle concentrations. At all stations, particle concentrations below the clear water minimum were the highest in the bottom mixed layer, whose thickness ranged from 95 to 320 m, and decreased generally with height above the bottom. The thickness of strong BNLs varied from 482 to 1358 m and the vertical integral of particle concentration in excess to that at the clear water minimum varied from 1 x 10 4 to 2 x 10 6 mg m −2 , among different stations. Second, the particle-radionuclide model is fitted to data from stations GT11-04 (New England continental rise) and GT11-08 (Hatteras abyssal plain), where samples for radionuclide analyses were collected in the BNL. The model can reproduce simultaneously the increase of particle concentration with depth, the low 231 Pa d and 230 Th d in the BNLs, and the high 231 Pa p and 230 Th p near the bottom. According to the model, at heights less than about 300 m above the seafloor, the dissolved phase was set primarily by a balance between adsorption and desorption, with vertical turbulent mixing playing a secondary role, whilst the particulate phase behaved largely as a non-reactive constituent supplied laterally and transported vertically by particle settling and turbulent mixing. Sensitivity tests with the model suggest that lateral particle sources near continental slopes and similar reliefs can produce significant biases both in the 230 Th normalization method and in the interpretation of sediment 231 Pa/ 230 Th records. Our findings yield insights into the influence of sediment resuspension and transport on 231 Pa and 230 Th in the deep ocean and highlight the need for considering these processes in paleoceanographic applications.

Nepheloid layer↗
DOE OSTI2026

Measurement of low energy characteristic X-rays emitted present in U-10Mo HALEU alloy fuel

Advance high density monolithic alloy HALEU fuels have been scanned with a silicon drift detector scanning system to measure low-energy characteristic X-rays emitted by uranium daughters, as well as zirconium present as a foil diffusion barrier. Four peaks were measured across the surfaces of three plates, and are consistent with other thorium and protactinium peaks present in depleted uranium samples that are induced by the decay of 235 U and 238 U. Of the four peaks detected, three are dominated by the decay of 235 U, and one peak at 15.70 keV covers two characteristic X-rays from the zirconium diffusion barrier (Kα 1 ) and from a 231 Th 15.62 keV X-ray induced by 235 U α-decay. The low energies of these lines suggest that they are mostly emitted from the fuel meat surface, and the poor counting statistics caused by strong self-attenuation make these data a poor candidate for 235 U/ 238 U ratio analysis. We suggest, then, that these X-rays could be used for passive measurement of variations in the cladding thickness of these fuels to complement manual thickness measurement methods.

HALEU↗
DOE OSTI2024

Evaluation of material accountancy techniques for 233 Pa from thorium nuclear fuels

Thorium is a promising alternative to uranium as nuclear fuel with advantages such as higher abundance, lower production of long-lived transuranic elements, and potentially better proliferation resistance. However, thorium presents a potential pathway for proliferation where produced 233 Pa can be diverted for the clandestine production of safeguarded 233 U. To prevent this, the ability to detect and measure 233 Pa must be assessed. This paper reviews several nuclear material accountancy techniques to determine their suitability for detecting 233 Pa extracted from irradiated thorium fuel. Hybrid K-edge densitometry and passive gamma spectroscopy have been found to be the best options based on technology maturity, cost, accuracy, and acquisition time. Thorium can be used in various reactor designs such as pressurized water reactors (PWRs), Canada deuterium uranium (CANDU) reactors, and molten salt reactors (MSRs). Therefore, thorium-uranium oxide fueling was modeled for three representative reactors (PWR, CANDU, MSR), burning the fuel to 47 GWd/MTHM for PWR, 19 GWd/MTHM for CANDU, and at a steady power of 52.711 MW/MTHM for MSR. Within each model, the protactinium element in the used fuel was extracted and its isotopic content analyzed. Simulated results indicated that 233 Pa can be detected using passive gamma spectroscopy in each fuel type at all decay times (0–300 days) following separation.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
NASA NTRS2019

A Model Study of the Relative Influences of Scavenging and Circulation on 230Th and 231Pa in the Western North Atlantic

The oceanic cycles of thorium-230 and protactinium-231 are affected by a number of processes, such as removal by adsorption to settling particles and transport by ocean currents. Measurements obtained as part of GEOTRACES and earlier programs have shown that, in the North Atlantic, the activities of dissolved 230Th (230Thd) and 231Pa (231Pad) at abyssal depths are lower near the western margin than in the basin interior. At least two factors could explain the lower 230Thd and 231Pad near the margin: (i) intensified scavenging in benthic nepheloid layers (BNLs) extending a thousand meters or more above the seafloor; and (ii) ventilation by relatively 230Thd- and 231Pad-poor waters emanating from the Deep Western Boundary Current (DWBC).Here a regional ocean circulation model with ?eddy-permitting' resolution (1/4) that incorporates 230Th and 231Pa is used in an effort to reproduce the observed distributions of 230Th and 231Pa in the western North Atlantic. In this model, 230Th and 231Pa removal from solution is governed by a prescribed distribution of particulate matter that is derived from a recent synthesis of nephelometer and transmissometer data. The model simulates a meandering Gulf Stream and a DWBC along the continental slope and rise, although noticeable differences with physical observations also exist. A model solution is found that explains most of the variance of 230Thd measurements (85%) and 231Pad measurements (81%) from (pre-)GEOTRACES cruises. On the other hand, measurements of particulate 230Th (230Thp) and 231Pa (231Pap) are more difficult to reproduce, with the same solution accounting for only 49% (11%) of the 230Thp (231Pap) variance. Sensitivity experiments suggest that the low 230Thd and 231Pad activities observed near the western margin are due to enhanced removal rates of both nuclides in BNLs rather than to deep water ventilation from the western boundary. The radionuclide activities present in the DWBC at its inflow location are also found to strongly influence the basin-scale distributions of 230Th and 231Pa. Overall, our study points to BNLs as important sites of 230Th and 231Pa scavenging in the ocean and illustrates the difficulty to explain simultaneously radionuclide measurements in dissolved and particulate forms in the studied area.

Lerner, Paul↗
NASA NTRSDate not supplied

Influence of sediment resuspension on deep-ocean Pa-231 and Th-230 cycling: A PROGRESS REPORT

The naturally-occurring particle-reactive radionuclides protactinium-231 (231Pa) and thorium-230 (230Th) are used as tracers of a variety of oceanic processes, both at present and in the past. Most notably, the sediment 231Pa/230Th ratio has been used to infer changes in the Atlantic Meridional Overturning Circulation over the last (de)glaciation. However, recent measurements along the U.S. GEOTRACES North Atlantic transect (GA03) revealed two features which are at odds with current understanding about 231Pa and 230Th behaviour in the ocean: (i) a sharp decrease in dissolved 231Pa and 230Th activities with depth below 2000-4000 m and (ii) very large particulate 231Pa and 230Th activities near the bottom, at a number of stations between the New England continental shelf and Bermuda. Concomitant measurements of particulate matter concentration and potential temperature showed that both features are associated with the benthic nepheloid layer (BNL) and the bottom mixed layer (BML) that are present at these stations. Here we develop and apply a simplified model of the exchange of particles, 231Pa, and 230Th between the BNL and the upper sediment, to explore the extent to which the radionuclide anomalies observed near the bottom at a number of GA03 stations can be explained by local sediment resuspension. We find that the model can broadly reproduce the observed anomalies at two stations where samples for radionuclide analyses were collected near the seafloor. Sensitivity tests with the model show that the 231Pa/230Th ratio of particles in the BML and the sediment varies by a factor of 3 as the sediment resuspension rate fluctuates within a range consistent with observational estimates. The modelled variability is comparable to the spatial variability of 231Pa/230Th of suspended particles in the modern North Atlantic and to the variability of Atlantic sediment 231Pa/230Th records across the last (de)glacial period. Two factors are found to contribute to the modelled sensitivity of the sediment 231Pa/230Th to sediment resuspension rate: the vertical turbulent mixing in the BML and the differential scavenging intensity of Pa and Th due to variation in particle concentration. Overall, our study indicates that the exchange of material between the BNL and the upper sediment can affect the particulate 231Pa/230Th ratio in the bottom water and the sediment, which may complicate the use of sediment 231Pa/230Th as a palaeoceanographic tracer.

particle-reactive radionuclides↗
DOE OSTI2024

Updated uranium reference material 231 Pa/ 235 U consensus model ages for nuclear forensics

Radiochronometry provides the model age of nuclear materials, which is useful for understanding the production history of materials found outside of regulatory control. Certified reference materials (CRMs) are important for radiochronometry to increase confidence in measurement quality; however, the absence of 231 Pa/ 235 U CRMs necessitates that nuclear forensic laboratories measure the 231 Pa/ 235 U model ages of preexisting uranium reference materials. Here, in this work, new consensus 231 Pa/ 235 U model ages are reported from three nuclear forensic laboratories for three reference materials using current analytical methods. These updated consensus values can be used for quality control of 231 Pa/ 235 U model age measurements.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2025

Model ages of three uranium metal CRMs and implications for radiochronometry data interpretation

In this study, we report 230 Th/ 234 U and 231 Pa/ 235 U model ages in three uranium metal certified reference materials with distinct production histories and isotopic compositions ranging from depleted to highly enriched (CRMs 112-A, 115, and 116-A). Here, our results provide the first model age values for these materials using multiple radiochronometers, which can be used as reference values for quality control of radiochronometry measurements performed during nuclear forensic investigations. Furthermore, we evaluate the model ages in the context of available production records for the materials, which provides insight into the processes that may impact radiochronometry systems during uranium metal production.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗