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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↗

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↗

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↗

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↗

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↗