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At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Separation of protactinium from uranium-niobium alloys for 231 Pa– 235 U radiochronometry in nuclear forensic investigations

The isolation and purification of protactinium from uranium materials is essential for 231 Pa– 235 U radiochronometry, but separating Pa from uranium-niobium alloys, a common material in the nuclear fuel cycle, is challenging due to the chemical similarity of Pa and Nb. Here, in this work, we present three resin chromatography separation techniques for isolating Pa from U and Nb which were independently developed by three different laboratories through ad hoc adaptations of standard operating procedures. Our results underscore the need for and value of purification methods suitable for a diversity of uranium-based materials to ensure the operational readiness of nuclear forensics laboratories.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

Radiochronometry in the CMX-4 Exercise-Draft

In a recent international exercise, 10 international nuclear forensics laboratories successfully performed radiochronometry on 3 low-enriched uranium oxide samples, providing 12 analytical results using 3 different parent-daughter pairs serving as independent chronometers. The vast majority of the results were consistent with one another and consistent with the known processing history of the materials. In general, for these particular samples, mass spectrometry gave more accurate and more precise analytical results than decay counting measurements. In addition, the concordance of the 235 U- 231 Pa and 234 U- 230 Th chronometers confirmed the validity of the age dating assumption, increasing our confidence in the resulting conclusions.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2016

On the role of fusion neutron source with thorium blanket in forming the nuclide composition of the nuclear fuel cycle of the Russian Federation

The possible role of available thorium resources of the Russian Federation in utilization of thorium in the closed (U–Pu)-fuel cycle of nuclear power is considered. The efficiency of application of fusion neutron sources with thorium blanket for economical use of available thorium resources is demonstrated. The objective of this study is the search for a solution of such major tasks of nuclear power as reduction of the amount of front-end operations in the nuclear fuel cycle and enhancement of its protection against uncontrolled proliferation of fissile materials with the smallest possible alterations in the fuel cycle. The earlier results are analyzed, new information on the amount of thorium resources of the Russian Federation is used, and additional estimates are made. The following basic results obtained on the basis of the assumption of involving fusion reactors with Th-blanket in future nuclear power for generation of the light uranium fraction {sup 232+233+234}U and {sup 231}Pa are formulated. (1) The fuel cycle would shift from fissile {sup 235}U to {sup 233}U, which is more attractive for thermal power reactors. (2) The light uranium fraction is the most “protected” in the uranium fuel component, and being mixed with regenerated uranium, it would become reduced-enrichment uranium fuel, which would relieve the problem of nonproliferation of the fissile material. (3) The addition of {sup 231}Pa into the fuel would stabilize its neutron-multiplying properties, thus making it possible to implement a long fuel residence time and, as a consequence, increase the export potential of the whole nuclear power technology. (4) The available thorium resource in the vicinity of Krasnoufimsk is sufficient for operation of the large-scale nuclear power industry of the Russian Federation with an electric power of 70 GW for more than one quarter of a century. The general conclusion is that involvement of a small number of fusion reactors with Th-blanket in the future nuclear power industry of the Russian Federation would to a large extent solve its problems and increase its export potential.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2019

Minimization of Nuclear Waste using AHWR Reactor Technology

Nuclear sciences have grown from creating reactors to a greater understanding of how to dispose off the waste exhibited by the nuclear activities. Various methodologies have been proposed and are being used in order to do the same. This poster poses great attention to 'Using a fuel cycle dedicated to the production of the lower quantity of minor actinides, is one of the key targets in reducing nuclear waste in india'. A significant fraction of thorium is utilized as a fertile host in the Advanced Heavy Water Reactor (AHWR300-LEU) fuel. Being lower in the periodic table, it leads to a reduction of minor actinides. It produces only half of the minor actinides as a waste as compared to modern LWRs. As thorium oxide has inert nature, it benefits in its prolonged storage. Therefore, safe disposal of spent fuel is achieved due to the inert matrix, on completion of one fuel cycle mode. AHWR is a 300 MWe, vertical, pressure-tube type, boiling light water-cooled, and heavy water-moderated reactor. Employs natural circulation for removal of heat from the reactor core. In-situ conversion of {sup 232}Th into {sup 233}U. The reactor design permits flexible fuel cycle options. There are two types of AHWR depending upon the fuel cycle options. Uses thorium-based oxide fuels: two fuel cycle options. With the adoption of thorium fuel cycle, AHWR300-LEU produces less minor actinides. As compared to modern LWRSs, it produces almost 37% less amount of actinides for the same amount of energy production, which in turn minimizes the burden on waste disposal requirements. But, it is associated with radionuclides such as {sup 231}Pa (produced through absorption of one neutron and emission of two neutrons). Since, the reaction rate of (n,2n) reactions is very low in thermal neutron reactors, thus making the fuel cycle the favorable one. Thorium oxide (ThO{sub 2}) is chemically stable and is the highest oxidation state of thorium, therefore the inert nature of the matrix is advantageous for safe disposal of spent fuel in case of adoption of open fuel cycle mode and offers prolonged storage of spent fuel. The AHWR is thorium fueled Indian nuclear reactor that assimilates several new features with diminished environmental concern due to reduced waste generation. Since thorium fuel cycle produces less long lived nuclear waste, thus it can possibly bring the world cleaner and more sustainable nuclear energy. Currently, India being the only country with large scale research program of thorium nuclear power serves a platform for the development and demonstration of all technologies and advanced safety systems.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2016

Physical particularities of nuclear reactors using heavy moderators of neutrons

In nuclear reactors, thermal neutron spectra are formed using moderators with small atomic weights. For fast reactors, inserting such moderators in the core may create problems since they efficiently decelerate the neutrons. In order to form an intermediate neutron spectrum, it is preferable to employ neutron moderators with sufficiently large atomic weights, using {sup 233}U as a fissile nuclide and {sup 232}Th and {sup 231}Pa as fertile ones. The aim of the work is to investigate the properties of heavy neutron moderators and to assess their advantages. The analysis employs the JENDL-4.0 nuclear data library and the SCALE program package for simulating the variation of fuel composition caused by irradiation in the reactor. The following main results are obtained. By using heavy moderators with small neutron moderation steps, one is able to (1) increase the rate of resonance capture, so that the amount of fertile material in the fuel may be reduced while maintaining the breeding factor of the core; (2) use the vacant space for improving the fuel-element properties by adding inert, strong, and thermally conductive materials and by implementing dispersive fuel elements in which the fissile material is self-replenished and neutron multiplication remains stable during the process of fuel burnup; and (3) employ mixtures of different fertile materials with resonance capture cross sections in order to increase the resonance-lattice density and the probability of resonance neutron capture leading to formation of fissile material. The general conclusion is that, by forming an intermediate neutron spectrum with heavy neutron moderators, one can use the fuel more efficiently and improve nuclear safety.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2016

Nuclear Data Sheets for A = 227

The evaluated spectroscopic data are presented for ten known nuclides of mass 227 (Po, At, Rn, Fr, Ra, Ac, Th, Pa, U, Np). For {sup 227}Po, {sup 227}At, {sup 227}Rn, {sup 227}Pa, {sup 227}U and {sup 227}Np nuclei, only the ground-state information is available. Their decay characteristics are mostly unknown. Levels in {sup 227}Fr are known only from the decay of {sup 227}Rn to {sup 227}Fr. This decay scheme at present cannot be normalized to deduce γ intensities per 100 decays due to lack of knowledge about multipolarities of many low-energy transitions. The levels in {sup 227}Ra, {sup 227}Ac and {sup 227}Th are known from several decays and reactions, including particle-transfer data for {sup 227}Ra and {sup 227}Ac. The decay scheme of {sup 227}Ra to {sup 227}Ac was last studied in 1971 using small Ge detectors. Improved γ-ray intensity data need to be obtained with a better γ-detection system. The datasets for {sup 227}Ac have undergone extensive revisions, including detailed data for 231Pa α decay from 1986BaYK report, and single-proton transfer data from 1986MaYU thesis. High-spin (J>13/2 or so) structures are known only for 227Th. Level lifetime data are quite scarce for all the nuclides in this mass chain, thus limiting the knowledge of reduced transition probabilities. Band structures for {sup 227}Fr, {sup 227}Ra, {sup 227}Ac and {sup 227}Th are known in detail, together with evidence of weak octupole deformation and consequent parity-doublet structures. This evaluation was carried out as part of a joint IAEA-ICTP workshop for Nuclear Structure and Decay Data, organized and hosted by the IAEA, Vienna and ICTP, Trieste, March 24–28, 2014. The evaluation work was coordinated by B. Singh (McMaster). This work supersedes previous A=227 evaluation (2001Br31) published by E. Browne which covered literature before May 2001.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2016

Pursuing Cost Effective Tank Waste Characterization at the Savannah River Site - 16172

The U. S. Department of Energy Office of Environmental Management has tasked the Savannah River National Laboratory (SRNL) with developing strategies and technologies to understand, optimize, scale, and speed up tank waste characterization. This scope is part of a multi-year project with the end goal of implementing programmatic changes that accelerate tank waste processing and tank closure schedules, and at the same time reduce characterization costs, while maintaining data integrity. The project is currently in its second year. During the first year of the project, SRNL completed a series of activities focused on understanding the range of current characterization practices, needs, gaps, risks, and potential alternative approaches. Based on the results, conclusions were drawn regarding aspects of the programs that are most costly and time consuming; particular waste constituents that drive costs, schedule, and program risks; alternative characterization approaches (other than sampling and analysis) that are less expensive and more rapid; new laboratory methods holding the greatest promise for reducing characterization costs and schedule; and in whole, the primary areas where current characterization practices can be improved. SRNL's current scope is focusing on three primary activities: 1) development of a technical basis/strategy for improving the cost effectiveness and schedule of SRNL's tank closure characterization program; 2) design/assembly of hardware, plumbing, and software for automating select radiochemical separation and waste removal processes; and 3) development and testing of alternative radiochemical separation protocols most likely to improve high resource demand/time consuming analysis methods (such as Ra-226, Pa-231, Tc-99/I-129, and/or Y/trivalent actinide separations). (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2019

A Method for Understanding the Behaviour of Radioactive Decay Chains in Radiological Assessments - 19382

In many radiological groundwater pathway assessments, especially those where the assessment timescales of interest are relatively short (say a few thousand years or less), contributions to effective dose or radiological risk are dominated by radionuclides such as C-14, Cl-36 or I-129. Over longer timescales, additional radionuclides can also become key contributors to risk. In particular, members of the U-238 decay chain, notably Ra-226 and Pb-210, are likely to be key radionuclides. Other decay chains that can contribute significantly to dose or risk at times far into the future include Np-237 → U-233 → Th-229 and U-235 → Pa-231 → Ac-227. In this paper, a method is described for understanding decay chain behaviour in radiological assessments. The method uses a graphical approach in which the various modes of transport and decay in a system of connected compartments are represented as pathways between two nodes in a two-dimensional grid. Each pathway corresponds to a distinct transport and decay process. By so doing, the different transport and decay processes can be identified in a systematic way. The result is an algorithm for generating the contributions to effective dose or radiological risk without explicit solution of the transport equations. The method has been tested against numerical models and analytic solutions and found to give excellent agreement, while at the same time providing information about decay chain behaviour that would be difficult to obtain from a numerical assessment model. The power of the method is illustrated by applying it to some examples based on real repository concepts. (authors)

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2019

Preparation and calibration of a 231 Pa reference material

A 231 Pa reference material has been characterized for amount of protactinium. This reference material is primarily intended for calibration of 233 Pa tracers produced for 235 U– 231 Pa model age measurements associated with nuclear forensics and nuclear safeguards. Primary measurements for characterization were made by isotope dilution mass spectrometry of a purified 231 Pa solution using a 233 Pa isotopic spike. The spike was calibrated by allowing multiple aliquots of the 233 Pa spike solution to decay to 233 U and then measuring the ingrown 233 U by isotope dilution mass spectrometry using a certified uranium assay and isotopic standard as a reverse-spike. In conclusion, the new 231 Pa reference material will simplify calibration of the 233 Pa isotope dilution spikes, provide metrological traceability, and potentially reduce the overall measurement uncertainty of model ages.

231Pa↗
DOE OSTI2023

Uranium Processing Signatures for Nuclear Forensics (NA22 End of FY23 Report)

A vacuum induction melting (VIM) furnace was used to produce an ~120 kg depleted uranium (DU) rod in November 2021 from well characterized feedstock to investigate the separation of thorium (Th) and protactinium (Pa) from uranium (U) during U metal casting and quantify the behavior of the 230 Th/ 234 U and 231 Pa/ 235 U radiochronometry systems. This work suggested that while 234 Th, measured by gamma spectrometry, appears to segregate to the top and surface of the rod, the concentration of 230 Th determined by isotope dilution mass spectrometry (IDMS) in drill turnings from multiple locations in the rod, including the hot top, is relatively consistent. To evaluate whether Th is potentially enriched at only the very outer surface of the cast DU rod relative to the bulk material in the cast rod, thin surface samples were collected from the cast DU rod. Locations sampled included the inner diameter (ID) and outer diameter (OD) of the bottom of the casting and the ID, OD, and top face of the hot top (very top of the casting). The locations are shown in Figure 1. Four samples were taken from each location at different depths in the cast material. Each cut took approximately 0.03 – 0.05” off of the casting.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2023

A chromatography chemistry for purifying $\mathrm{Pa}$ from $\mathrm{U-Nb}$ metal alloys

Here we present a chromatography chemistry for purifying protactinium from uranium metal alloys containing weight-percent concentrations of niobium. Niobium is precipitated in 9 M HCl without the co-precipitation of Pa as demonstrated by gamma-ray spectrometry. Protactinium is further purified using Bio-Rad™ anion resin AG® 1-X8 and 9 M HCl + 0.0128 M HF. A Pa/Nb separation factor of 85,000 and a 90% Pa recovery is demonstrated, which is amenable to 231 Pa concentration determination by isotope dilution and 231 Pa/ 235 U model age calculation for nuclear forensics.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2022

Real-Time Inventory Change Detection for the Protactinium Decay Inventory of the Molten Salt Breeder Reactor

This work presents a novel monitoring method for detecting material loss from the decay inventory of the molten salt breeder reactor (MSBR) by monitoring for changes to the system dynamics using an isotopic ratio. Here the isotopic masses in the decay inventory of a MSBR were simulated under several material loss scenarios. In each case, the ratio of 231 Pa to 233 Pa served as a sensitive and lasting indicator of material loss. This isotope ratio quickly decreased outside the normal range after a material loss, and the ratio remained depressed for several years after the loss. The dynamics of this ratio were driven by the periodic batch discard from the decay inventory every 220 days, which was specified in the MSBR design to periodically remove fission product buildup. For this method, isotopic ratios were found to be rapid and enduring indicators of inventory change if they comprise a pair with a short half-life (e.g., 233 Pa) and a long half-life (e.g., 231 Pa) relative to the effective half-life induced by the driving system process (e.g., the batch discard cycle). Using such an isotope pair enabled a method to monitor for changes to the effective half-life of the system and by extension changes to the system inputs and outputs.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
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 OSTI2020

An interlaboratory collaboration to determine consensus 231 Pa/ 235 U model ages of a uranium certified reference material for nuclear forensics

Application of the 231 Pa/ 235 U radiochronometer for nuclear forensic investigations is challenged by a lack of certified reference materials with 231 Pa/ 235 U model purification dates. The Japan Atomic Energy Agency, Los Alamos National Laboratory, and Lawrence Livermore National Laboratory completed an interlaboratory study measuring 231 Pa/ 235 U model ages of New Brunswick Laboratory CRM U100. Results from independent laboratories were combined to calculate a consensus 231 Pa/ 235 U model purification date for CRM U100 of March 26, 1959 ± 237 days. This 231 Pa/ 235 U consensus date for CRM U100 may be used by the nuclear forensic community for quality control of 231 Pa/ 235 U radiochronometry measurements of unknown materials.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2023

Results from a controlled depleted uranium metal casting experiment designed to investigate nuclear Forensic Radiochronometry Signatures

The accurate interpretation of uranium metal 230 Th/ 234 U and 231 Pa/ 235 U radiochronometry model ages requires an understanding of how uranium parent nuclides and decay progeny ( 230 Th and 231 Pa) behave during uranium metal casting. In order to directly measure the spatial distribution of 230 Th and 231 Pa in uranium metal before and after vacuum induction melting (VIM), Los Alamos National Laboratory identified uranium metal feedstock, characterized the metal feedstock, conducted a controlled casting experiment of an approximately 120 kg uranium metal rod, and characterized the cast metal. Herein this study presents radiochronometry results and quantified 230 Th and 231 Pa VIM separation factors from bulk uranium.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
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 OSTI2021

Transport model predictions of 225 Ac production cross sections via energetic p, d and α irradiation of 232 Th targets

Monte Carlo transport codes PHITS and MCNP6 were used to calculate the production cross sections of 225,227 Ac, 227,229 Th, 223,225 Ra, and 229,230,231 Pa via the bombardment of a 232 Th target with energetic protons, deuterons, and α-particles. The incident projectile energies ranged between 10 and 800 MeV/nucleon. When possible, the predicted production cross sections were compared with the available experimental data and other predictions. Here, the degree of the codes’ abilities to match the measured data provides a qualitative assessment of the codes’ abilities to predict data from similar, but unmeasured, projectile/target systems. In addition, a comparison between calculated cross sections and data may provide insight into possible improvements in the physics models employed by those transport codes.

223Ra↗
DOE OSTI2020

International cooperation in age-dating uranium standards for nuclear forensics using the 231 Pa/ 235 U radiochronometer

During 2017–2018 Los Alamos National Laboratory, Lawrence Livermore National Laboratory and the China Institute of Atomic Energy collaborated in an interlaboratory 231 Pa/ 235 U radiochronometry exercise. The laboratories used different analytical methods to obtain a consensus model purification date for CRM U010 of December 28, 1958 ± 198 days and for CRM U850 of May 20, 1958 ± 363 days. These results agree with previously reported model dates using the 230 Th/ 234 U radiochronometer as well as the production histories of these materials. The concordance of interlaboratory data here confirms the ability of laboratories to make reproducible radiochronometry measurements using distinct analytical approaches.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗