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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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At least 181 records · Page 10

Enhanced Neutron and γ-Ray Detection via 6 Li Substitution in Undoped and Tl-Doped Zero-Dimensional Perovskite Cs 3 Cu 2 I 5 Scintillators

Radiation detectors are crucial in a wide variety of research and commercial applications, such as oil and gas exploration, medical imaging, nuclear nonproliferation, and homeland security. Neutron and gamma-ray detectors are fundamental components in portal monitors at ports and border crossings, bolstering national security against radiological threats. This study presents a dual-mode scintillator, undoped and Tl-doped 6 Li-Cs 3 Cu 2 I 5 , and demonstrates its potential as a promising material for simultaneous thermal neutron and gamma-ray detection. We explore the Bridgman growth of both undoped and thallium doped Li → Cu and Li → Cs substitutional systems with various Li doping levels and assess their impact on scintillation properties. Under 662 keV gamma-ray excitation, the undoped crystals had light yields up to 35,900 ph/MeV, with energy resolutions down to 4.5%. The Tl-doped crystals performed better than the undoped crystals with light yields peaking at 65,900 ph/MeV and energy resolutions as low as 3.5%. When exposed to a moderated 252 Cf excitation source, our crystals had light yields between 102,900 and 167,200 photons per thermal neutron capture, with a full energy thermal neutron peak reaching 3 MeV in gamma equivalent energy. Pulse shape discrimination studies reveal well-separated gamma and neutron events, resulting in Figure-Of-Merit (FOM) as high as 3.7. Furthermore, these findings highlight the potential of Li-doped Cs 3 Cu 2 I 5 as a viable candidate for next-generation dual-mode scintillators.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Quantitative Encapsulation and Homogeneity Assessment of Sol–Gel Based Nuclear Explosive Debris Simulants

Nuclear explosive debris simulants are an important material in training and validating aspects of post-detonation nuclear forensic processes. Realistic simulants should replicate several aspects of nuclear explosive debris such as the size, shape, color, density, and chemical and radiological properties. Silica particles produced via sol-gel synthesis have recently been found to successfully reproduce many of these parameters including the controllable incorporation of radionuclide content. However, to be useful as a benchmarking material for validation and verification of laboratory methodologies, radionuclide content from batch-to-batch must be reproducible. Here, in this work, we explore the variance in radionuclide distribution incorporated into sol-gel benchmarking materials with respect to sample subdivision. Results will help inform the sample sizes required to minimize variance between samples.

36 - MATERIALS SCIENCE↗

Automated Calibration for Rapid Optical Spectroscopy Sensor Development for Online Monitoring

An automated platform has been developed to assist researchers in the rapid development of optical spectroscopy sensors to quantify species from spectral data. This platform performs calibration and validation measurements simultaneously. Real-time, in situ monitoring of complex systems through optical spectroscopy has been shown to be a useful tool; however, building calibration models requires development time, which can be a limiting factor in the case of radiological or otherwise hazardous systems. While calibration time can be reduced through optimized design of experiments, this study approached the challenge differently through automation. The ATLAS (Automated Transient Learning for Applied Sensors) platform used pneumatic control of stock solutions to cycle flow profiles through desired calibration concentrations for multivariate model construction. Additionally, the transients between desired concentrations based on flow calculations were used as validation measurements to understand model predictive capabilities. This automated approach yielded an incredible 76% reduction in model development time and a 60% reduction in sample volume versus estimated manual sample preparation and static measurements. The ATLAS system was demonstrated on two systems: a three-lanthanide system with Pr/Nd/Ho representing a use case with significant overlap or interference between analyte signatures and an alternate system containing Pr/Nd/Ni to demonstrate a use case in which broad-band corrosion species signatures interfered with more distinct lanthanide absorbance profiles. Both systems resulted in strong model prediction performance (RMSEP < 9%). Lastly, ATLAS was demonstrated as a tool to simulate process monitoring scenarios (e.g., column separation) in which models can be further optimized to account for day-to-day changes as necessary (e.g., baseline correction). Ultimately, ATLAS offers a vital tool to rapidly screen monitoring methods, investigate sensor fusion, and explore more complex systems (i.e., larger numbers of species).

47 OTHER INSTRUMENTATION↗

Friends or Foes: Fundamental Principles of Th-Organic Scaffold Chemistry Using Zr-Analogs as a Guide

The fundamental interest in actinide chemistry, particularly for the development of thorium-based materials, is experiencing a renaissance owing to the recent and rapidly growing attention to fuel cycle reactors, radiological daughters for nuclear medicine, and efficient nuclear stockpile development. Herein, we uncover fundamental principles of thorium chemistry on the example of Th-based extended structures such as metal–organic frameworks in comparison with the discrete systems and zirconium extended analogs, demonstrating remarkable over two-and-half-year chemical stability of Th-based frameworks as a function of metal node connectivity, amount of defects, and conformational linker rigidity through comprehensive spectroscopic and crystallographic analysis as well as theoretical modeling. Despite exceptional chemical stability, we report the first example of studies focusing on the reactivity of the most chemically stable Th-based frameworks in comparison with the discrete Th-based systems such as metal–organic complexes and a cage, contrasting multicycle recyclability and selectivity (>97%) of the extended structures in comparison with the molecular compounds. Altogether, the presented work not only establishes the conceptual foundation for evaluating the capabilities of Th-based materials but also represents a milestone for their multifaceted future and foreshadows their potential to shape the next era of actinide chemistry.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Polyoxometalate-Assisted Crystallization: A General Strategy Enabling Structural Characterization of Molecular Radium Complexes

A fundamental understanding of radium (Ra) coordination chemistry has been hindered by the scarcity and radiological hazards of 226 Ra, leaving the structural characterization of molecular Ra complexes almost entirely unexplored. Here, we introduce a polyoxometalate (POM)-assisted crystallization strategy that enables single-crystal X-ray diffraction analysis of Ra–chelator complexes from microgram-scale samples. Employing the plenary Keggin anion [SiW 12 O 40 ] 4– , we isolated and structurally characterized Ra 2+ complexes of 18-crown-6 and the bis-picolinate macrocycle macropa, together with their Sr 2+ and Ba 2+ analogues. The resulting structures reveal systematic, size-dependent trends in coordination number and metal-donor distances across the alkaline earth series and provide the first direct experimental measurements of Ra–N and Ra–OCOO bond distances. Together, these results establish POM-assisted crystallization as a robust approach for obtaining solid-state structural information on Ra 2+ complexes of organic chelators, opening new opportunities to advance the coordination chemistry needed to fully realize radium’s potential in isotope production and targeted radiotherapy. More broadly, this approach expands the experimental toolkit available for studying scarce, highly radioactive elements accessible only in microgram quantities.

Anions↗

Actinide Elemental Ratios of Spent Nuclear Fuel Samples by Resonance Ionization Mass Spectrometry

While resonance ionization mass spectrometry (RIMS) has demonstrated utility in measuring isotopic compositions of elements in complex matrices without the need for chemical separation to remove isobaric interferences, it has had limited application in measuring elemental compositions. The ability to determine elemental compositions via an in situ method like RIMS would be an exceptional asset in spent nuclear fuel analysis, where they are important in assessing reactor histories and whose chemical separation presents a radiological hazard. However, quantitative elemental analysis by RIMS requires special considerations because each element is ionized by its own set of lasers tuned to element specific resonant ionization wavelengths. We present the first comprehensive study of measuring elemental ratios by RIMS in spent nuclear fuel. All actinides produced by neutron capture are enhanced significantly radially from the center to the edge of a fuel pellet. This edge effect is not readily accessible by conventional bulk measurements.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Investigating trends in actinide covalency and magnetism with 35/37 Cl SSNMR spectroscopy and first-principles calculations

Solid-state NMR (SSNMR) spectroscopy is a powerful technique for studying actinide chemistry but has been significantly limited due to the complex paramagnetism, and radiological hazards presented by these materials. Lanthanide and actinide salts often feature magnetic ordering and can be paramagnetic, ferromagnetic, or antiferromagnetic depending on temperature and electronic structure. Paramagnetic interactions can manifest in SSNMR both as secular spectral shifts and/or couplings as well as contributions from non-secular relaxation. Both effects can be directly measured with NMR and used to extrapolate rich chemical information such as coordination environments, bonding characteristics, local molecular dynamics, and correlation times. Typically, these studies are carried out on high-γ and highly abundant NMR-active isotopes (e.g., 1 H, 6/7 Li, 19 F, 23 Na, etc.) or on enriched rare isotopes (e.g., 2 H and 17 O), which can be expensive. Herein, we present a facile methodology to measure the 35/37 Cl electric-field gradient (EFG) and paramagnetic shift anisotropy (SA) tensor components using static wideline SSNMR measurements of LaCl 3 , NdCl 3 , UCl 3 , and UCl 4 . The static powder spectra were measured with both 35 Cl and 37 Cl SSNMR to increase the fidelity of the extracted tensor parameters. Variable temperature NMR of a select case confirms the Curie–Weiss paramagnetism. Relaxation measurements of both nuclei further corroborate observations owing to the paramagnetic relaxation enhancement and reveal simultaneous quadrupolar relaxation mechanisms. Density functional theory (DFT) calculations using Hubbard U corrections to the uranium valence orbitals show excellent agreement with experimental EFG tensor parameters and help describe the bonding characteristics in these lanthanide and actinide systems.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Using nuclear observations to improve climate research and GHG emission estimates – the NuClim project

Project NuClim (Nuclear observations to improve Climate research and GHG emission estimates) aims to use high-quality measurements of atmospheric radon activity concentration and ambient radioactivity to advance climate science and improve radiation protection and nuclear surveillance capabilities. It is supported by new metrological capabilities developed in the EMPIR project 19ENV01 traceRadon. This work reviews the scientific objectives of project NuClim in terms of both climate science and radiological protection, and provides an overview of the NuClim field campaign and the various nuclear measurements being implemented within the scope of the project.

54 ENVIRONMENTAL SCIENCES↗

Dry Deactivation of Sodium Metal in a Molten LiCl-KCl-CsCl-NaCl System

An experimental study was performed with the objective of investigating and characterizing a dry technique for deactivation of sodium metal in a molten salt system. The study was performed in three parts. First, proof-of-principle testing of the technique was performed at bench scale. It involved loading and melting tens of grams of clean sodium metal atop a pool of LiCl-KCl-CsCl eutectic at ∼300°C and then adding ammonium chloride particles while mixing. The ammonium chloride reacted with sodium to form sodium chloride and nitrogen/hydrogen off-gases. The sodium chloride assimilated into the salt pool, forming a quaternary salt mixture of LiCl-KCl-CsCl-NaCl. The proof-of-principle testing repeatedly exhibited complete deactivation of the loaded sodium metal. Second, characterization of a LiCl-KCl-CsCl-NaCl system was performed using differential scanning calorimetry to produce a partial phase diagram of LiCl-KCl-CsCl eutectic versus NaCl, which identified the liquidus, solidus, and two-phase regions of the quaternary system. Third, the dry deactivation technique was demonstrated at kg-scale in an inert atmosphere radiological glovebox with sodium metal that was previously separated in the same glovebox from uranium metal in unirradiated blanket elements for the Fermi-1 nuclear reactor. The quaternary salt product at the end of the demonstration was sampled and showed complete deactivation of the sodium metal. Here, in short, this study qualified a technique to completely deactivate batches of sodium metal in the absence of air or water. While this study focused on the deactivation of sodium metal, including bond sodium from unirradiated blanket elements, the technique is applicable to other sources of sodium metal, such as sodium metal from batteries. Furthermore, the technique could also be extended to other alkali metal systems, including lithium, sodium, potassium, rubidium, cesium, and mixtures thereof.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Species Transport Framework Development in SAM for System-Level Tritium Source Term Analysis

The SAM code is under development as a modern system-level modeling and simulation tool for advanced non–light water reactor safety analyses, with recent efforts to add capabilities to evaluate radiological source term risks in these novel reactor concepts. By leveraging the established system-level multiphysics thermal-hydraulic models in SAM, a framework for tightly coupled species transport modeling has been integrated into the code for engineering-scale source term evaluation. This species transport framework was first applied to the simulation of tritium, which is a well-known source term in conventional light water reactors. Tritium poses a unique risk in salt-cooled reactors, especially those with lithium-bearing salts such as the fluoride salt–cooled high-temperature reactor (FHR) concept, as tritium is generated in the salt coolant in significant quantities due to neutron interactions. A compounding factor is the increased mobility of tritium at high temperatures, which is able to permeate through metals while also potentially being retained in graphite pebbles and structures. Engineering-scale models for the tritium transport pathways in a FHR have been developed using the new species transport framework in SAM. The capabilities are assessed through analytical verification problems and validated with data from a graphite retention experiment. In conclusion, the system-level model is demonstrated by performing an initial estimate of baseline tritium generation and flows in a generic reference SAM FHR model, setting a foundation for future studies of source term transient analysis with the potential for further multiscale and multiphysics integration.

SAM↗

Mass Optimization of a Multilayered Shield for Transportable Microreactors

The ability to easily transport microreactors is a major selling point for deploying microreactors to remote areas. However, this creates a unique shielding challenge, especially when the microreactor is being shipped after irradiation. A traditional reactor configuration utilizes a separate biological shield and pressure vessel to meet radiological shielding and pressure needs. The limited space available for transportable microreactors for both shielding and pressure vessels requires a revised assessment of separating out the biological shield and pressure vessel. To address these concerns, we examine a nuclear-grade sandwich composite (NGSC) that combines the reactor pressure vessel and biological shielding functions into a single component. Through a series of optimization problems for both transportation and operational use cases, the NGSC is able to minimize dose, minimize the vessel cost, and ensure that weight requirements are met for transportation. Initial results show that using a tungsten-tetraboride cermet in the first two layers of a six-layer NGSC provides adequate shielding for both use cases. These results show promise that an NGSC has enough overlap between operational and transportation cases to help reduce the design space for future analysis and assessment.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Investigating the Role of Accident Tolerant Cladding on Source Term Reduction for High-Burnup PWRs Using MELCOR

The use of accident tolerant fuel (ATF) cladding can increase coping times during and beyond design basis accidents. While such gains may be incremental, they provide a margin that can potentially be recovered to enable high-burnup (HBU) operation. Realizing such a margin requires demonstrating that the combination of HBU and ATF has not led to an overall increase in source term. This study investigates the influence of cladding technology (Zr-based, Cr-coated Zr, and FeCrAl) and fuel cycle length (18 and 24 months) on radiological dose at the boundary of the exclusion zone for a four-loop pressurized water reactor to investigate whether ATF claddings can provide such benefits. We analyze a recovered large break loss-of-coolant accident scenario to investigate the impact of transient timescale on the benefits of such coping time increases. The simulations have been performed using the MELCOR and MELCOR Accident Consequence Code System codes. For the cases analyzed, increased fuel cycle length did not necessarily increase radionuclide release and hydrogen generation, as these were found to be sensitive to the core power distribution. Similarly, off-site dose consequence is dominated by short-lived radionuclides that tend to saturate earlier in the burnup, so higher burnup operation did not necessarily increase the source term for the phenomena and transients analyzed here. Delays in recovery of the lowpressure safety injection system increase hydrogen production and radionuclide release, especially between 780 s and 1620 s, due to the nonlinear oxidation and core degradation behavior. Results show that Cr-coated Zr enhances safety by delaying heatup and gap release. Here, when uncertainty propagation on oxidation properties is considered, FeCrAl exhibits the lowest overall radionuclide release and off-site dose throughout the spectrum. However, while the considered “base model” performance is superior under delayed injection scenarios, upper-bound cases display hydrogen generation risk comparable to the Zr-based cladding.

Accident Tolerant Fuel↗

Loading Capacity and Dilute Nitric Acid Rinse of Diglycolamide Resin for the Recovery of Transplutonium and Rare Earth Elements from Mark-18A Targets

N,N,N′,N′-tetraoctyldiglycolamide (TODGA) as a resin (“DGA resin”) produced by Eichrom Technologies will be used by Savannah River National Laboratory for the indiscriminate extraction of trivalent actinides and rare earth elements with the intent of recovering Cm and Am from dissolved irradiated 242 Pu Mark-18A targets in 7 to 9 M nitric acid. The extracted constituents will be recovered as an oxide by direct thermal decomposition of the loaded resin followed by calcination of the resultant residue. The characteristics of DGA resin with non-radiological feed simulant representative of the anticipated feed in the Mark-18A process, with Sm and Nd as surrogates for Cm and Am, respectively, including breakthrough point and saturation capacity were evaluated in this work. Additionally, this work examined the losses from the loaded resin by rinsing the resin bed with dilute acid to reduce the nitrate concentration in the resin bed prior to thermal decomposition operations to improve the safety posture of the process. A resin loading profile was developed, and the resin was determined to have a trivalent metal saturation capacity of 74 μmol/mL resin under the experimental conditions evaluated. Following a wash of the loaded resin bed with fresh 8 M HNO 3 , the trivalent metals retained was reduced to 68 μmol/mL resin, which represents the practical capacity of the resin for the Mark-18A process. Lighter lanthanides breakthrough the resin well before the saturation capacity is reached. Rinsing the saturated resin bed with 0.26 M HNO 3 was found to result in a rapid reduction in retention of rare earth elements by the resin. After 2.8 bed volumes of dilute acid rinse, the mean resin bed free acid concentration was reduced to 0.28 M and 3.1 bed volumes of dilute acid rinse resulted in a reduction of the cumulative rare earth element retention to 52 μmol/mL of resin.

Transplutonium separations↗

Emergency Radiation Dose Rate Monitoring During Prolonged Armed Conflict

The 2022 Russian full-scale invasion of Ukraine has introduced unprecedented challenges for the nuclear power generation and radiological safety communities, including occupation and disturbance of highly-contaminated areas, occupation of a nuclear power plant, and strikes near and within boundaries of nuclear sites. The war has necessitated the implementation of a supplementary dose rate sensor network to provide resilient measurement data for public protection and leadership awareness. This paper discusses the implementation of such a system, the factors determining what equipment is best suited for the purpose, and practical factors regarding deployment of the system and data management. The crucial factors for operating a supplementary dose rate sensing network are backup power and communications options for dose rate sensors to make the network resilient to the effects of military operations. The most important implementation factor is to plan for extended operations beyond those typically considered for emergency response given the unpredictable nature of warfare.

resilience↗

Technological developments and accelerator improvements for the FRIB beam power ramp-up

The Facility for Rare Isotope Beams (FRIB) began operation with 1 kW beam power for scientific users in May 2022 upon completion of 8 years of project construction. The ramp-up to the ultimate beam power of 400 kW, planned over a 6-year period, will enable the facility to reach its full potential for scientific discovery in isotope science and applications. In December 2023, a record-high beam power of 10.4 kW uranium was delivered to the target. Technological developments and accelerator improvements are being made over the entire facility and are key to completion of the power ramp-up. Major technological developments entail the phased deployment of high-power beam-intercepting systems, including the charge strippers, the charge selection systems, the production target, and the beam dump, along with support systems, including non-conventional utilities (NCU) and remote handling facilities. Major accelerator improvements include renovations to aging legacy systems associated with experimental beam lines and system automation for improved operational efficiency and better machine availability. Experience must be gained to safely handle the increased radiological impacts associated with high beam power; extensive machine studies and advanced beam tuning procedures are needed to minimize uncontrolled beam losses for the desired operating conditions. This paper discusses the technological developments and accelerator improvements with emphasis on major R&D efforts.

43 PARTICLE ACCELERATORS↗

A Review of the Resuspension of Radioactively Contaminated Particles by Vehicle and Pedestrian Traffic—Current Theory, Practice, Gaps, and Needs

Here, the resuspension of radioactively contaminated particles in a built environment, such as from urban surfaces like foliage, building exteriors, and roadways, is described empirically by current plume and dosimetry models used for hazard assessment and long-term risk purposes. When applying these models to radiological contamination emergencies affecting urban areas, the accuracy of the results for recent contamination deposition is impacted in two main ways. First, the data supporting the underlying resuspension equations was acquired for open, quiescent conditions with no vehicle traffic or human activities, so it is not necessarily representative of the urban environment. Second, mechanical disturbance by winds in urban canyons and during emergency operations caused by vehicle traffic and human activities are not directly considered by the equations. Accordingly, plume and dosimetry models allow the user to input certain compensating values, but the models do not necessarily supply users instructions on what values to use. This manuscript reviews the available literature to comprehensively and consistently pool data for resuspension due to mechanically induced resuspension applicable to urban contamination. Because there are few studies that directly measured radioactive resuspension due to vehicles and pedestrians, this review novelly draws on a range of other studies involving non-radioactive particles, ranging from outdoor air pollution emissions to indoor allergen transport. The results lead to tabulated, recommended values for specific conditions in the emergency phase to help users of plume and dosimetry models maintain the conservativeness needed to properly capture the potential radiation dose posed by mechanically induced resuspension. These values are of benefit to model users until better data are available. The results also suggest the types of data that may result in improved plume and dose modeling.

61 RADIATION PROTECTION AND DOSIMETRY↗

Conversion of Site-Specific Meteorological Data for use in CAP-88 PC

CAP-88 PC is a commonly used radiological atmospheric dispersion model. This US EPA-approved model is used to demonstrate compliance with atmospheric emission regulations for radionuclides. While the model includes a large library of meteorological data for use across the United States, there are applications when users may wish to use onsite meteorological data as an input to the CAP-88 PC model. Here, in this work, we present a work-around process for preparing and converting onsite data for use in CAP-88 PC. However, the use of local data should provide a more realistic estimate of doses to members of the public in the immediate vicinity of a facility, although the regulatory agency having jurisdiction may not accept the use of local data for compliance. Additionally, the historical meteorological records from 20+ years ago (at a site many kilometers away) might not be representative of current local weather patterns, highlighting another benefit of using local meteorological data.

54 ENVIRONMENTAL SCIENCES↗

Distribution of Natural Radionuclides at the Nevada National Security Site

According to the United Nations Scientific Committee on the Effects of Atomic Radiation (UNSCEAR) publications, contributions of terrestrial gamma doses are mainly from the presence of 40 K, and of 238 U and 232 Th together with their progeny in various rocks and soils. A survey of soil distributions of radionuclides 40 K, 238 U, and 232 Th was performed at the Nevada National Security Site (NNSS) using in situ gamma-ray spectrometry with a high-purity germanium (HPGe) detector. The average activity concentrations of 40 K, 238 U, and 232 Th in natural soils at the NNSS are 867 Bq kg -1 (range from 150 ± 8 to 1297 ± 56 Bq kg -1 ), 50 Bq kg -1 (range from 29 ± 3 to 74 ± 8 Bq kg -1 ), and 56 Bq kg -1 (range from 11 ± 2 to 96 ± 10 Bq kg -1 ), respectively. The concentration at each location is significantly associated with its geological lithology. The terrestrial gamma dose rates around the NNSS were estimated from 26 to 144 nSv h -1 with mean value of 93 nSv h -1 . In conclusion, our results provide useful information about the natural background radiation and radiological effects of naturally occurring radionuclides at the NNSS.

environmental assessment↗