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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 1,027 records · Page 57
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

A new TEVA-DGA chromatography procedure to separate Pu, Am, and Np from bulk U materials

Trace actinides present within uranium (U) material are diagnostic signatures of U processing history. For example, the emplacement of U material within the high neutron-flux environment of a nuclear reactor can cause neutron capture of U to form 241-plutonium ( 241 Pu). Plutonium-241 then decays to progeny isotopes 241-americium ( 241 Am) and 237-neptunium ( 237 Np); therefore, the presence and relative abundances of these trace actinides is indicative of the material’s production history and intended employment (Mayer et al., 2013). During a pre-detonation nuclear forensics investigation, measurement of trace actinide 241 Pu, 241 Am, and 237 Np concentrations by an analytical laboratory may be requested. However, chemically purifying these elements from bulk U is a challenging and involved procedure requiring several sequential chromatography columns across 4+ days. To expedite Pu-Am-Np separation from bulk U material, and to improve the yield recovery of these elements, this DHS Postdoc Fellowship has worked to create a new chromatography separation chemistry.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2020

Unprecedented Radiation Resistant Thorium–Binaphthol Metal–Organic Framework

A thorium–organic framework (TOF-16) containing hexameric secondary building units connected by functionalized binaphthol linkers was synthesized, characterized, and irradiated to probe its radiation resistance. Radiation stability was examined using γ-rays and 5 MeV He 2+ ions to simulate α particles. γ-irradiation of TOF-16 to an unprecedented 4 MGy dose resulted in no apparent bulk structural damage visible by X-ray diffraction. To further probe radiation stability, we conducted the first He 2+ ion irradiation study of a metal–organic framework (MOF). Diffraction data indicate onset of crystallinity loss upon approximately 15 MGy of irradiation and total loss of crystallinity upon exposure to approximately 25 MGy of He 2+ ion irradiation. In conclusion, the high radiation resistance observed suggests MOFs can withstand radiation exposure at doses found in nuclear waste streams and highlights the need for a systematic approach to understand and eventually design frameworks with exceptional radiation resistance.

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

Impact of trivalent f-element complexation and chemical environment on the radiation-induced chemical reactivity of TODGA and HOPO ligands

Understanding the impact of ionizing radiation on ligands employed and proposed for the separation, recovery, and transport of actinide ions is of vital importance for the innovation of nuclear fuel cycle technologies. In the presence of ionizing radiation fields, complexing ligands are subject to radiolytic processes, that lead to their destruction and the formation of potentially detrimental degradation products. Consequently, mastery of the radiation-induced behavior of these ligands is essential for predicting and optimizing their effectiveness, longevity, and minimizing the negative impacts of radiolysis. Furthermore, this knowledge is critical for the design of more radiation resistant molecules to be incorporated into advanced separation technologies. That said, the radiation chemistry of most actinide complexants have only been studied in the absence of their targeted metal ion complexes, which can lead to inaccurate conclusions on their radiolytic robustness and impacts on performance. With this in mind, we present our findings on the impact of f-element complexation and chemical environment on the radiation-induced chemical reactivity of N,N,N',N'-tetraoctyl diglycolamide (TODGA) and the model octadentate hydroxypyridinone ligand 3,4,3-LI(1,2-HOPO) (abbreviated as HOPO), both promising candidates for actinide separations

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2020

EFRC Materials Science of Actinides (Final Report)

The Energy Frontier Research Center Materials Science of Actinides (MSA) conducted basic research from 2009-2019. The scientific personnel and participating institutes changed several times during the evolution of the Center, and in total included 24 senior investigators, four national laboratories, and ten universities. Workforce development was a motivating goal of the university-led Center, which included many undergraduate, graduate, and post-doctoral researchers. The center focused on the actinide elements, which arise from the sequential filling of the 5f electron orbitals. Although the specific themes evolved during the Center’s history, the final research themes were: (1) Nanoscale Cage Clusters, (2) Complex Ceramic and Metallic Materials, and (3) Materials Under Extreme Environments. To date, the Center has produced 254 peer-reviewed journal publications and book chapters that acknowledged only the EFRC funding, and an additional 161 journal publications and book chapters that acknowledged funding from the EFRC and additional sources (a few manuscripts are still in preparation). Broad highlights include: (1) Development of an extensive family of actinide nanomaterials that self-assemble in aqueous solution, an understanding of their formation mechanisms and stabilities, and possible uses in nuclear fuel cycles; (2) Establishment of facilities and methodologies to conduct high-temperature calorimetry on transuranium materials, and extensive thermodynamic-based studies of uranium and thorium compounds important to the nuclear fuel cycle; (3) A vastly improved understanding of the behavior of actinide materials in extreme conditions, including high radiation fields, temperatures, and pressures, as well coupled effects of two or more of these; (4) Development of resonance ultrasound spectroscopy and direct measurement of aging of plutonium alloys.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Cross sections and calculated yields of some radionuclides of yttrium, strontium and rubidium formed in proton-induced reactions on enriched strontium-86: possibility of production of 85g Sr, 83 Rb and 82m Rb in no-carrier-added form

Here, cross sections of the 86 Sr(p,3n) 84m Y, 86 Sr(p,αn) 82m Rb, and 86 Sr(p,x) 85g Sr reactions were measured from their respective thresholds up to 16.2 MeV and from 23.0 to 44.1 MeV at FZJ, and from 14.3 to 24.5 MeV at LBNL, using 96.4% enriched 86 SrCO 3 as target material. Thin targets prepared by sedimentation were irradiated with protons in a stacked-form, and the induced radioactivity was measured by high-resolution γ-ray spectrometry. Nuclear model calculations based on the code TALYS reproduced our experimental cross section data well. From the excitation functions, the integral yields of the above three radionuclides were calculated. The yield of 85g Sr via the natSr(n,γ) process was also measured using the TRIGA Mark-II reactor at AERE, Savar. A comparison of the reactor and cyclotron production of carrier-added 85g Sr is given. The production possibilities of the three investigated radionuclides in no-carrier-added forms at a 30 MeV cyclotron via new routes are discussed.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2020

Rapid Determination of Uranium Isotopic Abundance from Cotton Swipes: Direct Extraction via a Planar Surface Reader and Coupling to a Microplasma Ionization Source

The collection of solid particulates and liquids from surfaces by the use of cloth swipes is fairly ubiquitous. In such methods, there is a continuous concern regarding the ability to locate and quantitatively sample the analyte species from the material. In this effort, we demonstrate the initial coupling of an Advion Plate Express plate reader to a liquid sampling–atmospheric pressure glow discharge (LS-APGD) microplasma ionization source with an Orbitrap mass spectrometer to perform uranium isotopic analyses of solution residues on cotton swipes. The Plate Express employs a sampling probe head to engage and seal against the swipe surface. Subsequentially, the analyte residues are desorbed and transported within a 2% HNO 3 electrolyte flow to the ionization source. Quantitative recoveries were observed following a single 30 s extraction step, with the absolute mass sampled per extraction being ~100 ng. While the intrasample variability in the analytical responses for triplicate sampling of the same swipe yield ~30% RSD, this lack of precision is offset by the ability to determine isotope ratios for enriched uranium specimens with a precision of better than 10% RSD. Pooled, intersample precision ( n = 9) was found to be <5%RSD across the various sample compositions. Finally, 235 U/ 238 U determinations (ranging from 0.053 to 1.806) were accurate with errors of <10%, absolute. The 234 U- and 236 U-inclusive ratios were determined with similar accuracy in enriched samples. While the driving force for the effort is in the realm of nuclear nonproliferation efforts, the ubiquitous use of cloth swipes across many application areas could benefit from this convenient approach, including the use of versatile, reduced-format mass spectrometer systems.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2026

Experimental and Multiscale Modeling Insights for Radiation-Driven Neptunium Redox Processes at Elevated Temperatures

Studies of the radiation-driven reactions of actinide elements at elevated temperatures are extremely limited, but important given that radiation heating of used nuclear fuel can affect the radiolytically promoted actinide redox processes occurring in hydroprocessing environments. Under these conditions, the high concentration of nitric acid present makes the reaction of actinides, such as neptunium, with nitric acid radiolysis products significant. Therefore, here we present derivation of the rate coefficients for the reaction of pentavalent neptunium with the nitrate radical at elevated temperature, resulting in Eyring and Arrhenius parameters for this important reaction. Here, we also revisit our previously published multiscale model predictions for radiation-induced neptunium redox chemistry and present an iteration which successfully operates over a wider range of nitric acid concentrations, 0.1–6.0 M.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2021

Postclosure Inspection and Monitoring Report for Surface Corrective Action Unit 417 at the Central Nevada Test Area, Nevada, Site

This report presents results of the biennial postclosure site inspection conducted by the U.S. Department of Energy (DOE) Office of Legacy Management (LM) at the Central Nevada Test Area (CNTA), Nevada, Site (Figure 1) surface Corrective Action Unit (CAU) 417. The report has been prepared in accordance with the Post-Closure Monitoring Plan contained in the Closure Report for Corrective Action Unit 417: Central Nevada Test Area Surface, Nevada (NNSA/NV 2001), hereafter called the CAU 417 Closure Report. The site closure process was completed in 2001 in accordance with the amended Federal Facility Agreement and Consent Order (FFACO 1996, as amended) (FFACO) and all applicable Nevada Division of Environmental Protection (NDEP) policies and regulations. Responsibility for environmental site restoration was transferred from the DOE National Nuclear Security Administration Nevada Field Office to LM on October 1, 2006. This report summarizes investigation activities associated with CAU 417 that LM conducted from September 2018 through August 2020. A postclosure inspection was conducted in 2020 to document the physical condition of the CAU 417 soil covers, monuments, signs, fencing, and use-restricted areas.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2021

Imaging 192/193m Ir sources using digital autoradiography for nuclear forensic applications [Slides]

This work aims to develop a new methodology for assaying 192/193m Ir-containing materials. SDDs cannot determine activity spatially, thus it is important that the prepared samples are uniformly distributed. Autoradiography is used to image radioactive samples using imaging media by direct exposure. Using this technique, radio-iridium samples will be imaged to determine uniformity and self-attenuation as a function of mass.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2024

Radiochemical diagnostics at the National Ignition Facility

Since the National Ignition Facility (NIF) was commissioned in 2009, radiochemical techniques have been viewed as a potential method for diagnosing the performance of an NIF fusion shot. Radiochemical methods can also be used in conjunction with NIF shots to measure nuclear reaction cross sections in regimes that are inaccessible at accelerator facilities and can provide a route to produce radioactive tracer materials that can be used for other applications. Here, this review presents the current status of radiochemical diagnostics at the NIF. Experimental results and the status of both solid and gaseous debris collection radiochemistry are presented.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2020

Effects of chronic low-dose radiation on cataract prevalence and characterization in wild boar (Sus scrofa) from Fukushima, Japan

This study evaluated cataracts in wild boar exposed to chronic low-dose radiation. We examined wild boar from within and outside the Fukushima Exclusion Zone for nuclear, cortical, and posterior subcapsular (PSC) cataracts in vivo and photographically. Plausible upper-bound, lifetime radiation dose for each boar was estimated from radioactivity levels in each animal’s home range combined with tissue concentrations of 134+137Cesium. Fifteen exposed and twenty control boar were evaluated. There were no significant differences in overall prevalence or score for cortical or PSC cataracts between exposed and control animals. Nuclear (centrally located) cataracts were significantly more prevalent in exposed boar (p<0.05) and had statistically higher median scores. Plausible upper-bound, lifetime radiation dose ranged from 1 to 1,600 mGy in exposed animals, with no correlation between dose and cortical or PSC score. While radiation dose and nuclear score were positively associated, the impact of age could not be completely separated from the relationship. Additionally, the clinical significance of even the highest scoring nuclear cataract was negligible. Based on the population sampled, wild boar in the Fukushima Exclusion Zone do not have a significantly higher prevalence or risk of cortical or PSC cataracts compared to control animals.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2019

Understanding the Interactions of Seawater Ions with Amidoxime through X-Ray Crystallography

Insoluble polymer substrates functionalized with the amidoxime (R-C(NH 2 )=NOH) functional group have been demonstrated as a technically feasible platform for extracting uranium from seawater, a potential source of extremely abundant uranium for use as nuclear fuel. While it is possible to isolate macroscopic amounts of uranium from the ocean with a positive energy return on investment using these materials, both the economic and energetic costs are many times greater than those of terrestrial uranium mining. Currently, the major contribution to this cost is the production of the sorbent itself, so being able to recycle the sorbent even a small number of times will have a huge impact on lowering the cost of their use. However, amidoxime resins show capacity fading when stripped by strong acids, presently limiting their recyclability. Both alternative extractants and alternative elution chemistries are under development with promising results but are yet at too early a stage to make predictions about their ultimate success. Given the potentially huge impact of a successful recycling process on the viability of seawater extraction of uranium, there is a strong need to pursue additional routes to elution chemistry. During the course of this project, we studied the interactions of amidoxime-containing small molecules with the abundant metal ions in seawater, including Li, Na, K, Mg, Ca, Fe, Cu, and V, to understand the interactions of [UO 2 ] 2+ with amidoxime. By using small molecules with multiple adjacent functional groups, we crystallized the resulting metal complexes and used single crystal X-ray diffraction (SCXRD) as our primary tool for structural characterization. We also investigated the use of solutions of hydroxylammonium salts in weak acids as eluents for stripping and recycling amidoxime-based sorbents. The replacement of strong acids, which react with and destroy the amidoxime functional groups, with weak acids based on hydroxylammonium, a reagent that is actually used to make the amidoxime groups, is expected to avoid capacity loss on recycling and possibly even regenerate functionality that was lost due to exposure to the marine environment.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2022

Purification and Concentration of 99 Mo from a UREX raffinate

The medical isotope 99m Tc ( t ½ = 6.0 h) accounts for over 80% of isotopes used in diagnostic nuclear medicine today and is normally derived from its transient equilibrium parent 99 Mo ( t ½ = 66 h). To reduce U.S. dependence on 99 Mo derived from HEU by foreign suppliers, the NNSA/M3 program—under the American Medical Isotope Production Act—has been tasked with facilitating the work of domestic 99 Mo suppliers that do not utilize HEU. Superconducting electron linear accelerators with high-Z converter targets can generate bremsstrahlung photons and neutron fluxes that can induce photonuclear reactions and LEU fission. After sufficient production intervals, targets can be rotated out and processed while another batch is irradiated. The process flow chemistry is shown in Figure 1. The irradiated U 3 O 8 targets are retrieved and dissolved in HNO 3 ; the volatile fission products are expelled and captured during this step. The HNO 3 liquor bearing the uranyl, fission and activation products is injected into the UREX suite of liquid-liquid extraction banks. The uranyl is partitioned in typical fashion using tri-$\textit{n}$-butyl phosphate (TBP) in a hydrocarbon diluent. The raffinate—comprising mainly 99 Mo and fission products—is then injected into the MoLLE (Molybdenum Liquid-Liquid Extraction) flowsheet, where the Mo is selectively extracted by an organophosphorous acid extractant such as di-(2-ethylhexyl phosphoric acid) (HDEHP). Trace amounts of Nb, Zr, Np, I, and Te are co-extracted. The Mo is stripped using acetohydroxamic acid (AHA) and fed onto an anion exchange column. Following a series of hydroxide, HCl, and oxalic acid wash steps, the Mo can be recovered in NaOH/NaCl. A manuscript describing this process chemistry in more detail was recently published.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2024

A Road Map to Determine Chemical Phenomenology Required for Molten Salt Reactor Accident Modeling

The differences between molten salt reactors (MSRs) and light water reactors (LWRs) has required modification of previous approaches to model reactor accident progression. Part of this is related to the different chemical phenomenology of these reactors as their fuel is not as contained and can react with their surroundings. MELCOR is a reactor simulation tool that has implemented methods and models to model MSRs. However, additional development of MELCOR for modeling MSRs is required. Although understanding the chemistry surrounding MSRs is important to general MSR licensing and operation, only a subset of reactions and phenomenology are required to model beyond design basis incidents and therefore to be captured by MELCOR. This report is intended to guide the chemical phenomenology to improve MELCOR MSR accident modeling and discusses phenomenology models that are in development.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2021

Experiments with a prototype titanium hot cavity surface ionization source intended for electromagnetic separation of radioactive samarium and other lanthanide elements

This paper reports experimental results of a prototype titanium surface ionization source. For the first time, a lanthanide ion beam has been produced with a surface ionizer composed completely of titanium metal. Titanium does not readily activate with neutron irradiation. This offers the potential for inserting an ion source made of titanium directly into a reactor with a pre-loaded non-radioactive lanthanide target. This seamlessly integrates target irradiation with isotope separation, eliminating post irradiation sample manipulation. Samarium ion beam currents up to 960 nA have been produced in an off-line test bench equipped with rudimentary beam optics. This is a crucial step toward the development of an ionization source adopted for the electromagnetic isotope separator (EMIS) facility, which has been designed for high throughput separations of radioactive 153 Sm and other lanthanides of interest in the field of nuclear medicine. The ion current and important factors affecting the performance of the ion source, such as the ionizer temperature and thermal gradient, are discussed. Lastly, the experimental results are presented together with a discussion of future modifications to optimize the overall surface ionization source performance.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2022

Coincidence measurements of radioxenon using passive implemented planar silicon (PIPS) detector

The Comprehensive Test Ban Treaty (CTBT) bans nuclear weapons testing and establishes the International Monitoring System (IMS) for the purpose of treaty verification. IMS is a detector network that confirms that global nuclear activity is peaceful in nature. These detector systems use β-γcoincidence measurements to characterize atmospheric samples containing radioxenon isotopes. The goal of this work is to use the system consisting of two sodium iodide detectors and two PIPSbox detectors to characterize isotopically pure samples of 131m Xe, 133m Xe, 133 Xe, and 135 Xe via β, γ, and β-γ coincidence measurements.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2020

Nuclear spin conservation enables state-to-state control of ultracold molecular reactions

Quantum-state control of reactive systems has enabled microscopic probes of underlying interaction potentials and the alteration of reaction rates using quantum statistics. However, extending such control to the quantum states of reaction outcomes remains challenging. Here in this work, we realize this goal by utilizing the conservation of nuclear spins throughout the reaction. Using resonance-enhanced multiphoton ionization spectroscopy to investigate the products formed in bimolecular reactions between ultracold KRb molecules we find that the system retains a near-perfect memory of the reactants’ nuclear spins, manifested as a strong parity preference for the rotational states of the products. We leverage this effect to alter the occupation of these product states by changing the coherent superposition of initial nuclear spin states with an external magnetic field. In this way, we are able to control both the inputs and outputs of a reaction with quantum-state resolution. The techniques demonstrated here open up the possibilities to study quantum entanglement between reaction products, and ultracold reaction dynamics at the state-to-state level.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2021

Nuclear Data Needs for Radiochemistry

There are many elements of interest to the weapons community that include light elements, activation products, fission products, actinides and heavy elements. Of course, that is the whole periodic table! In this memo we summarize a down-selected list, 22 of 118+ of elements that have or could serve as radiochemical diagnostic measurements. The simulations would need cross sections for nuclides (and metastable states) of these elements to be able to calculate values for comparison with debris measurements.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗