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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 955 records · Page 53
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Demonstration of 151 Sm analysis using Trinity nuclear debris samples

Here, the long-lived fission product 151 Sm (T 1/2 ≈ 90 y) present in archived dissolved Trinity nuclear test debris samples was analyzed using liquid scintillation counting and the results were compared to the expected values based upon historical analysis results. The measured 151 Sm activities were found to agree with the expected values within experimental error. This demonstration validates the use of this technique in situations where the sample is too old for traditional shorter half-life radioactive fission product signatures such as 99 Mo (T 1/2 = 2.75 d), 97 Zr (T 1/2 = 16.7 h), 147 Nd (T 1/2 = 10.98 d), and 153 Sm (T 1/2 = 46.3 h), or too dilute for determining fissions through stable isotope ratio measurements.

151Sm↗
DOE OSTI2024

Kinetics of Radiation-induced Cr( II ) and Cr( III ) Redox Chemistry in Molten LiCl-KCl Eutectic

Chromium (Cr) is a frequent constituent of the metal alloys proposed for molten salt nuclear reactor (MSR) applications, and is typically the least noble metal ion present. Consequently, chromium is preferentially corroded into molten salt solutions. Here, the redox poise and redox cycling of chromium ions in the salt can greatly influence its corrosivity towards structural alloys, ultimately impacting the longevity of MSR systems. Radiation-induced chemistry is expected to play a significant role in determining the chromium oxidation state distribution during MSR operations. In the present research, electron pulse radiolysis techniques were employed to characterize the reactivity of Cr(II) and Cr(III) ions with primary radiolysis products in molten lithium chloride–potassium chloride (LiCl–KCl) eutectic over a temperature range of 400–600 °C. Both chromium oxidation states were found to rapidly react with the primary products of molten chloride salt radiolysis, i.e., the solvated electron (e S - ) and the dichlorine radical anion (Cl 2 ˙ - ). For reactions with the e S - , second-order rate coefficients (k) of k = (4.1 ± 0.2) and (6.1 ± 0.3) × 10 10 M -1 s -1 at 400 °C for Cr(II) and Cr(III), respectively, were determined. Temperature-dependent measurements allowed for the derivation of activation parameters for electron capture by Cr(II) and Cr(III). Both chromium ions also react with Cl 2 ˙ - , k = (7.2 ± 0.3) and (1.4 ± 0.1) × 10 9 M -1 s -1 at 400 °C for Cr(II) and Cr(III), respectively.

37 - INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL C↗
DOE OSTI2020

Radionuclide Screening Analysis and Transport Parameters for Pahute Mesa Detonations, Nevada National Security Site

A “screening analysis” is implemented at Pahute Mesa (PM), Nevada National Security Site (NNSS), to determine subsets of the 43 radionuclides listed in the radionuclide inventory of Finnegan et al. (2016) that are of relevance or potential relevance to the hydrologic source term (HST) for assessment of radionuclide transport in groundwater. Consideration is added to how levels of contamination are defined and whether any other radionuclides not in the inventory are relevant to the HST. A model is developed to estimate a range of possible source concentrations in groundwater that account for uncertainty in partitioning into melt glass and sorption into surrounding rock of the exchange zone for the 82 PM underground nuclear tests detonated in vertical shafts. The model also accounts for the varied hydrogeochemical settings. Transport parameters needed for the screening model calculations are developed from databases for hydrogeologic units, chemistry, mineralogy, fracture spacing, fracture aperture, fracture openness, matrix porosity, bulk density, saturation, and alteration. Of key importance is consideration of diagenetic zonation of the mineralogy related to hydrothermal alteration. The screening analysis compares model results with available groundwater radiochemistry data. Consistency between screening model results and available data helps validate the model for application to all 43 radionuclides, most of which have no measurements or only non-detect measurements of concentration in groundwater. The screening analysis determines that ten radionuclides – tritium, Sr-90, I-129, Cs-137, U-232, U-233, U-234, U-238, and the total of Pu-239 and Pu-240 are relevant to the HST. Determination of relevance is primarily based on data and/or model results indicating source concentration exceeding a maximum contaminant level (MCL) out to 100 years since the time of detonation. U-238 is relevant to assessment of contamination relative to MCLs for uranium and gross alpha particle activity. Five other radionuclides – C-14, Cl-36, Tc-99, Np-237, and Pu-238 – are determined potentially relevant to the HST based on a 0.1 MCL threshold. The screening analysis recommends additional attention to the natural daughter radionuclides of the uranium series (U-238) and thorium series (Th-232) decay chains, particularly Ra-226 and Ra-228, that were not included the inventory.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2022

Radiochronometric analysis of an historic Cs-137 activity standard

In this work, a 137 Cs activity standard discovered during routine inventory was analyzed to determine its model age using radiochronometry. The aqueous activity standard was separated using an established separation method that employs commercially available Sr resin. The method was also tested against a nuclear forensics reference material developed specifically for benchmarking 137 Cs radiochronometry methods. Results of the analyses showed good agreement between the results and the certified values of the reference material. Analysis of the discovered activity standard were also in good agreement with the activity certification date, though uncertainty was higher due to natural Ba contaminating the sample and the stable 133 Cs used as a carrier during the standard’s production.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2020

Advanced Analysis of Plutonium: Pre- and Post-Detonation Scenarios

A Dissertation Presented for the Doctor of Philosophy Degree in Nuclear Engineering. Overarching research question: Do nuclear reactions in surface environment lead to distinctive chemical and isotopic signatures that are not present in nature? Testable hypothesis: Nuclear processes will lead to distinctive chemical and isotopic patterns of partitioning because high-temperature processes under high radiation rarely occur in natural surface environment.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2025

147 Nd Quantification Using HSCCC-Purified Samples

Quantifying the fission product 147 Nd in nuclear debris samples is an important component of post-detonation nuclear forensics. The most accurate quantifications are obtained when Nd is purified from all other fission products, actinides, activation products, and environmental matrix contained within the debris. In this study, a recently developed method for Nd purification was tested, purifying 147 Nd from solutions of mixed fission products using high-speed counter-current chromatography (HSCCC). Importantly, the new method allowed for faster elution of Nd from the column as compared with established high performance liquid chromatography (HPLC) methods, and resulted in accurate/precise 147 Nd quantification by gamma-ray spectrometry. While the up-front equipment costs associated with HSCCC may be higher, its operational costs are on par with those of HPLC (solvents, extractants, power). Gas-flow proportional beta decay counting revealed contamination from the nearest neighbor lanthanide 143 Pr (a gamma-silent radioisotope) in the HSCCC-purified samples, but the activity contribution from 147 Nd could still be quantified. Remarkably consistent elution profiles were observed for the HSCCC method, spanning rare earth element (REE) loadings of more than 10 orders of magnitude (tracer to mmol quantities). In conclusion, the reliability and speed of the new method suggest utility for the rapid separation and quantification of 147 Nd in unknown samples.

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

Pu(VI) Oxalate Crystal Structure and Evidence of Photoreduction to Pu(IV) Oxalate

We report the first crystal structure of a Pu(VI)-oxalate compound. This compound, [PuO 2 (C 2 O 4 )(H 2 O)]·2(H 2 O) (1), crystallizes in space group P21/c with a = 5.5993(3) Å, b = 16.8797(12) Å, c = 9.3886(6) Å, and β = 98.713(6)°. It is isostructural with the previously reported U(VI) compound, [UO 2 (C 2 O 4 )(H 2 O)]·2(H 2 O). Each plutonyl ion (PuO 2 2+ ) is coordinated in the equatorial plane by two side-on bidentate oxalates, creating an infinite chain along [001]. A coordinated water molecule and twisting of the oxalates lead to a distorted pentagonal bipyramidal geometry of the Pu. A photochemical degradation was observed for 1, which resulted in the formation of a secondary crystalline phase. The absorption spectrum of this secondary phase confirmed the presence of Pu(IV), but it did not match the spectrum of Pu(C 2 O 4 ) 2 ·6H 2 O, which is considered to be the primary product of Pu-oxalate precipitation. While compound 1 has previously been proposed to exist in solution, this is the first time it has been isolated via crystallization. Although redox interactions between Pu and oxalate have been documented in the literature, the present study is the first observation of a photochemical reduction of Pu(VI)-oxalate. Finally, this study has expanded on the limited understanding of the Pu(VI)-oxalate system, which is important for nuclear fuel cycle applications.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2024

Milestone 1.2.16. Reconciling the Impacts of Thermal Pretreatment on Radiation-Induced H2 Generation from Aluminum-Clad Spent Nuclear Fuel Surrogate Materials

To support the technical basis for the extended dry storage of aluminum-clad spent nuclear fuel (ASNF), thermal pretreatment procedures to minimize the radiation-induced generation of molecular hydrogen (H2) have been investigated. The aim of thermal pretreatment is to eliminate the residual adsorbed water content on the ASNF’s corrosion layers, precursors for H2 generation. To date, irradiation studies in this area have found conflicting results for the effectiveness of thermal pretreatment procedures. The aim of this study was to reconcile those differences. However, the presented results, which utilized a modified in situ thermal pretreatment procedure, afforded H2 yield data that further indicates that thermal pretreatment does not significantly reduce the radiation-induced yield of H2 from gamma irradiated ASNF surrogate materials. Assessment of the differences between thermal pretreatment studies suggests that stainless-steel—present in the irradiation setup of studies that demonstrated a reduction in the yield of H2 with thermal pretreatment—may afford not only unanticipated interfacial chemistry, but also the formation and radiolytic contribution of iron oxides to the chemistry underpinning the formation of H2 in these systems. Given the Department of Energy Standard Canister—proposed for the extended dry storage of ASNF—is predominantly composed of stainless-steel, the potential contribution of stainless-steel and its corrosion layers to radiolytic H2 production should be further investigated. This research was funded by the U.S. Department of Environmental Management, Office of Technology Development, under contract DE-AC07-05ID14517.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2022

Radiation-induced reaction kinetics of Zn 2+ with e S - and Cl 2 ˙ - in Molten LiCl–KCl eutectic at 400–600 °C

We report molten chloride salts are currently under consideration as combined coolant and liquid fuel for next-generation molten salt nuclear reactors. Unlike complementary light-water reactor technologies, the radiation science underpinning molten salts is in its infancy, and thus requires a fundamental mechanistic investigation to elucidate the radiation-driven chemistry within molten salt reactors. Here we present an electron pulse radiolysis kinetics study into the behaviour of the primary radiolytic species generated in molten chloride systems, i.e., the solvated electron (e S - ) and di-chlorine radical anion (Cl 2 ˙- ). We examine the reaction of e S - with Zn 2+ from 400–600 °C (E a = 30.31 ± 0.09 kJ mol -1 ), and the kinetics and decay mechanisms of Cl 2 ˙- in molten lithium chloride-potassium chloride (LiCl–KCl) eutectic. In the absence of Zn 2+ , the lifetime of e S - was found to be dictated by residual impurities in ostensibly “pure” salts, and thus the observed decay is dependent on sample history rather than being an intrinsic property of the salt. The decay of Cl 2 ˙- is complex, owing to the competition of Cl 2 ˙- disproportionation with several other chemical pathways, one of which involves reduction by radiolytically-produced Zn + species. Overall, the reported findings demonstrate the richness and complexity of chemistry involving the interactions of ionizing radiation with molten salts.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2022

Characterization of PIPS detectors for measurement of radioxenon

The International Monitoring System arm of the Comprehensive Nuclear-Test-Ban Treaty Organization utilizes sampling of atmospheric radioxenon to scan the world for nuclear testing events. Current designs utilized in the field involve plastic scintillator cells run in coincidence with Sodium Iodide (NaI) or High Purity Germanium (HPGe) detectors. The use of plastic scintillators as electron detectors exhibit some issues in comparison to other materials. Silicon detectors are analyzed as an alternative to plastic scintillators for beta detection based on their higher energy resolution and lowered memory effect. A radioxenon detection setup was created with the intent of measuring radioxenon samples using coincidence counting between silicon and NaI detectors as well as silicon and HPGe. Finally, the absolute efficiency of both setups is calculated and compared.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2022

The influence of cooling rate on condensation of iron, aluminum, and uranium oxide nanoparticles

Fundamental observations of particle size distributions are needed to develop models that predict the fate and transport of radioactive materials in the atmosphere following a nuclear incident. The extent of material transport is influenced by the time scales of particle formation processes (e.g., condensation, coagulation). In this study, we investigated the influence of cooling time scales on size distributions of uranium, aluminum, and iron oxide particles that are synthesized separately under identical run conditions inside the controlled environment of an argon plasma flow reactor. Two distinct temperature distributions are imposed along the flow reactor by varying the argon flow rate downstream of the plasma torch. The vaporized reactants of uranium, aluminum, and iron are cooled from about 5000K to 1000K before they are collected on silicon wafers for ex situ scanning electron microscope analysis. The microscope images show that the sizes of the largest aluminum and iron oxide particles heavily depend on the cooling time scales, whereas significant size variation with cooling rate is not observed for uranium oxide particles. In addition, the size distribution of aluminum oxide particles exhibits the broadest range among all three metal oxides studied. We performed simulations of particle size distributions using a kinetic model that couples gas phase oxidation chemistry with particle formation processes, including nucleation, condensation, and coagulation. The model results demonstrate the strong sensitivity of particle size distribution to different cooling histories (i.e., temperature vs residence time) along the flow reactor. In conclusion, the kinetic model also helps identify directions for future research to improve the predictions.

36 MATERIALS SCIENCE↗
DOE OSTI2022

The electronic Raman scattering spectrum of PuO 2

Here the Raman spectrum of PuO 2 was measured up to 13,000 cm –1 with three different laser excitation wavelengths spanning the resonance (405 nm), near-resonance (457 nm), and preresonance (514 nm) energy range. Approximately 26 never-before-seen bands were observed between 3500 and 13,000 cm –1 . Given the very high energy of the Raman shifts of these bands and the relative insensitivity of their spectral position to the interrogating laser wavelength, they are believed to arise from an electronic origin. These bands are present in both freshly calcined and radiolytically aged PuO 2 , although a broad luminescence is observed in the aged material, which obscures many of the high frequency features. In situ laser annealing of the material attenuated this luminescence and allowed for clear observation of these never-before-seen spectral features. Discovery of these high-energy bands presents a new way of identifying PuO 2 for nuclear nonproliferation and forensics purposes.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2023

Metal-oxide cages open up strategy for processing nuclear waste

We report the ability to separate the radioactive element americium from spent nuclear fuel would lower the long-term hazards of nuclear waste. An inorganic molecular cage that selectively binds to americium opens up a separation strategy.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2024

Design of a high-temperature cell for cobalt-60 irradiations of aqueous solutions with in situ UV–visible spectroscopy

To understand the speciation of solutes in aqueous solutions in high temperature radiation environments, we report the design and fabrication of a custom-built, high temperature (≤300 °C) titanium irradiation cell with in situ optical spectroscopy capabilities, as afforded by coupled fiber optic cables. The wetted surfaces of the 8-inch tall cylindrical cell with 3.5 in. diameter are entirely made of titanium, sapphire, and gold, which are chemically and radiolytically inert. The initial benchmarking results are reported, including the baseline spectrum of deionized water as a function of temperature, the stability of a spectrum over 4 h at 100 °C, and an irradiated Fricke dosimetry solution under ambient irradiator temperature conditions (27.0 ± 0.5 °C). Further, the average gamma radiation dose rate in the cell in its current configuration is 26.1 ± 1.3 Gy min -1 . This cell has application in studying several processes throughout the nuclear fuel cycle, including the reactor coolant behavior.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2022

Age determination of a 75 Se gamma radiography source for nuclear forensics

Here, two methods were used to evaluate the age of 75 Se sealed source material. Both methods utilized gamma spectroscopy to determine the quantity of parent 75 Se present, but they differed in the technique used to determine the quantity of daughter 75 As. In one method, 75 As was quantified using inductively coupled plasma-mass spectrometry (ICP-MS) after using chromatographic techniques to separate the parent and daughter isotopes. In the other method, total As was measured using optical emission spectroscopy (OES), which did not require separation prior to measurement. The OES method was faster and gave slightly lower uncertainties, but required more daughter material to be present because of higher concentration requirements, making it unsuitable for young material. Both methods are hampered by the monoisotopic nature of As, but still gave reasonable model ages that were in agreement with each other.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2020

The Scientific Justification for a U.S. Domestic High-Performance Reactor-Based Research Facility

The Basic Energy Science Advisory Committee (BESAC) was charged with forming a subcommittee to assess the scientific justification for a U.S. domestic high-performance reactor-based research facility in order to continue providing the U.S scientific community with leading neutron capabilities in support of DOE's missions in science, energy, environment, and national security. The assessment included consideration of current international plans and existing domestic facility infrastructure. The subcommittee held a series of meetings from August 19, 2019 to April 24, 2020 that included DOE senior officials, leaders of national and international neutron facilities (SNS, HFIR, NIST, ILL, FRM-II), chairs of the NAS and POPA HEU-LEU committees, and outside experts on important areas of science, technology, and industry where high flux nuclear reactor facilities make important contributions. Also included were tours of neutron facilities (SNS, HFIR, NIST, BR2 reactor, and the planned Jules Horowitz Reactor). This July 2020 (revised 10-28-2020) report describes scientific use cases, brief summaries of existing and planned neutron facilities in the US and Europe, a comprehensive review of HFIR, a comprehensive discussion of the current state of progress on HEU-LEU conversion, user information from NIST and ORNL, and three recommendations to DOE for moving forward.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Modeling of Radiolytic Hydrogen Generation of Irradiated Surrogate Aluminum Plates

The hydrogen generation from oxyhydroxide layers under irradiation is an important effect to understand for the long-term storage of aluminum-clad spent nuclear fuel. The original chemical model shows steady production of hydrogen from aluminum oxyhydroxide layers, with no roll-over effect in the curves of the hydrogen concentration until significant pressure has built up within the canister. This study uses a variety of kinetic fits to adjust the old chemical model to have roll-over effects that are consistent with new high-dose experiments. The data from aluminum 6061 coupon tests at high doses were used to fit several kinetic models. The 6061 aluminum samples are representative of the aluminum-clad fuel from the ATR. The fitted kinetic models were then used in a model of a mini-canister with much higher packing density to determine which kinetic rates would fit both sets of experimental tests. The rate constants for the kinetic mechanisms that were close were then tweaked such that the chemical models fit both the experimental data from the capsule tests and the data from the mini-canister tests. The kinetic models which fit the best are either inhibition by hydrogen, or a back reaction wherein H radical is reabsorbed onto the oxyhydroxide layer. The H back reaction rolls over quicker and may fit future collected data.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗