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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 91 records · Page 5
All sourcesNASA NTRSDOE OSTI
DOE OSTI2019

Analysis of Cygnus Electrical Signals

The United States initiated the Subcritical Experiment (SCE) program to support a stockpile stewardship mission shortly after the 1992 moratorium on underground nuclear testing was established. Many SCE’s are conducted at the Nevada National Security Site (NNSS) in Nevada. Cygnus is a high-energy radiation generating device (RGD) located and operated at the NNSS and is a primary diagnostic for the SCE program. The Cygnus Dual Beam Radiographic Facility consists of two identical radiographic sources, Cygnus 1 and Cygnus 2. From creation of the high power V-I drive to energy transport and X-ray conversion at the rod-pinch diode, the Cygnus machines utilize the following components: oil-filled Marx generator, water-filled pulse-forming line (PFL), water-filled coaxial transmission line (CTL), three-cell vacuum induction voltage adder (IVA), and rod-pinch diode. The diode pulse has the following electrical specifications: 2.25 MV, 60 kA, 60 ns. Each source has the following X-ray specifications: 1 mm diameter, 4 rad at 1 m, and 50 ns radiation pulse. SCEs are both single-event and high-value; therefore, a high level of performance in reliability and reproducibility are key issues of Cygnus. Prior to executing such a SCE, there are a formidable number of shots (e.g., each of the two Cygnus RGDs charging and discharging properly into the rod-pinch diode load) that must be executed to determine reliability and reproducibility of the Cygnus RGDs. For every shot on Cygnus, voltages and currents along the machine are recorded and analyzed. In this paper we summarize attributes of the voltage and current waveforms at different locations using distribution plots. These distribution plots are used to quantify the reliability and reproducibility for Cygnus. This analysis methodology will provide a standard to trouble shoot results of individual Cygnus shots, and also to monitor long term Cygnus performance. Accordingly, this type of extensive analysis will contribute to optimized Cygnus performance on SCEs.

42 ENGINEERING↗
DOE OSTI2019

Integrated Methodology for the Impact Assessment of an Uranium Mill Contaminated Site - 19031

This work describes the development of mathematical models for radionuclides distribution and transport in the environment. The applicability of the models involves an integrated approach to assess the quantitative dispersion of the radionuclides in different environmental compartments when released from uranium tailings or from other low-activity mining wastes storages. For every compartment the important pathways of contamination and the radionuclides of major concern are identified and selected, based on their chemical, physical, radiological and toxic properties. Each compartment represents an environmental media: air, soil, water, vegetation and biota. Depending on the characteristics of the sources different types of possible releases are evaluated using phenomenological models. Models of environmental release, dispersion, transport and fate within each environmental compartment, as well as models of transfer between them, are applied to a specific site. The model outputs are the radionuclides activities for each one of the environmental compartments, where relevant exposure end-points are previously identified. The methodology was applied to a specific Uranium Mill Site, referred here as the 'Mill'. The site comprises approximately 3.2 km and includes two inactive mills, former ore stockpiles areas, a partially reclaimed tailings pond disposal area and a current tailings pond disposal area. The Mill site began operations in the late 1950's extracting uranium ore by alkaline leaching. Later on, a new facility using acid leaching for extracting uranium begun to operate in 1980. The mill operated first continuously and after intermittently until its closure, in March 2006. The data required for the model input was acquired from different sources: direct measurements from this particular site and available from multiple site investigation reports (in particular, environmental data for groundwater, soil, surface water, sediments and biota); other, were selected from published data. For the unknown data, assumptions were made. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2020

Opportunities to Implement Solutions to Achieve Remedial Action Objectives in Consideration of Stakeholder Interests - 20365

A case study in the implementation of a soils excavation and removal project conducted at a Formerly Utilized Sites Remedial Action Program (FUSRAP) Maywood Superfund Site (FMSS) vicinity property; an active commercial business, in a densely populated area, with significant operational, technical and, logistical constraints that were expected to limit areas that could be remediated. The United States Army Corps of Engineers-led (USACE) team successfully navigated complex overlapping stakeholder interests to achieve a more efficient and complete removal of contaminated soils and debris while minimizing unnecessary excess costs to the Government. This paper centers on FUSRAP activities at the FMSS vicinity property located at 149-151 Maywood Avenue, Maywood, Bergen County, New Jersey. For most of its FUSRAP history, this ∼109,000 square meter (27-acre) property housed a now-demolished ∼26,000 square meter (6.5-acre) warehouse operated by Sears Logistics Services, a unit of the Sears Roebuck Company (Figure 2). Sears ended its property lease and vacated the warehouse in December 2016. Given that long history and for the purposes of this paper, the property will be referred to as the 'Sears property' or simply 'the property.' The Sears property is approximately 109,000 square meters (27-acres) and is currently zoned for commercial use. The property is bound to the north and northwest by 100 West Hunter Avenue (the Stepan Company), to the northeast by 205 Maywood Avenue, to the east by Maywood Avenue, to the south by 23 West Howcroft Road, and to the west by businesses on NJ Route 17 and the NJ Route 17 roadway. Until December 2016, the property housed a warehouse and distribution center operated by Sears Logistical Services. On-site structures were demolished by the property owner in 2017. The warehouse covered the north section of the property along the Stepan Company property line. A railroad spur from the adjacent property now known as the Maywood Interim Storage Site (MISS) ended at the northeast corner of the warehouse. Wetlands were located east of the warehouse; the rest of the property was covered with paved parking lots and grassed areas. During remediation at the property, opportunities frequently arose where the project team was able to coordinate effectively with stakeholders to sequence remediation activities to facilitate removal of otherwise inaccessible soils and identify opportunities for materials reuse when supported by residual radiological and chemical levels. Some specific opportunities include: - remediating individual truck loading dock bays to maintain tenant operations; - working along a busy highway and in a utility corridor containing a 30-inch high pressure gas main; - remediating Lodi Brook and associated wetlands requiring bypass pumping and other diversionary structures to maintain local community stormwater drainage; - protecting during remediation and supporting access to facilitate tenant/owner maintenance of critical fire protection and water supply system service lines buried in contaminated soils and necessary for safe warehouse operations; and - coordinating with stakeholders to ensure non-radiological contaminants of concern for the site (unaffiliated with FUSRAP) were addressed by the responsible party in a manner that maximized benefit to all parties while supporting an efficient overall site remediation program. Once the property was vacant and the warehouse structure and radiologically non-impacted above-grade structures were demolished, the project identified an opportunity to significantly reduce the volume of waste associated with the foundation of the former warehouse, a foundation suspected of being partially constructed in radiologically contaminated soils. The project developed and implemented supplemental radiological verification survey and sampling strategies based on radiological cross-contamination risk potential with process flow-charts and screening-level based decision points; a program that classified saw-cut sections of concrete based on observed residual surface radioactivity conditions using a combination of gamma sensitive sodium-iodide scans and beta sensitive Geiger-Muller direct measurements. The proposed approach was reviewed with stakeholders with feedback, including consideration of applicable State of New Jersey Site Remediation Program criteria and guidance before implementation. Once classified, additional sampling was performed at frequencies driven by screening. The sampling methods, stockpile sampling frequencies, criteria and, approach to data evaluation were developed in consideration of existing site cleanup standards, regional background ranges, State of New Jersey radiological remediation program guidance, and specific stakeholder input With the property remediation and survey efforts nearly completed, it is relevant to examine retrospectively the objectives, assumptions and limitations in the remedial design (i.e., what was planned) versus what was able to be accomplished through effective teaming. Benefits to other environmental remediation site programs include better understanding of how to work effectively with stakeholders to achieve win-win outcomes, and approaches to site remediation, waste minimization and materials reuse that were successful in their overall outcomes. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2023

In-situ Synthesis of PuCl 3 and Corresponding Raman and Density Functional Theory Vibrational Modes

The experimental and calculated Raman spectrum of PuCl 3 has been reported for the first time. PuCl 3 is a primary species found in plutonium metal refinement, specifically in pyrochemical salt processes including multicycle direct oxide reduction, metal chlorination, and electrorefining. As such, Raman signatures of PuCl 3 could serve as potential forensic indicators of material process history. A novel technique for synthesizing PuCl 3 from the in situ chlorination of plutonium metal with HCl was developed to establish these signatures. Cerium metal surrogates were utilized to ensure optimization of the plutonium experiments and to minimize personnel exposure, and all experiments were carried out in a Raman reaction chamber designed for air-tight, high vacuum environments. In situ Raman spectroscopy was employed in conjunction with density functional theory (DFT) to investigate the vibrational modes of PuCl 3 . Associated mixed oxy and hydroxyl phases are also reported. The combined Raman and DFT results have eliminated inconsistencies in Raman mode assignments for the MX 3 family of metal chlorides having P6 3 /m symmetry, and IR modes derived from the DFT calculations are additionally presented. The data observed in this study are of potential interest to nuclear forensic analyses, nuclear sample aging, nuclear energy, plutonium processing, and stockpile stewardship.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Prospects for Surrogate Neutron Capture Measurements with Radioactive Ion Beams and GODDESS

Neutron capture reactions are responsible for the synthesis of almost all of the elements heavier than iron through the slow s-process, that proceeds close to the line of stability, and the rapid r-process, with very neutron-rich waiting points. Uncertainties in (n,γ) rates in neutron rich nuclei, especially near closed neu- tron shells, can have significant impact [1] on the predictions of final abundances for different astrophysical scenarios for the r process. Understanding (n,γ) rates on neutron-rich fission fragments is also important for nuclear forensics and stockpile stewardship science. Ratkiewicz et al. [2 and references therein] has recently demonstrated that the (d,pγ) reaction is a valid surrogate for (n,γ), where the formation of the compound nucleus from the breakup of the deuteron has been calculated in a reaction model and the subsequent measured gamma-decay probabilities are reproduced with standard level density and strength functions in a Bayesian approach. In parallel to the surrogate validation efforts, we have demonstrated that the (d,pγ) reaction can be measured in inverse kinematics with Gammasphere ORRUBA: Dual Detectors for Experimental Structure Studies (GODDESS) [3] where the Gammasphere array of Compton-suppressed HPGe detectors is coupled to the Oak Ridge Rutgers University Barrel Array of position-sensitive silicon strip detectors. During the commissioning campaign we measured the (d,pγ) reaction with 134 Xe and 95 Mo beams, the latter to demonstrate the surrogate method in inverse kinematics. The present talk will present preliminary results from this campaign including γ-decay probabilities and prospects for surrogate (n,γ) measurements with 143 Ba fission-fragment beams.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2025

Opportunities for Cerium Valorization in the Rare Earth Supply Chain

Rare earth (RE) elements are co-located in ore deposits and must be treated together during the difficult extraction and separation. Cerium is the majority element in most deposits (> 50 %), and the growing need for Nd, Pr and the heavy lanthanides in permanent magnets and other energy transition technologies results in costly stockpiling of cerium oxide which has low demand. Finding new high-value applications for cerium or its compounds is therefore a sought-after goal to improve the profitability of rare earth mining and processing. Here, this contribution will highlight the use of cerium in high-strength aluminum alloys and the preparation of Ce-based permanent magnets as two emerging technologies for high-value products that have potential to stabilize the fluctuating rare earth market, substitute critical materials, support the nascent domestic rare earth industry and provide technologies for the pending green energy transition.

Energy - Conversion, Materials science↗
DOE OSTI2021

On the Feynman-alpha method for reflected fissile assemblies

The Feynman-alpha method is a neutron noise technique that is used to estimate the prompt neutron period of fissile assemblies. The method and quantity are of widespread interest including in applications such as nuclear criticality safety, safeguards and nonproliferation, and stockpile stewardship; the prompt neutron period may also be used to infer the k eff multiplication factor. The Feynman-alpha method is predicated on time-correlated neutron detections that deviate from a Poisson random variable due to multiplication. Traditionally, such measurements are diagnosed with one-region point kinetics, but two-region models are required when the fissile assembly is reflected. This paper presents a derivation of the two-region point kinetics Feynman-alpha equations based on a double integration of the Rossi-alpha equations, develops novel propagation of measurement uncertainty, and validates the theory. Validation is achieved with organic scintillator measurements of weapons-grade plutonium reflected by various amounts of copper to achieve k eff values of 0.83–0.94 and prompt periods of 5–75 ns. The results demonstrate that Feynman-alpha measurements should use the two-region model instead of the one-region model. The simplified one-region model deviates from the validated two-region models by as much as 10% in the estimate of the prompt neutron period, and the two-region model reduces to the one-region model for small amounts of reflector. The Feynman-alpha estimates of the prompt neutron period are compared to those of the Rossi-alpha approach. The comparative results demonstrate that the Feynman-alpha method is more precise than the Rossi-alpha method and more accurate for k eff < 0.92, whereas the Rossi-alpha method is generally more accurate for higher multiplications. Here, the uncertainty propagation developed in this work should be used for all Feynman-alpha measurements and will therein improve fitting accuracy and appropriate precision estimates.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗
DOE OSTI2020

Validation of the two-region Rossi-alpha model for reflected assemblies

Nuclear criticality safety, nonproliferation and safeguards, emergency response, and stockpile stewardship utilize estimates of the k eff multiplication factor. The value of k eff cannot be directly measured, but it can be inferred from the prompt neutron period. One modality of measuring the prompt neutron period is the Rossi-alpha method, which is predicated on fitting a histogram of detection time differences due to the nonrandom temporal distribution of same-fission-chain neutrons. Recent works have developed the motivation and theory to expand traditional one-region point kinetic models resulting in one-exponential histogram fits to two-region models that result in two-exponential fits. This paper validates the new two-region model using organic scintillator measurements of copper-reflected weapons-grade plutonium (0:83 ≤ k eff ≤ 0:94) and high-density- polyethylene-reflected highly enriched uranium (0:73 ≤ k eff ≤ 0:95). Furthermore, the results show that more thermal systems have shorter prompt neutron periods in the core region due to increased induced-fission probabilities for moderated neutrons. Here, a new parameter introduced by the two- region model is also shown to be correlated to the amount of reflection, and may be used to infer assembly properties such as type and amount of reflector.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2024

GENESIS: Gamma Energy Neutron Energy Spectrometer for Inelastic Scattering

Improved neutron inelastic scattering cross section data are needed to inform integral benchmark studies and advance applications in a wide variety of areas including nuclear energy, stockpile stewardship, nonproliferation, and space exploration. Neutron inelastic scattering also serves as a non-selective probe of low-lying nuclear structure. To help meet these needs, the Gamma Energy Neutron Energy Spectrometer for Inelastic Scattering (GENESIS) was constructed at the 88-Inch Cyclotron at Lawrence Berkeley National Laboratory. This array couples high-resolution γ-ray detectors and fast neutron detectors to achieve single and coincident n/γ detection over a broad energy range. The current configuration of the array includes 26 organic liquid scintillators and four high-purity germanium detectors (two single-crystal and two four-crystal CLOVER detectors with two-fold segmentation). The array was constructed with minimal supporting material and designed to cover a wide range of secondary particle angles and energies with limited inter-element scattering. Data acquisition is accomplished using Mesytec MDPP-16 multi-channel high-resolution digital pulse processing modules. The array characteristics, including γ-ray and neutron energy resolution, timing resolution, and detection efficiency were measured and used to validate a Geant4 model of the array. Furthermore, the primary sources of neutron background and the uncertainties in the determination of incident and secondary neutron energy were assessed. GENESIS provides a new capability to address nuclear data needs and facilitates the advancement of a wide range of nuclear applications.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2025

Commissioning of the neutron irradiation station at the University of Notre Dame

Cross section data for neutron-induced reactions are needed for applications in nuclear astrophysics, stockpile stewardship, and nuclear reactor design but often contain discrepancies and gaps. A neutron source with a high neutron flux, a well-characterized neutron energy distribution, and a wide range of available neutron energies is ideal for studying such reactions in order to improve on existing data and provide new experimental results. For this purpose, the Neutron Irradiation Station (NIS) was developed using the 7 Li(p,n) 7 Be reaction. Neutron energy profiles were obtained using 3 He spectrometers and neutron standards were used to determine the neutron flux using the activation method. The neutron energy profile was found to be quasi-monoenergetic and neutrons were produced at energies from 1 keV to 1 MeV. Finally, the flux at the production target was found to be (1.42 ± 0.20) x 10 8 s −1 cm −2 .

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2025

Radiation hot spot formation on UF 6 30B cylinders

The accurate material accountancy of a country's enriched uranium hexafluoride (UF 6 ) stockpiles is imperative to the International Atomic Energy Agency (IAEA) for determining appropriate material safeguards. Uranium hexafluoride is typically stored in large cylinders with enrichment verification typically performed with a NaI gamma detector using the enrichment meter method. This approach for calculating enrichment assumes that the UF 6 is homogeneous inside the cylinder. Here, the measurements and tests presented in this manuscript show that the UF 6 in cylinders left outside in the elements can experience fractionation, leading to inhomogeneity, and subsequent development of radiation hot spots. These hot spot locations can produce errant enrichment measurements. In dark-colored cylinders that experience significant surface heating from the sun, UF 6 sublimates off the cylinder walls, leaving only the uranium daughter products in a horizontal patch (stripe) along the cylinder's midline. This daughter patch is hypothesized to be the source of the radiation hot spots. The patch forms during the summer and tends to decay away during the winter, when solar intensity and temperatures are reduced.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2025

Do Households Adapt? Repeated Hurricane Exposure and the Purchasing of Bottled Water

Understanding how households adapt to hurricanes is increasingly important as these events become more frequent and severe. This paper examines how past hurricane exposure influences current household preparedness, focusing specifically on the stockpiling of bottled water. Leveraging scanner data on bottled water purchases for households in the Southeastern United States, we employ a difference-in-differences event study framework to analyze how repeated hurricane experiences affect consumer behavior. Our results indicate that households exposed to hurricane warnings do not increase their preparedness in the subsequent hurricane season, and those experiencing a landfall event underprepare. These results suggest limited learning from past events.

D12↗
DOE OSTI2025

Adsorption and Chromatographic Behavior of Dispersed Sodium Bismuthate Systems for the Separation of Americium from Curium

The selective partitioning of americium (Am) and curium (Cm) is integral for nuclear science areas such as the nuclear fuel cycle, stockpile stewardship, and isotope production but remains a long-standing radioanalytical challenge due to nearly identical chemical properties. Differences in redox chemistry can be exploited since Am can be oxidized to the hexavalent oxidation state. Sodium bismuthate (NaBiO 3 ) exhibits favorable oxidation and ion exchange characteristics conducive to a rapid and efficient Am/Cm chromatographic separation. Contact of nitric acid with NaBiO 3 was shown to significantly decrease the nitric acid concentration and solution volume. The adsorption, kinetic, and chromatographic behavior of Am and Cm in systems that disperse NaBiO3 in filter aids was evaluated. Further, dispersion of NaBiO 3 increased separation factors to over 100, with rapid kinetics achieved within 1 min of contact and sustained for at least 2 h. The adsorption capacity was more than doubled from 0.066 mequiv g –1 for solid NaBiO 3 alone to 0.149(6) and 0.156(9) meq g –1 when dispersed in Celite 545 and silica gel, respectively. Complete separation was achieved in all systems with ~100% recovery in the respective eluted fractions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Hyperstoichiometric Uranium Dioxides: Rapid Synthesis and Irradiation-Induced Structural Changes

Uranium dioxide (UO 2 ), the primary fuel for commercial nuclear reactors, incorporates excess oxygen forming a series of hyperstoichiometric oxides. Thin layers of these oxides, such as UO 2.12 , form readily on the fuel surface and influence its properties, performance, and potentially geologic disposal. This work reports a rapid and straightforward combustion process in uranyl nitrate–glycine–water solutions to prepare UO 2.12 nanomaterials and thin films. We also report on the investigation of the structural changes induced in the material by irradiation. Despite the simple processing aspects, the combustion synthesis of UO 2.12 has a sophisticated chemical mechanism involving several exothermic steps. Raman spectroscopy and single-crystal X-ray diffraction (XRD) measurements reveal the formation of a complex compound containing the uranyl moiety, glycine, H 2 O, and NO 3 – groups in reactive solutions and dried combustion precursors. Combustion diagnostic methods, gas-phase mass spectroscopy, differential scanning calorimetry (DSC), and extracted activation energies from DSC measurements show that the rate-limiting step of the process is the reaction of ammonia with nitrogen oxides formed from the decomposition of glycine and uranyl nitrate, respectively. However, the exothermic decomposition of the complex compound determines the maximum temperature of the process. In situ transmission electron microscopy (TEM) imaging and electron diffraction measurements show that the decomposition of the complex compound directly produces UO 2 . The incorporation of oxygen at the cooling stage of the combustion process is responsible for the formation of UO 2.12 . Spin coating of the solutions and brief annealing at 670 K allow the deposition of uniform films of UO 2.12 with thicknesses up to 300 nm on an aluminum substrate. Irradiation of films with Ar 2+ ions (1.7 MeV energy, a fluence of up to 1 × 10 17 ions/cm 2 ) shows unusual defect-simulated grain growth and enhanced chemical mixing of UO 2.12 with the substrate due to the high uranium ion diffusion in films. As a result, the method described in this work allows the preparation of actinide oxide targets for fundamental nuclear science research and studies associated with stockpile stewardship.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2020

Tools and Incentives for Implementing Codes of Ethics to Help Prevent the Reemergence of Chemical Weapons

Since the entry into force of the Chemical Weapons Convention (CWC) and the establishment of the Organisation for Prohibition of Chemical Weapons (OPCW) in 1997, 96% of the world’s declared stockpile, comprising 72,305 metric tons of chemical warfare agents have been destroyed. Despite this notable progress, the convergence of chemistry and biology brings new challenges to preventing chemical weapons production, as the technical capability to manipulate the chemistry of microorganisms has diffused beyond the chemical industry and academic research communities. The development and voluntary adoption by chemical practitioners around the world of ethical codes or guidelines, such as The Hague Ethical Guidelines and the Global Chemists’ Code of Ethics (GCCE) , are important steps in strengthening international nonproliferation efforts through their potential to impact the intent of the individual by normalizing ethical behavior. However, the simple act of adopting a code does not guarantee ethical behavior. Care must be taken to ensure those adopting the code understand specifically the behavior being asked of them, and they must be given ample opportunities to practice exercising those behaviors in low-risk situations and encouragement to keep trying when they fail. Furthermore, in small-to-medium chemical companies, concerns that adopting such measures could negatively impact profit margins may dissuade some business owners from voluntarily adopting ethical codes, while a country’s decision makers may not prioritize establishment of new regulatory mechanisms that could address some of these concerns. In this paper, factors that may positively influence a chemical company’s decision to adopt ethical guidelines, such as integration of social sustainability elements into frameworks and approaches to maintain social legitimacy in the eyes of the broader community, are explored. Voluntary adoption of ethical codes gives teeth to arms control regimes. By encouraging chemical companies to become engaged in the community around them and providing easy-to-use tools like scenario-based E-learning to enable remote engagement and facilitate understanding of the principles undergirding the GCCE, they actively participate in making the world a better place and minimizing the potential for reemergence of chemical weapons.

Small Chemical Companies, Codes of Ethics, E-learn↗
DOE OSTI2021

Irradiation-Driven Restructuring of UO 2 Thin Films: Amorphization and Crystallization

Combustion synthesis in uranyl nitrate–acetylacetone–2-methoxyethanol solutions was used to deposit thin UO 2 films on aluminum substrates to investigate the irradiation-induced restructuring processes. Thermal analysis revealed that the combustion reactions in these solutions are initiated at ~160 °C. The heat released during the process and the subsequent brief annealing at 400 °C allow the deposition of polycrystalline films with 5–10 nm UO 2 grains. The use of multiple deposition cycles enables tuning of the film thicknesses in the 35–260 nm range. Irradiation with Ar 2+ ions (1.7 MeV energy and a fluence of up to 1 × 10 17 ions/cm 2 ) is utilized to generate a uniform distribution of atomic displacements within the films. X-ray fluorescence (XRF) and alpha-particle emission spectroscopy showed that the films were stable under irradiation and did not undergo sputtering degradation. X-ray photoelectron spectroscopy (XPS) showed that the stoichiometry and uranium ionic concentrations remain stable during irradiation. The high-resolution electron microscopy imaging and electron diffraction analysis demonstrated that at the early stages of irradiation (below 1 × 10 16 ion/cm 2 ) UO 2 films show complete amorphization and beam-induced densification (sintering), resulting in a pore-free disordered film. Prolonged irradiation (5 × 10 16 ion/cm 2 ) is shown to trigger a crystallization process at the surface of the films that moves toward the UO 2 /Al interface, converting the entire amorphous material into a highly crystalline film. This work reports on an entirely different radiation-induced restructuring of the nanoscale UO 2 compared to the coarse-grained counterpart. The preparation of thin UO 2 films deposited on Al substrates fills an area of national need within the stockpile stewardship program of the National Nuclear Security Administration and fundamental research with actinides. Here, the method reported in this work produces pure, robust, and uniform thin-film actinide targets for nuclear science measurements

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Impact of Precipitation Parameters on the Specific Surface Area of PuO 2

Controlling the properties of PuO 2 through processing is of vital importance to environmental transport and fate, production of nuclear fuels, nuclear forensic analyses, stockpile stewardship, and storage of nuclear wastes applications. A number of processing conditions have been identified to control final product properties, including specific surface area (SSA), residual carbon content, adsorption of volatile species, morphology, and particle size. In this paper, a novel approach is developed for the prediction of PuO 2 SSA via the synthetic route of Pu(IV) oxalate precipitation followed by calcination. The proposed model utilizes multivariate regression methodology and leave one out formalism to link Savannah River Site (SRS) precipitation and calcination production data to the SSA of the final product. A comparison among the models provides insight into the accuracy and ability to identify variations amongst the processing data. Additionally, the models may also be used to fit new data outside of the parameters explored in a production facility. Finally, the trained model was compared to a similarly trained conventional model form to illustrate the influence of precipitation parameters on the prediction of the final SSA. The models presented here attempt to provide new methods for more accurate prediction of the PuO 2 product properties in a production scale environment for key environmental and nuclear applications.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗