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Alpha Decay Chains as Thermal Power Sources: Analysis and Applications for RTGs

Radioactive sources can provide power in remote and environmentally harsh locations such as the arctic or space. The generators powered by such sources are rugged and can withstand extreme temperatures, lack of sunlight, and require no human intervention for multiple years. Radioisotopes are used in thermoelectric generators to provide power at remote sites and deep in space. Isotopes like Pu-238, Cm-244, and Am-241 are used in these generators by NASA for power in space probes and spacecrafts. These power sources deliver a steady supply of energy over extended periods of time. Alpha particles created during decay do not travel far in a material. Their kinetic energy is transferred to heat that we can then convert into energy. Unlike beta and gamma decay, the slower-moving alpha particles stop in the material, making their energy available for use. Energy from these natural decay processes provides a reliable source of power. Spontaneous fission is rare and unreliable, and unlike induced fission processes, alpha decay occurs naturally and does not require external management or ignition. The ideal properties of an isotope for use as a power source depend upon the intended use. For use in an Arctic research base over a period of several years, but less than a decade, an isotope that provides high power output over a shorter lifespan may be the most suitable option. Whereas, for deep space missions where a consistent power source for decades or perhaps more than 100 years is needed that would require a very different isotope. One with a much longer half-life that would provide consistent power throughout that time and survive in that state in for these extended periods of time. These examples represent two extreme sides in terms of time frames. By analyzing the power produced by different radioactive decay processes over time, we can evaluate the suitability of various isotope decay chains for specific uses. Some unstable isotopes undergo a series of radioactive decays, transforming into different isotopes at each step and resulting in a stable isotope. The lists of isotopes in these decay processes are known as decay chains. Some of these chains, illustrated in the figures below, are currently being investigated for use in radioisotope thermoelectric generators (RTGs) designed for a range of operational durations.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Studies on the Mechanisms of Microbial Adaptation to the Physical Environment

The environmental factors which affect humans and other animals also influence the microorganisms which are such an important part of our ecology. Some of the microorganisms are very closely associated with animals, living in the digestive tract and synthesizing essential nutrients for the host. For these microbes, most external physical changes are of little consequence, because they are well shielded by the animals' homeostatic systems. The vast majority of microorganisms, however, live free in nature, especially in the soil and oceans. It has been estimated that the upper 15 cm of a fertile soil may contain over 4000 kg of bacteria and fungi per hectare. These organisms are responsible for degrading the complex molecules of plants and animals when they die, eventually producing simple organics, carbon dioxide, and inorganics, which are then used for the next cycle of plant growth. It is believed that over 90 % of the biologically produced carbon dioxide results from the metabolic activity of bacteria and fungi. In addition to recycling plant nutrients, soil bacteria also provide new nutrients through 'fixation' of atmospheric nitrogen into ammonia and nitrate, the forms which can be used by plants. Microorganisms so have an enormous capacity for detoxifying both natural and man-made poisons. All of these functions of microorganisms are essential to the operation of the material cycles on Earth. This is true of all locations on the planet, regardless of the climate or other environmental factors. In fact, one of the most impressive attributes of microorganisms is their ability to adapt to every stable environment on Earth. These include such extremes as polar regions, hot springs, water saturated with salt, mountain tops, ocean depths, acid and alkaline waters, deserts, intense radioactivity, soil and water contaminated with toxic chemicals or petroleum, and areas devoid of oxygen.

Heinrich, M. R.↗

Summary of Gas Generation Behavior Observed in 3013 Surveillance and Monitoring Program Shelf-Life Experiments

Gas generation experiments have been conducted in small- and full-scale test containers at Los Alamos National Laboratory on samples of plutonium oxide material collected from plutonium processes across the DOE complex and tested at the bounding conditions for the Department of Energy 3013 Standard. The gas composition and pressures in the sealed experimental containers were measured over periods of months to years. These experiments have provided results for the formation and consumption of hydrogen and other gases. The conditions supporting the formation of flammable gas mixtures of hydrogen and oxygen in flammable gas mixtures were also determined. Different behaviors were observed between the materials tested based on their compositions, the stabilization performed on the material, and the post stabilization handling of the material. Many of the experiments are still ongoing. This report summarizes the results obtained for the gas generation behavior for high-purity plutonium oxides and salt-bearing impure plutonium oxides in sealed containers.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Charpy Impact Characterization of Surveillance Specimens Harvested from Palisades High Fluence A-60 Capsule

Located on the shores of Lake Michigan, the Palisades Nuclear Generating Station (PNGS) was a nuclear power plant that operated in Covert Township, Michigan. The plant had a single pressurized water reactor that produced electricity for the region. The PNGS was shut down in 2022 after more than four decades of service. The PNGS included in its surveillance program a surveillance capsule, designated A-60, containing specimens of a weld metal with nickel content of about 1.36 wt% and copper content of about 0.25 wt%. The capsule was removed from its surveillance position in early 1995 and has been resident in the spent fuel pool since that time. This capsule was irradiated to a fluence of 1.96×10 20 n/cm 2 (E>1MeV) that is equivalent for more than 150 effective full power years (EFPYs) for the US reactor pressure vessel (RPV) fleet. The material is also of special interest because of its very high nickel content and potential for development of NiMnSi (nickel-manganese-silicon) precipitates. Combination of very high fluence and very high Ni and Cu content makes the material in this capsule of great interest as benchmark for currently developing embrittlement trend curves (ETC) aiming to predict embrittlement at high fluences. Multi-year efforts by the Light Water Reactor Sustainability (LWRS) Program personnel from the Materials Research Pathway (MRP) to harvest this capsule finally succeeded in 2023. As a result, the Westinghouse Electric Company (WEC) through contract with Oak Ridge National Laboratory (ORNL) came to PNGS site, retrieved the A-60 capsule, brought it to WEC Churchill hot cell facility, opened the capsule and sent all surveillance specimens in the capsule to ORNL for future characterization by July 2023. Total of 9 tensile and 48 Charpy specimens were inventoried in the ORNL hot cells. Testing plan has been developed based on available specimens. It includes hardness, tensile, Charpy impact, Mini-CT fracture toughness testing, in-situ thermal annealing, and microstructural characterization, including Atom Probe Tomography (APT). Charpy impact testing has been completed and results are presented in this report. Moreover, negotiations with Pressurized Water Reactors Owners Group (PWROG) and Westinghouse resulted in Westinghouse donating to ORNL a piece of archive weld and base metal such that unirradiated characterization of these materials can be performed as part of this project. Comparison of measured hardening and embrittlement has been performed and data are compared to available large database.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Coal Ash Beneficial Use at Savannah River Site

The Savannah River Site (SRS) has over 1.4 million cubic meters of coal ash and coal fines left over from coal-burning power plants that operated on site. Currently, the coal ash must be disposed of in an approved landfill or the coal ash-containing basins must be closed in place (i.e. consolidation, appropriate cover and liner system). Potential beneficial uses of the coal ash include geotechnical fill, such as backfill needed in the closure cap of the Z-area Saltstone Disposal Units (SDU), and use in cementitious material applications like thermal beneficiation or cement kiln feed, thereby reducing the environmental footprint of SRS. In this study, samples of coal ash from SRS were obtained and characterized for chemical and physical properties. Coal ash samples did not leach sulfates or heavy metals, so the coal ash is a candidate for geotechnical fill use. The samples also did not increase the acidity of the leachate during leaching tests, so it would not be detrimental to use as geotechnical fill near cementitious materials. The composition and energy potential of the coal ash makes it favorable for use as feed for external/off-site cement kilns or thermal beneficiation plants

01 COAL, LIGNITE, AND PEAT↗

129 I, 99 Tc, and U Distribution Coefficients of Subsurface Sediments Collected from the Proposed Site of the Environmental Management Disposal Facility

Performance Assessment calculations were completed in 2020 to evaluate the Environmental Management Disposal Facility (EMDF), a proposed new low-level radioactive waste (LLW) disposal facility on the U.S. Department of Energy’s Oak Ridge Reservation (ORR). Among the large number of input parameters needed for such calculations, are distribution coefficients (K d values; radionuclide concentration solid: liquid ratio) that provide a measure of the tendency of radionuclides to bind to sediments. The objective of this study was to measure K d values of three radionuclides that may pose a disproportionately large amount of risk, U, iodine-129 ( 129 I) and technetium-99 ( 99 Tc). The average 129 I K d value for the 14 geological materials recovered from the proposed EMDF site was 37.8 mL/g and ranged from 0.45 to 140.9 mL/g. These values were consistent, but somewhat larger than previous measurements made with ORR sediments and were about an order of magnitude greater than those used in previous EMDF PA calculations. The median 99 Tc K d value was 365.7 mL/g, much greater than previously reported using ORR geological materials. Five of the 14 tested geological materials sorbed large quantities of 99 Tc, suggesting that the weakly sorbing 99 Tc(VII) species had been reduced to the sparingly soluble 99 Tc(IV) species. The five strongly sorbing sediments had apparent 99 Tc solubility values of approximately <10 -8 mol/L. The median U K d value was 5,726 mL/g. All of the tested geological materials had large K d values, ranging from 625 to >10,208 mL/g. Among the sediment samples that exhibited strong U binding, the apparent solubility value was approximately <10 -9 mol/L. Based on sediment properties and general ORR geological considerations, it was proposed that much of the 129 I and 99 Tc retention could be attributed to the site materials exhibiting low pH (average pH = 4.94), and/or the elevated levels of iron oxides, manganese oxides, and natural organic matter. Similarly, the extremely high U binding measured in these sediments may also be attributed to the low conditions of carbonates, which can complex and therefore solubilize uranyl in these tests due to the low pH, and also the relatively high concentrations of iron and organic coatings on these samples. An implication of this study is that the areas of the EMDF subsurface environment may have natural properties for attenuating 129 I, 99 Tc, and U movement, and potentially other radionuclides, thereby possibly reducing risk posed by burial of LLW at this site.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Corrosion Testing of Refractory in Contact with Molten Glasses Designed for Waste Vitrification - HAL24 M1 Matrix Glasses

It is known that the predictive life of the refractory ceramic liner of nuclear waste glass melters is conservative, as demonstrated by performance of these materials such as in the Defense Waste Processing Facility (DWPF). The motivation for this task is to maximize the useful life of the melters that will be operated at the Waste Treatment and Immobilization Plant (WTP), which will in turn minimize procurement and disposal costs and melter outage times, as well as to identify maximum loadings in the waste glass of those species that corrode melter components. This task was initiated jointly with Pacific Northwest National Laboratory (PNNL) with the objective to develop a methodology and model to enable more accurate prediction of refractory service life under prototypic conditions from laboratory-scale material corrosion tests.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

The Effects of Beta Irradiation on the Performance of ATR Fiber Probes

The use of real-time inline monitoring to track the chemical composition of slurries is recognized as a promising method to reduce the processing time of Hanford tank waste. The conversion of waste into glass suitable for long-term storage requires adherence to waste acceptance criteria and process control limits that respectively ensure safe operation of the vitrification facility and suitable glass quality. Real-time measurements of blended waste materials can ensure that the various criteria are met or can be addressed in a timely manner.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Corrosion Testing of Refractory in Contact with Molten Glasses Designed for Waste Vitrification – VSL Touchpoint Matrix Glasses (Revision 1)

It is known that the predictive life of the refractory ceramic liner of nuclear waste glass melters is conservative, as demonstrated by performance of these materials such as in the Defense Waste Processing Facility (DWPF).[1] The motivation for this task is to maximize the useful life of the melters that will be operated at the Waste Treatment and Immobilization Plant (WTP), which will in turn minimize procurement and disposal costs and melter outage times, as well as to identify maximum loadings in the waste glass of those species that corrode melter components. This task was initiated jointly with Pacific Northwest National Laboratory (PNNL) with the objective to develop a methodology and model to enable more accurate prediction of refractory service life under prototypic conditions from laboratory-scale material corrosion tests.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Extinct radionuclides

Extinct radionuclides, or radioactive isotopes with lifetimes of the order of 1 to 100 Myr that are now extinct in the solar system are discussed. Evidence is presented for the presence of such radionuclides in the early solar system, including Al-26, Mn-53, Pd-107, I-129, Pu-244, and Sm-146. It is suggested that the abundances of these species provide constraints on nucleosynthetic time scales and the history of solar system materials before they became the solar system. The shortest-lived species is Al-26, which may have been sufficiently abundant to be the major heat source for meteorite parent-body metamorphism or igneous differentiation.

Podosek, F. A.↗

Monitoring Plan for the Idaho National Laboratory Remote Handled Low Level Waste Disposal Facility

This monitoring plan for Idaho National Laboratory’s Remote-Handled Low Level Waste Disposal Facility was developed to meet the requirements for monitoring low-level waste disposal facilities according to the U.S. Department of Energy (DOE) Order 435.1, “Radioactive Waste Management,” and the guidance provided in the associated technical standard “Disposal Authorization Statement and Tank Closure Documentation” (DOE-STD-5002-2017). The purpose of this monitoring plan is to document a monitoring strategy that includes (1) compliance monitoring activities to demonstrate compliance with regulatory standards/limits and (2) performance monitoring to build confidence the facility is performing as demonstrated in the facility performance assessment (PA) (DOE-ID 2018a), composite analysis (CA) (DOE ID 2012), and CA addendum (DOE-ID 2018b). The de minimus impact to the aquifer predicted by the PA suggests that aquifer compliance monitoring should be augmented with performance monitoring of the drainage course materials and sedimentary interbeds in the vadose zone beneath the facility to provide a more effective means of identifying performance deviations. The monitoring approach delineated in this document was informed by the systems evaluation of natural and engineered facility features presented in the PA, an assessment of aquifer baseline conditions (INL 2017d), the dose analysis conducted in support of the PA and CA, and monitoring data collected during the first four years of facility operations (baseline monitoring phase) (INL 2023b). This plan provides monitoring locations, sampling frequencies, and sampling methods; recommendations for data evaluation; and a description of the monitoring plan implementation. Collected data will be used to demonstrate facility compliance and to identify conditions that are not consistent with the key assumptions made by the PA and CA.

12 - MGMT OF RADIOACTIVE AND NON-RADIOACTIVE WASTE↗

Plutonium oxide melt structure and covalency

Advances in nuclear power reactors include the use of mixed oxide fuel, containing uranium and plutonium oxides. The high-temperature behaviour and structure of PuO 2-x above 1,800 K remain largely unexplored, and these conditions must be considered for reactor design and planning for the mitigation of severe accidents. Here, in this study, we measure the atomic structure of PuO 2-x through the melting transition up to 3,000 +/- 50 K using X-ray scattering of aerodynamically levitated and laser-beam-heated samples, with O/Pu ranging from 1.57 to 1.76. Liquid structural models consistent with the X-ray data are developed using machine-learned interatomic potentials and density functional theory. Molten PuO 1.76 contains some degree of covalent Pu-O bonding, signalled by the degeneracy of Pu 5f and O 2p orbitals. The liquid is isomorphous with molten CeO 1.75 , demonstrating the latter as a non-radioactive, non-toxic, structural surrogate when differences in the oxidation potentials of Pu and Ce are accounted for. These characterizations provide essential constraints for modelling pertinent to reactor safety design. The molten structure of plutonium oxide-a component of mixed oxide nuclear fuels-is measured, showing some degree of covalent bonding. Its atomic structure is similar to that of cerium oxide, which could be a non-radioactive structural surrogate.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Results of Long-Term Analyses of the Salt (Macro) Batch 11 Tank 21H Qualification Sample

Savannah River National Laboratory (SRNL) analyzed samples from Tank 21H in support of qualification of Salt Waste Processing Facility (SWPF) Salt Batch 11. This document reports the long-term results of the analyses of the sample of Tank 21H. Analysis of this sample indicates that the material does not display any unusual characteristics or observations, such as visually apparent solids. However, the sample was dark colored. This report satisfies Deliverable 3 of the Technical Task Request (TTR). This revision adds a further triplicate analysis for 129 I content.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Collection, analysis, and archival of LDEF activation data

Samples intentionally placed aboard the LDEF and samples obtained from the LDEF structure were studied at NASA Marshall and seven national labs to determine the radioactivity produced in orbit. The gamma ray spectra from these studies have provided information concerning the type and quantity of radioactive nuclei produced by various activating particles. The gamma ray spectra, the resulting activation, and the experimental arrangements are being collected at Marshall and Eastern Kentucky Univ. for review, further analysis, and future archival. An overview of this process and the type of information that will be available for future reference is given. This information includes the samples studied, the location of the samples on LDEF, the amount and type of covering material, the types of detector systems, the format of the gamma ray spectra, and the corrections for geometry, self-absorption, detector efficiency, and background needed to obtain accurate specific activations (activation per kilogram) of material. Plans are given as to the archival of the data for such future reference and how other scientific investigators or spacecraft designers can access the data.

Laird, C. E.↗

Analytical Results of the Tank 51H Sludge Batch 11 As-Received Qualification Sample

Savannah River National Laboratory (SRNL) has been requested by Savannah River Mission Completion (SRMC) to qualify the next sludge batch, Sludge Batch 11 (SB11), for processing at the Defense Waste Processing Facility (DWPF). This report documents the first steps of the qualification process, characterization of the Tank 51H as-received qualification material. SRMC sent SRNL two 200 mL samples received from Tank 51H on the 12th of August 2024. The combined sample, HTF-51-24-85/86, was analyzed for the following: supernate and slurry density, weight percent solids, settling, chemical composition, and radionuclides.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Uncertainty propagation and sensitivity analysis for constrained optimization of nuclear waste vitrification

Abstract The vitrification of high‐level waste (HLW) by heating a mixture of glass‐forming chemicals (GFCs) with the waste can be improved using a constrained optimization problem. This study explores how different uncertainty propagation (UP) methods implemented with the optimization process can affect the glass formulation of nuclear waste glasses. UP is the effort of propagating uncertain inputs through a system to understand and quantify output distributions. Uncertainty intervals are crafted from output distributions to inform the optimization algorithm. UP is often implemented with Monte Carlo (MC) sampling for large nonlinear systems, which can be difficult to implement within a constrained optimization algorithm that requires derivative information. Other UP methods often used for optimization under uncertainty (OUU) can be designed to work within an established constrained optimization framework. Methods of UP are evaluated in this study including iterative sampling approaches, first‐order approximations, and surrogate modeling with machine learning (ML). A method of dimensional reduction based on global sensitivity analysis is introduced to support the UP methods for the large dimensionality of the problem. Analytical UP methods able to achieve similar optimums 10 times faster than the baseline MC approach, and produce 93.9% similar output distributions are reported.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Data-driven background model for the CUORE experiment

Here, we present the model we developed to reconstruct the CUORE radioactive background based on the analysis of an experimental exposure of 1038.4 kg yr. The data reconstruction relies on a simultaneous Bayesian fit applied to energy spectra over a broad energy range. The high granularity of the CUORE detector, together with the large exposure and extended stable operations, allow for an in-depth exploration of both spatial and time dependence of backgrounds. We achieve high sensitivity to both bulk and surface activities of the materials of the setup, detecting levels as low as 10 nBq kg −1 and 0.1 nBq cm −2 , respectively. We compare the contamination levels we extract from the background model with prior radio-assay data, which informs future background risk mitigation strategies. The results of this background model play a crucial role in constructing the background budget for the CUPID experiment as it will exploit the same CUORE infrastructure.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Analytic models of the chemical evolution of galaxies

Techniques are described for constructing analytic models of the chemical evolution of galaxies subject to infall of metal-poor material onto a maturing disk. A class of linear models is discussed which takes the star-formation rate within a defined region to be proportional to the mass of interstellar gas within that region, and the instantaneous recycling approximation is adopted. The solutions are obtained by approximately matching the infall rate to parametrized familiies of functions for which the equations are exactly soluble. The masses, the primary and secondary metallicities, and the gas concentrations of radioactive chronometers can all then be analytically expressed. Surveys of galactic abundances in location and in time can be compared to the parameter spaces of the analytic representations.

Clayton, Donald D.↗