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At least 73 records · Page 4

Identifying chemically similar multiphase nanoprecipitates in compositionally complex non-equilibrium oxides via machine learning

Abstract Characterizing oxide nuclear fuels is difficult due to complex fission products, which result from time-evolving system chemistry and extreme operating environments. Here, we report a machine learning-enhanced approach that accelerates the characterization of spent nuclear fuels and improves the accuracy of identifying nanophase fission products and bubbles. We apply this approach to commercial, high-burnup, irradiated light-water reactor fuels, demonstrating relationships between fission product precipitates and gases. We also gain understanding of the fission versus decay pathways of precipitates across the radius of a fuel pellet. An algorithm is provided for quantifying the chemical segregation of the fission products with respect to the high-burnup structure, which enhances our ability to process large amounts of microscopy data, including approaching the atomistic-scale. This may provide a faster route for achieving physics-based fuel performance modeling.

36 MATERIALS SCIENCE↗

Where there is a wind, there is a way

A shift in USA energy policy from oil or natural gases to thermonuclear fission and solar energy is predicted. A massive diversified energy research and development effort to productively harness the energy in the winds is outlined to develop commercially feasible wind energy conversion systems - considered a form of solar energy - in the near future.

Mosher, C. A.↗

Dating native gold by noble gas analyses

Our recent work on He, Ne, and Ar in Alpine gold samples has demonstrated that gold is extremely retentive for He and could thus, in principle, be used for U/Th-He-4 dating. For vein-type gold from Brusson, Northern Italy, we derived a U/Th-He-4 age of 36 Ma, in agreement with the K-Ar formation age of associated muscovites and biotites. However, in placer gold from the Napf area, Central Switzerland, we observed large excesses of both He-4 and radiogenic Ar-40 (Ar-40 sub rad, defined as Ar-40-295.5-Ar-.36). The gas release systematics indicate two distinct noble gas components, one of which is released below about 800 C and the other one at the melting point of gold (1064 C). We now present results of He and Xe measurements in a 1 g placer gold sample from the river Kruempelgraben, as well as He and Ar data for Brusson vein-type gold and for gold from the Lily Gold Mine, South Africa. We calculate reasonable U/Th-He-4 as well as U-Xe ages based on those gases which are released at approximately 800 C. Probably the low-temperature components represent in-situ-produced radiogenic He and fission Xe, whereas the gases evolving when gold melts have been trapped during gold formation. Therefore, only the low-temperature components are relevant for dating purposes.

Niedermann, S.↗

The excess fission xenon problem in lunar samples

This paper presents noble-gas (neon, krypton, and xenon) data obtained in stepwise heating of five lunar breccias: 14063, 14082, 15205, 15405, and 15445. These data are discussed in terms of spallation gas content, cosmic-ray exposure ages, and content of fission xenon. None of these samples is rich in solar-wind gases, and none contains more fission xenon than would be expected for in situ fission of U-238 and Pu-244. The essential features of the excess-fission-xenon phenomenon seen in several Apollo 14 samples are reviewed, as are models which might account for this phenomenon and criteria by which these models may be evaluated. The lack of excess fission xenon in 14063 and 14082 eliminates models relying on microscale xenon redistribution. A model is proposed in which the excess fission xenon originates in local material and percolates through and is adsorbed on regolith material.

Drozd, R. J.↗

Computing the solubility of argon and xenon in molten sodium chloride and potassium chloride salts

Molten salt reactors (MSRs) offer significant advancements in nuclear reactor safety and efficiency by operating at higher temperatures and lower pressures compared to traditional reactors. A critical aspect of MSR operation involves understanding the solubility of fission byproducts, particularly noble gases, in the molten salts used. This study employs molecular dynamics (MD) simulations to compute Henry’s law constants and enthalpies of solvation for argon and xenon in molten sodium chloride (NaCl) and potassium chloride (KCl). We developed a new pairwise potential for the noble gas and salt interactions based on first principles calculations. We then used this potential to calculate Henry’s law constants of the two gases in the molten salts, which were modeled using both a rigid ion model (RIM) and a polarizable ion model (PIM). The solubility calculations, performed using the Widom insertion method, show qualitative agreement with limited experimental data, highlighting the temperature dependence and greater solubility of both gases in KCl compared to NaCl. Additionally, free volume analysis elucidated the role of available space within the molten salts in governing solubility trends. Our findings suggest that PIM trajectories provide more reliable predictions for noble gas solubility than RIM due to their accurate density representation. Furthermore, these results enhance understanding of gas solubility in MSR environments, and the methods can be readily extended to other systems.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

University of Florida nuclear pumped laser program

The mechanism of excitation of laser gases by fast ions (triton, proton, or fission fragments) and especially any role UF6 might play in radiative deexcitation of these gases were investigated. Population densities of excited important for laser action were obtained. Nuclear pumped CW-laser systems, especially He-Ne and CO2, were studied using steady state reactors. It was demonstrated that He-Ne lases in a CW-mode with nuclear pumping at both the red and the infrared transition. The infrared transition was observed to be superradiant.

Richard T. Schneider↗

The regolith history of 14307

Noble gas and trace element analyses of matrix and a clast from breccia 14307 are reported. This sample was exposed to a large neutron fluence, as seen by an elevated Sm-150/Sm-149 ratio and by noble gases, particularly Xe-136 from neutron fission of U-235. Strong constraints on the exposure history result from combined consideration of Sm-150, Xe-136, and spallation noble gases. Both clast and matrix were irradiated for about 1 AE under substantial shielding beginning at least 2 AE ago, probably more than 3 AE ago. The manifestations of soil exposure seen in the matrix - solar wind gases, glass formation, etc. - thus must have been acquired in an ancient epoch. The matrix has had a longer exposure to cosmic rays than the clast, presumably during its prebrecciation history as a soil. Brecciation probably occurred more than 1 AE ago, perhaps more than 3 AE ago, but at least 0.4 AE after the formation of the matrix constituents.

Bernatowicz, T.↗

Chemical Modeling of the Capture of Radioiodine Species

Iodine is a common fission product resulting from the transmutation of uranium fuel in nuclear power reactors. The short-lived radioactive isotope, 131 I, with a half-life of around eight days, would be a particular health concern if released into the environment. Capture materials, such as activated carbon, are used routinely in nuclear power plants and medical isotope production facilities to remove this hazard during normal operations to reduce emissions to acceptable levels. Iodine, unlike other common fission products such as noble gases, is challenging because of the wide range of molecular forms and oxidation states (from +VII in IF 7 to -I in iodide) that it displays, which can interconvert both in the gas phase and in the solution phase for example. The work in this project is focused on three computational tasks. In the first, we consider the binding of iodine-containing molecules of varying oxidation states to the major component of activated carbon – pristine graphene-like sheets. The second task focused on molecular binding and possible chemical transformations resulting from the reaction of molecular iodine with chemical functional groups on the edge of the graphene sheets or surface defects in the sheet itself. The final task was associated with radiolytic breakdown of 131 I to 131 Xe in iodine containing molecules and investigated the resulting molecular fragmentation process both in the gas phase and on the graphene-like surface. For each of the tasks, the intent was to learn about the thermodynamics and kinetics of the chemical transformations and use the calculations to provide parameters for input into kinetic models describing these processes for interpretation of experimental data in future work.

07 ISOTOPE AND RADIATION SOURCES↗

Excess fission xenon at Apollo 16

Results are reported of stepwise heating analyses of Xe and Kr in four Apollo 16 low-grade breccias: 60019, 60225, 60275, and 67455. All four samples contain significant amounts of solar wind gases and at least three contain excess fission Xe. This observation indicates that the excess fission Xe effect is global rather than local, i.e., results from moon-wide redistribution of fission Xe rather than local redistribution in KREEP-rich Apollo 14 material. It is suggested that the excess fission Xe phenomenon represents a temporal variation in the amount of fission Xe available for redistribution, that it is prominent in samples from both highland sites simply because they are older than mare sites, and that samples from these sites had experienced at least some of their surface exposure at an early epoch.

Bernatowicz, T. J.↗

Monitoring Xenon Capture in a Metal Organic Framework Using Laser-Induced Breakdown Spectroscopy

Molten salt reactor operation will necessitate circulation of a cover gas to remove certain evolved fission products and maintain an inert atmosphere. The cover gas leaving the reactor core is expected to contain both noble and non-noble gases, aerosols, volatile species, tritium, and radionuclides and their daughters. To remove these radioactive gases, it is necessary to develop a robust off-gas system, along with novel sensors to monitor the gas stream and the treatment system performance. In this study, a metal organic framework (MOF) was engineered for the capture of Xe, a major contributor to the off-gas source term. The engineered MOF column was tested with a laser-induced breakdown spectroscopy (LIBS) sensor for noble gas monitoring. The LIBS sensor was used to monitor breakthrough tests with various Xe, Kr, and Ar mixtures to determine the Xe selectivity of the MOF column. This study offers an initial demonstration of the feasibility of monitoring off-gas treatment systems using a LIBS sensor to aid in the development of new capture systems for molten salt reactors.

47 OTHER INSTRUMENTATION↗

Multiphase Species Transport Modeling for Molten Salt Reactors in the System Analysis Module: Generation, Decay, Deposition, and Extraction of Insoluble Fission Products

With the increase of interests in the design and deployment of advanced reactor systems, a desire for simulation tools supporting system analysis of reactor operation and safety is rising. Molten salt reactors (MSRs), one of the advanced reactor systems, utilize liquid fused salt fuel as both coolant and fuel. During operation, MSR generates insoluble fission products, including noble metals and gases. The buildup of these species in fuel salt presents safety concerns as they may deposit on surfaces of critical components and produce excessive decay heat, causing the failure of system components. Timely removal of these noble metals and gases would ensure the safe operation of the reactor system. The dynamic nature of salt fuel system, involving the generation, decay, deposition, and extraction of noble metals and gases, calls for robust species transport models to facilitate system analysis and monitoring, and design of efficient species removal components. This paper concentrates on the development of a computational framework for species transport, consisting of multiphase transport model formulation, mass transfer between phases, numerical implementation in MOOSE environment, verification through Method of Manufacture Solutions (MMS) and validation against experimental data from the Molten Salt Reactor Experiment (MSRE). Integrating this framework into the System Analysis Module (SAM) code further enhances SAM’s capabilities for advanced reactor analysis in the future.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Possible impacts of molten salt reactors on the International Monitoring System

Molten salt reactors (MSRs) are gaining support as many countries look for ways to increase power generation and replace aging nuclear energy production facilities. MSRs have inherently safe designs, are scalable in size, can burn transuranic wastes from traditional solid fuel nuclear reactors, can store excess heat in thermal reservoirs for water desalination, and can be used to produce medical isotopes as part of the real-time liquid-fuel recycling process. The ability to remove 135 Xe in real time from the fuel improves the power production in an MSR because 135 Xe is the most significant neutron-absorbing isotope generated by nuclear fission. Xenon-135, and other radioactive gases, are removed by sparging the fuel with an inert gas while the liquid fuel is recirculated from the reactor inner core through the heat exchangers. Without effective abatement technologies, large amounts of radioactive gas could be released during the sparging process. This work examines the potential impact of radioxenon releases on samplers used by the International Monitoring System (IMS) to detect nuclear explosions. Here, atmospheric transport simulations from seven hypothetical MSRs on different continents were used to evaluate the holdup time needed before release of radioxenon so IMS samplers would register few detections. Abatement technologies that retain radioxenon isotopes for at least 120 d before their release will be needed to mitigate the impacts from a molten salt breeder reactor used to replace a nuclear power plant. A holdup time of about 150 d is needed to reduce emissions to the average level of current nuclear power plants.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Payload dose rate from direct beam radiation and exhaust gas fission products

A study was made to determine the dose rate at the payload position in the NERVA System (1) due to direct beam radiation and (2) due to the possible effect of fission products contained in the exhaust gases for various amounts of hydrogen propellant in the tank. Results indicate that the gamma radiation is more significant than the neutron flux. Under different assumptions the gamma contribution from the exhaust gases was 10 to 25 percent of total gamma flux.

Capo, M. A.↗

Basic Energy Sciences Roundtable: Foundational Science to Accelerate Nuclear Energy Innovation

Energy security, availability, and reliability are among the greatest challenges facing the nation and the planet. An abundant potential source of energy resides in the fundamental atomic building blocks of the universe in the form of nuclear fission and fusion reactions. In fact, energy from nuclear fission currently provides the majority of the world’s zero-carbon electricity, and future fusion energy systems offer great promise; carbon-free nuclear energy technologies can be key to the world’s decarbonized energy future. Although contemporary fission systems use well-established technologies to supply safe and efficient baseload power, they could be more fuel efficient and less costly. Moving beyond massive light-water fission reactors to a variety of advanced nuclear systems—which will vary in size and operate in extremes of temperature, corrosivity, and other parameters—will place stringent conditions on materials and chemical systems. New demands will be placed on the coolants and solvents, the materials, and the monitoring tools used in these reactors. Fusion-based nuclear energy will require superior materials to withstand extremely high temperatures, plasma exposure, radiation damage, and implanted gases. The advantages associated with these new fission and fusion technologies will be realized only through continued advancements in the fundamental science underpinning our knowledge of the physics and chemistry of nuclear systems gained via improved experimental and computational methods. In July 2022, the U.S. Department of Energy’s Office of Basic Energy Sciences—in coordination with the Offices of Nuclear Energy, Fusion Energy Sciences, and Advanced Scientific Computing Research—held a virtual roundtable titled “Foundational Science to Accelerate Nuclear Energy Innovation” to discuss the scientific and technical barriers for advanced nuclear energy systems. Five priority research opportunities were identified to address these scientific and technical challenges and to accelerate progress toward the realization of next-generation fusion and fission energy systems. The foundational science gaps inhibiting the advancement of nuclear energy technologies are identified and tackled in five priority research opportunities. These opportunities pave the way to accelerate the development and ultimately the adoption of new nuclear energy systems. They include the fundamental aspects of ion-electron interactions; novel properties of next-generation coolants and solvents; interfacial dynamics, not only in solids, but in other aspects of nuclear reactors; novel operando and in situ monitoring and sensing; and artificial intelligence to accelerate condensed phases discovery. Building on the foundation established by previous Basic Energy Sciences workshops, these opportunities encompass recent advances in fundamental knowledge and focus on the experimental and computational methods needed to resolve major technical challenges for nuclear energy technologies. Through developing fundamental scientific insight as well as pushing the frontiers of modeling complex systems and probing the operation of materials and chemical systems in extreme environments, research motivated by the priorities identified here will further develop the promise, potential, and utilization of nuclear energy for a clean energy future.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Current Ground Test Options for Nuclear Thermal Propulsion (NTP)

About 20 different NTP engines/ reactors were tested from 1959 to 1972 as part of the Rover and Nuclear Engine for Rocket Vehicle Application (NERVA) program. Most were tested in open air at test cell A or test cell C, at the Nevada Test Site (NTS). Even after serious engine breakdowns of the reactor (e.g., Phoebus 1A), the test cells were cleaned up for other engine tests. The engine test stand (ETS) was made for high altitude (approximately 1 psia) testing of an NTP engine with a flight configuration, but still had the exhaust released to open air. The Rover/NERVA program became aware of new environmental regulations which would prohibit the release of any significant quantity of radioactive particulates and noble gases into the open air. The nuclear furnace (NF-1) was the last reactor tested before the program was cancelled in 1973, but successfully demonstrated a scrubber concept on how to filter the NTP exhaust. The NF-1 was demonstrated in the summer of 1972. The NF-1 used a 44MW reactor and operated each run for approximately 90 minutes. The system cooled the hot hydrogen exhaust from the engine with a water spray before entering a particle filter. The exhaust then passed through a series of heat exchangers and water separators to help remove water from the exhaust and further reduce the exhaust temperatures. The exhaust was next prepared for the charcoal trap by passing through a dryer and effluent cooler to bring exhaust temperatures close to liquid nitrogen. At those low temperatures, most of the noble gases (e.g., Xe and Kr made from fission products) get captured in the charcoal trap. The filtered hydrogen is finally passed through a flare stack and released to the air. The concept was overall successful but did show a La plating on some surfaces and had multiple recommendations for improvement. The most recent detailed study on the NTP scrubber concept was performed by the ARES Corporation in 2006. The concept is based on a 50,000 lbf thrust engine (approximately 1 GW) with a maximum burn time of 1 hour. The concept utilized lessons learned from NF-1. The strategy breaks down the exhaust into parallel paths to allow flexibility with engine size and mass flow of exhaust. Similar to NF-1, the exhaust is slowed down, cooled, filtered of particulates, filtered of noble gases, and then the clean hydrogen is flared to open air. Another concept proposed by Steve Howe (currently Director of the Center for Space Nuclear Research) to simplify the NTP exhaust filtering is to run the hydrogen exhaust into boreholes underground to filter the exhaust. The two borehole site locations proposed are at the NTS and at the Idaho National Laboratory (INL). At NTS, the boreholes are 8' diameter and 1200' deep. The permeability of hydrogen through the soil and its buoyancy will allow it to rise up through the soil and allow the filtering of noble gases and radioactive particulates. The exhaust needs to be cooled to 600C before entering the borehole to avoid soil glazing. Preliminary analysis shows a small buildup of back pressure with time which depends on permeability. Noble gases entering the borehole walls deep can take a long time before reaching the surface. Other factors affecting permeability include borehole pressure, water saturation, and turbulence. Also, a possible need to pump out contaminated water collected at the bottom of the borehole. At INL, the borehole concept is slightly different. The underground borehole has openings to the soil at special depths which have impermeable interbeds above the water table and below the surface to allow the exhaust to travel horizontal between the impermeable layers. Preliminary results indicate better permeability than at NTS. The last option is total containment of the exhaust during the test run. The concept involves slowing down the flow to subsonic in a water cooled diffuser. The hydrogen is burned off in an oxygen rich afterburner with the only products being steam, oxygen, and some noble gases. A heat exchanger and water spray pulls heat from the steam and lowers the temperature for condensation. The optimum ratio between the two is being investigated, with a goal to minimize the total volume of the water hold tanks. A water tank farm collects the contaminated water. The amount of water produced from burning the hydrogen is approximately 100,000 gallons (not including cooling water) for a 25k lbf engine operating for 50 minutes. Residual gases (e.g., oxygen and some noble gases) can be captured at cryogenic levels with a liquid nitrogen cooled dewar. After a few weeks post-test, the radiation levels can drop to more favorable levels before slowly draining each capture tank and using existing filters. With today's environmental regulations, the NTP exhaust is filtered to meet 10 mrem/year exposure to the general public (at a DOE site) or 100 mrem/year (via NRC when tested elsewhere), when natural background radiation exposure to the general public is 300- 600 mrem per year. The current society feels more comfortable with filtering even lower to as low as reasonably achievable (ALARA).

Gerrish, Harold P., Jr.↗

Sensitivity of time-dependent density functional theory to initial conditions

Time-dependent density-functional theory is mathematically formulated through nonlinear coupled time-dependent three-dimensional partial differential equations, and it is natural to expect a strong sensitivity of its solutions to variations of the initial conditions, akin to the butterfly effect ubiquitous in classical dynamics. Since the Schrödinger equation for an interacting many-body system is, however, linear and mathematically the exact equations of the density-functional theory reproduce the corresponding one-body properties, it would follow that the Lyapunov exponents are also vanishing within a density-functional theory framework. Whether for realistic implementations of the time-dependent density-functional theory the question of the absence of the butterfly effect and whether the dynamics provided is indeed a predictable theory was never discussed. At the same time, since the time-dependent density-functional theory is a unique tool allowing us to study the nonequilibrium dynamics of strongly interacting many-fermion systems, the question of predictability of this theoretical framework is of paramount importance. Here our analysis, for a number of quantum superfluid many-body systems (unitary Fermi gas, nuclear fission, and heavy-ion collisions) with a classical equivalent number of degrees of freedom O(10 10 ) and larger, suggests that its maximum Lyapunov exponents are negligible for all practical purposes.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

SATS Transient Fission Gas Release Test with Irradiated Fuel under Loss of Coolant Accident Conditions

The transient fission gas release (tFGR) during the temperature ramp associated with a loss-of-coolant accident (LOCA) in light-water reactors (LWRs) is likely a significant contribution to the total pressure in a fuel rod and may cause an unexpected rod burst. The lack of data related to tFGR continues to be a key gap in understanding LWR cladding burst behavior under LOCA conditions. To fully characterize this behavior, tFGR data must be collected from several different systems that can capture all relevant testing conditions. Oak Ridge National Laboratory (ORNL) has developed a system to measure the integral tFGR from irradiated fuel segments. This system was designed to integrate with the existing Severe Accident Test Station (SATS) and to build upon decades of experience capturing fission gas to characterize fuel behavior. The tFGR system consists of a sweep gas system to transport gases from the in-cell SATS apparatus to an out-of-cell fission gas detection system composed of a series of cold traps to capture the off-gas from the heating tests and a gamma spectrometry system to detect and measure 85 Kr. Initial system testing operations were completed during which 85 Kr collection and measurement were verified along with the ability to detect stable inert gases. A tFGR test with a high-burnup fuel specimen was successfully conducted by the in-cell SATS-tFGR system at ORNL. The posttest examination is under way, the result of which will be reported in FY24.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗