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At least 19 records

Tensioned metastable fluid detector sensing technology for multifarious-multiscale applications in the nuclear fuel cycle

The nuclear fuel cycle presents formidable 10 30+ multiscale challenges for high-efficiency spectroscopic sensing of alpha-neutron-fission radiation signatures amidst extreme gamma-beta radiation backgrounds at various stages of the cycle; it involves diverse arenas ranging from continuous/pulsed power production, security/safeguards, spent fuel, environmental remediation, and personnel health-dosimetry. This paper discusses the novel tensioned metastable fluid detector (TMFD) sensor technology. It discusses the results of studies demonstrating extreme (10 4 Sv/h) gamma-beta field blind high intrinsic efficiencies (80–100%) for neutron-alpha-fission radiation spectrometric detection. Example studies discussed in this paper include Neutron detection with spectroscopy; H*10 neutron radiation dosimetry upwards from ultra-low10 −2 µSv/h levels; Air and/or liquid-borne trace (10 –3 Bq/mL) quantity, 1 keV energy resolved alpha/fission spectroscopy for Rn/Po/U/Pu/Am environmental isotope assays at 106:1 (β:α) ratios; Directional-position enabled extended standoff tracking of neutron emitting (shielded/unshielded) special nuclear materials while stationary or moving at highway speeds; and, U.S. Department of Energy nuclear complex wide nuclear waste reprocessing, criticality safety, health physics, and environmental applications.

Alpha-fission-neutron spectrometry

Non-Equilibrium Actinide Radiation Chemistry and the Nuclear Fuel Cycle

Invited John and Naomi Fackler Lectureship in Chemistry and English seminar at Valparaiso University, IN, USA. Actinides are inherently unstable elements that frequently coexist with other radioisotopes, generating intense ionizing radiation fields that drive the formation of non-equilibrium oxidation states. These transient species exert a profound mechanistic influence on the radiation response of actinide-containing systems due to their unique redox chemistry. Despite their importance, they remain poorly understood, yet such insight is essential for advancing actinide science and accurately predicting radiation-driven behavior. Actinide separations—critical for nuclear energy technologies, strategic deterrence, space exploration, and nuclear medicine—depend on precise control of actinide oxidation states to recover targeted elements from complex matrices such as used nuclear fuel. However, during these processes, actinides, their coordination complexes, and the separation media are all exposed to intense, multicomponent (alpha, beta, gamma, etc.) radiation fields that can alter process efficiency, selectivity, and chemical stability. Understanding, controlling, and mitigating radiation-induced reactions is therefore key to innovating and optimizing next-generation separation technologies. This seminar will provide an overview of the nuclear fuel cycle and non-equilibrium actinide radiation chemistry in the context of recovering actinides from used nuclear fuel, with a particular emphasis on direct-dissolution–based reprocessing strategies. We will explore time-resolved electron pulse radiolysis and gamma dose accumulation studies to elucidate the molecular-level roles of radiation-driven, non-equilibrium actinide species in process performance and in the radiolytic stability of organic ligands used for actinide recovery. These insights offer new pathways for designing advanced separation methods and next-generation solvent systems, with broad implications for the future of the nuclear fuel cycle.

37 - INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL C

Radiation Chemistry and the Nuclear Fuel Cycle

This presentation will give a general overview of radiation chemistry in the nuclear fuel cycle, and outline some relevant work being conducted in the INL Radiochemical Separations and Radiation Science Department. This will include a discussion of using multiscale modeling to study plutonium radiation chemistry in nitric acid solutions. (Presentation cancelled)

38 - RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCL

Backend Nuclear Fuel Cycle Radiation Chemistry

Given global commitments to significantly increase nuclear energy capacity, it is now more important than ever to develop efficient used nuclear fuel management strategies to improve resource utilization, energy security, and waste minimization. Here, an overview of nuclear energy, backend fuel cycle challenges, and advances in used nuclear fuel reprocessing radiation chemistry will be presented. More specifically, the use of electron pulse irradiation techniques to explore radiation-induced reaction mechanisms in actinide containing solutions and solvent systems.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA

Non-Equilibrium Actinide Radiation Chemistry and the Nuclear Fuel Cycle

Actinides are inherently unstable elements that frequently coexist with other radioisotopes, generating intense ionizing radiation fields that drive the formation of non equilibrium oxidation states. These transient species exert a profound mechanistic influence on the radiation response of actinide containing systems due to their unique redox chemistry. Despite their importance, they remain poorly understood, yet such insight is essential for advancing actinide science and accurately predicting radiation driven behavior. Actinide separations—critical for nuclear energy technologies, strategic deterrence, space exploration, and nuclear medicine—depend on precise control of actinide oxidation states to recover targeted elements from complex matrices such as used nuclear fuel. However, during these processes, actinides, their coordination complexes, and the separation media are all exposed to intense, multicomponent (alpha, beta, gamma, etc.) radiation fields that can alter process efficiency, selectivity, and chemical stability. Understanding, controlling, and mitigating radiation induced reactions is therefore key to innovating and optimizing next generation separation technologies. This seminar will provide an overview of the nuclear fuel cycle and non equilibrium actinide radiation chemistry in the context of recovering actinides from used nuclear fuel, with a particular emphasis on direct dissolution–based reprocessing strategies. We will explore time resolved electron pulse radiolysis and alpha and gamma dose accumulation studies, integrated with multiscale computational modeling, to elucidate the molecular level roles of radiation driven, non equilibrium actinide species in process performance and in the radiolytic stability of organic ligands used for actinide recovery. These insights offer new pathways for designing advanced separation methods and next generation solvent systems, with broad implications for the future of the nuclear fuel cycle.

37 - INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL C

Comparison of Gas Phase Fragmentation Behaviors of Nuclear Fuel Cycle Ligands in Lanthanide and Americium Metal Ligand Nitrate Clusters

Title (20 word): Comparison of Gas Phase Fragmentation Behaviors of Nuclear Fuel Cycle Ligands in Lanthanide and Americium Metal Ligand Nitrate Clusters Introduction (120 words): Transport of metal ions across the aqueous-organic phase boundary is an essential step in a hydrometallurgical nuclear fuel reprocessing strategy. The study of transport agents for nuclear fuel elements is imperative to guide the design of ligands that boost the separation efficiency of the recovery process from fission products. However, limited studies have been made on the chemistry of these transport agents when complexing with transuranic elements in gas-phase where all surrounding factors are essentially excluded. This work investigates the reagent ligand complexations to transuranic and other metals and their dissociations in the gas phase. Comparisons are made between 4f and 5f elements and between ligands. Methods (120 words): (N,N-diisobutylcarbamoylmethyl)phenyloctylphosphine oxide (CMPO) and N,N,N',N'-tetraoctyldiglycolamide (TODGA) have been selected to complex with metal nitrates. The actinide americium and lanthanides neodymium, samarium, and europium were investigated as part of this work. The lanthanides were selected to act as size and electron configuration analogues of the minor actinides. Metal complexes with two ligands and two nitrates ([M(NO3)2(CMPO)2]+, for example) are studied in Bruker micrOTOF-Q II mass spectrometer equipped with collision-induced dissociation capability. The comparisons of the mass spectra are made in groups of homogenous ligands and mixed TODGA-CMPO ligands clusters. Comparisons are also made based on the complexed metals (Am and lanthanides). Preliminary data (300 words): Collision-induced dissociation mass spectrometry data are collected on two ligands complexed with metal nitrates where the two ligands are homogenous, with (CMPO)2 or (TODGA)2, or heterogeneous, with (TODGA)(CMPO). Several fragmentation patterns are observed among complexes with the CMPO ligand whereas the TODGA ligand commonly dissociates intact from the complex. Most of the metal complexes exhibit similar fragmentation patterns, but there are a few notable deviations in fragmentation patterns between the Am and Ln-bearing complexes. For the [M(CMPO)2(NO3)2]+ complexes, the initial loss of nitrate in the form of nitric acid is observed in all four complexes. However, [Am(CMPO)2(NO3)2]+ exhibits an additional fragmentation not found in the lanthanide complexes. Also, a significantly different ratio of the second nitric acid loss is found in the Am complex. These deviations may indicate the different interaction behaviors between actinides and lanthanides. The [M(TODGA)2(NO3)2]+ complexes exhibit the fragmentation as the loss of one TODGA ligand as an intact form and the loss of nitrate as nitric acid. The Am complex exhibits an additional fragmentation after losing the TOGDA ligand, which is not observed among the Ln complexes. The heterogeneous [M(TODGA)(CMPO)(NO3)2]+ complexes exhibit both similarities and differences between the Am and Ln complexes. For example, the heterogenous Am complex does not exhibit the loss of an intact TODGA ligand while all three Ln complexes do. This indicates that TODGA may bind more strongly to Am than Ln. Additionally, the intensity of the loss of CMPO ligand (as partially or whole) is found to be significantly larger than that of the loss of TODGA (as partially of whole) indicating that TODGA is bound to the metal significantly stronger than CMPO. Planned computational analysis will help understand the deviation in fragmentation behaviors between americium and lanthanide metal centers, or between TODGA and CMPO ligands. Novel aspect (20 words): Gas-phase actinide and lanthanide complex formation and fragmentation provide insight into the coordination environment differences of f-element metals.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH

An analysis of the back end of the nuclear fuel cycle with emphasis on high-level waste management, volume 1

The programs and plans of the U.S. government for the "back end of the nuclear fuel cycle" were examined to determine if there were any significant technological or regulatory gaps and inconsistencies. Particular emphasis was placed on analysis of high-level nuclear waste management plans, since the permanent disposal of radioactive waste has emerged as a major factor in the public acceptance of nuclear power. The implications of various light water reactor fuel cycle options were examined including throwaway, stowaway, uranium recycle, and plutonium plus uranium recycle. The results of this study indicate that the U.S. program for high-level waste management has significant gaps and inconsistencies. Areas of greatest concern include: the adequacy of the scientific data base for geological disposal; programs for the the disposal of spent fuel rods; interagency coordination; and uncertainties in NRC regulatory requirements for disposal of both commercial and military high-level waste.

Source record

Neutron Total Scattering Analysis of Materials for the Nuclear Fuel Cycle

Here, this paper reviews recent experimental efforts at the University of Tennessee and Oak Ridge National Laboratory to comprehensively characterize the structural details of materials relevant for the nuclear fuel cycle by employing advanced neutron scattering techniques. For the study of nuclear ceramics, neutron scattering offers distinct advantages over traditional laboratory or synchrotron X-ray diffraction, including enhanced sensitivity to elements with a low atomic mass, such as oxygen, nitrogen, and carbon. The key to these efforts is the recent advancement in the neutron scattering infrastructure at the high-flux diffractometers at the Spallation Neutron Source. The high neutron flux at these instruments enables neutron total scattering, a nondestructive bulk technique that simultaneously captures both short-range structural effects through pair distribution function analysis and long-range order through diffraction pattern analysis. This approach is particularly important for a comprehensive description of defective, disordered, or amorphous nuclear materials. The case studies presented here include analyses of the local defect structure in hyperstoichiometric uranium oxides and short-range order of ion-irradiated ceramics. This advanced analytical methodology will improve our understanding of the behavior of materials in extreme environments and contribute to the development of more resilient nuclear materials.

Neutron scattering

Nuclear Fuel Cycle and Supply Chain (NFCSC) Technical Monthly September FY-24

AFC hosted the Light Water Reactor (LWR) Fuels Research Workshop and Electric Power Research Institute (EPRI) Collaborative Research on Advanced Fuel Technologies (CRAFT) Meeting September 9-13, 2024. The Department of Energy's (DOE) Advanced Fuels Campaign (AFC) Accident Tolerant Fuel (ATF) program is pivotal in advancing clean energy through collaborative innovation in fuel technology for light water reactors (LWRs). For over a decade, AFC has engaged a wide array of stakeholders—researchers, industry participants, and regulatory bodies—both within the U.S. and internationally to develop ATF technology. This initiative aims to enhance the safety and economic performance of both Pressurized Water Reactors (PWRs) and LWRs. To foster community relationships and disseminate research, AFC initiated annual LWR Fuel workshops in 2024, supplementing ongoing industry-led CRAFT workshops.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS

Oxygen stable isotopes in the nuclear fuel cycle: Assessment of the potential for determining the fabrication and provenance history of anhydrous and hydrous uranium oxides

Determining the origin and history of interdicted nuclear materials is a central challenge in nuclear forensics. The oxygen stable isotope composition of uranium oxide compounds has emerged as a promising forensic signature, attracting increasing attention since the early 2000s. This review examines analytical techniques for measuring oxygen isotope compositions in uranium oxides and evaluates how the nuclear fuel production cycle introduces or modifies these isotopic signatures. The potential for forensic geolocation is explored through workflows that calibrate the relationship between environmental water oxygen isotopes and those found in uranium oxides. Key strengths and limitations of this approach are assessed, including gaps in knowledge related to isotope fractionation during specific stages of the fuel cycle, and processing facility water inputs. The importance of proper sample handling and storage under inert atmospheres, as well as a deeper understanding of both intra-sample oxygen isotope heterogeneity, and hydrous uranium oxide phase formation, is highlighted for improving the reliability of forensic interpretations. In conclusion, the development of uranium oxide standards with well-characterized δ 18 O values and international collaboration toward consensus on their use are identified as essential steps for advancing the field.

Attribution

Recent Advances in Cladding Material Extraction from Fuels in Nuclear Fuel Cycles

An improved recycling and recovery process for the cladding material from spent nuclear fuels is very important toward confirming nuclear energy to support ongoing sustainable development of nuclear management by reducing waste and conserving resources. Nuclear spent fuel cladding materials such as zirconium alloys have economic values and can be recovered, and their recovery eliminates problems in waste disposal and conserves valuable resources. Over 110 published reports and journal articles are reviewed and summarized herein, with a main focus on documenting recovery techniques used to recover cladding materials from spent nuclear fuel and recent developments. Several recovery techniques which are used at present times, such as mechanical separation, chemical dissolution, and hydrometallurgical processes have been covered with examples and discussions. Difficulties within the recovery process are also discussed, and most probable areas for future research in improving efficiency and sustainability of recovering cladding material are identified and discussed at the end. Here, this review could be an important document to the field of spent nuclear fuel reprocessing, recovering valuables and thereby offering guidance on how to effectively manage, safely handle, and reduce nuclear waste. In addition to reducing the volume and radiotoxicity of high-level waste, this review also highlights the potential economic benefit of recovering zirconium from spent fuel cladding by relating typical zirconium metal prices to the mass of cladding per tonne of spent fuel, illustrating that the recoverable material value is non-negligible compared with back-end fuel-cycle costs.

Mondal, Kunal [Oak Ridge National Laboratory (ORNL

Comparison of Gas Phase Fragmentation Behaviors of Nuclear Fuel Cycle Ligands in Lanthanide and Americium Metal Ligand Nitrate Clusters

Introduction (120 words): Transport of metal ions across the aqueous-organic phase boundary is an essential step in a hydrometallurgical nuclear fuel reprocessing strategy. The study of transport agents for nuclear fuel elements is imperative to guide the design of ligands that boost the separation efficiency of the recovery process from fission products. However, limited studies have been made on the chemistry of these transport agents when complexing with transuranic elements in gas-phase where all surrounding factors are essentially excluded. This work investigates the reagent ligand complexations to transuranic and other metals and their dissociations in the gas phase. Comparisons are made between 4f and 5f elements and between ligands. Methods (120 words): (N,N-diisobutylcarbamoylmethyl)phenyloctylphosphine oxide (CMPO) and N,N,N',N'-tetraoctyldiglycolamide (TODGA) have been selected to complex with metal nitrates. The actinide americium and lanthanides neodymium, samarium, and europium were investigated as part of this work. The lanthanides were selected to act as size and electron configuration analogues of the minor actinides. Metal complexes with two ligands and two nitrates ([M(NO3)2(CMPO)2]+, for example) are studied in Bruker micrOTOF-Q II mass spectrometer equipped with collision-induced dissociation capability. The comparisons of the mass spectra are made in groups of homogenous ligands and mixed TODGA-CMPO ligands clusters. Comparisons are also made based on the complexed metals (Am and lanthanides). Preliminary data (300 words): Collision-induced dissociation mass spectrometry data are collected on two ligands complexed with metal nitrates where the two ligands are homogenous, with (CMPO)2 or (TODGA)2, or heterogeneous, with (TODGA)(CMPO). Several fragmentation patterns are observed among complexes with the CMPO ligand whereas the TODGA ligand commonly dissociates intact from the complex. Most of the metal complexes exhibit similar fragmentation patterns, but there are a few notable deviations in fragmentation patterns between the Am and Ln-bearing complexes. For the [M(CMPO)2(NO3)2]+ complexes, the initial loss of nitrate in the form of nitric acid is observed in all four complexes. However, [Am(CMPO)2(NO3)2]+ exhibits an additional fragmentation not found in the lanthanide complexes. Also, a significantly different ratio of the second nitric acid loss is found in the Am complex. These deviations may indicate the different interaction behaviors between actinides and lanthanides. The [M(TODGA)2(NO3)2]+ complexes exhibit the fragmentation as the loss of one TODGA ligand as an intact form and the loss of nitrate as nitric acid. The Am complex exhibits an additional fragmentation after losing the TOGDA ligand, which is not observed among the Ln complexes. The heterogeneous [M(TODGA)(CMPO)(NO3)2]+ complexes exhibit both similarities and differences between the Am and Ln complexes. For example, the heterogenous Am complex does not exhibit the loss of an intact TODGA ligand while all three Ln complexes do. This indicates that TODGA may bind more strongly to Am than Ln. Additionally, the intensity of the loss of CMPO ligand (as partially or whole) is found to be significantly larger than that of the loss of TODGA (as partially of whole) indicating that TODGA is bound to the metal significantly stronger than CMPO. Planned computational analysis will help understand the deviation in fragmentation behaviors between americium and lanthanide metal centers, or between TODGA and CMPO ligands. Novel aspect (20 words): Gas-phase actinide and lanthanide complex formation and fragmentation provide insight into the coordination environment differences of f-element metals.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH

Experimental Investigation of Vibratory Stresses in a Concentric-Ring Direct-Air-Cycle Nuclear Fuel Element

Preliminary tests made by the General Electric Company indicated that aerodynamic loads might cause large enough distortions in the thin sheet-metal rings of a nuclear fuel element to result in structural failure. The magnitude of the distortions in a test fuel element was determined from strains measured with airflow conditions simulating those expected during engine operation. The measured vibratory strains were low enough to indicate the improbability of failure by fatigue. A conservative estimate of the radial deflection that accompanied peak strains in the outer ring was +0.0006 inch.

Chiarito, Patrick T.

Life‐cycle greenhouse gas emissions associated with nuclear power generation in the United States

Under the 2022 Inflation Reduction Act, tax credits of up to $3/kgH 2 are available to hydrogen producers if they generate emissions at levels below 0.45 kgCO 2 e/kgH 2 , spurring producers to explore how hydrogen production via electrolysis using electricity generated by nuclear power may qualify for such tax credits. With uranium as a primary fuel for nuclear power plants (NPPs) and no on-site emissions, the upstream emissions associated with nuclear fuel supply chains largely determine the carbon intensity of nuclear energy. Using the GREET (Greenhouse gases, Regulated Emissions, and Energy use in Technologies) model, we evaluated the life-cycle greenhouse gas (GHG) emissions of uranium production and the use of uranium to generate electricity in light water reactor (LWR) NPPs. We evaluated the process chemicals and energy inputs throughout the nuclear fuel supply chain to identify the major contributors to nuclear fuel cycle GHG emissions. Such emissions are estimated at 3.0 gCO 2 e/kWh at NPPs in the United States. The greatest share of nuclear fuel cycle GHG emissions—comprising 53% of total emissions—are associated with electricity consumption throughout the fuel supply chain. We extended the analysis to include an evaluation of the carbon intensity of H 2 production via electrolysis using nuclear power from LWRs. Finally, we examined the impact of future (2035 and 2050) electricity supply chain scenarios on nuclear fuel cycle GHG emissions. Our analysis revealed a decrease of 33% (2035) and 46% (2050) in the carbon intensity of nuclear electricity relative to current nuclear fuel cycle GHG emissions.

greenhouse gas emissions

Field Testing of Safeguards Technologies in the Hot Fuel Examination Facility

Recent developments in nuclear fuel reprocessing techniques have yielded more efficient processes and fuel cycle options that strengthen the nuclear industry and production of clean energy. One such area of interest is pyroprocessing of used oxide fuel. However, with these advances in the back end of the nuclear fuel cycle, advances in safeguards instrumentation, measurements, and approaches are needed to ensure special nuclear material (SNM) is accounted for according to regulatory requirements. As a high-level overview of a nominal pyroprocessing approach, used oxide fuel from commercial light water reactors (LWR) is mechanically removed from the metallic cladding. Then the fuel is crushed and randomized representative samples are taken and sent to an analytical lab for analysis. The analytical results of the feed material are used for input accountancy into the rest of the process. The crushed oxide fuel is then moved to the oxide reduction (OR) furnace where it is reduced from an oxide to metallic form. The OR product is distilled to remove salt and then moved to an electrorefiner (ER), where it is immersed in a eutectic mixture of lithium chloride potassium chloride (LiCl-KCl) that typically ranges between 450-550 ?. Within the ER, the usable uranium is electrochemically transported through the molten salt from the anode to the cathode, and then subsequently removed as a relatively pure U product.. A simplified model of pyroprocessing techniques with added emphasis on the safeguards can be seen below in Fig. 1

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS