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DOE OSTI2025

Quantifying the Economic Impacts of Managing Irradiated High-Assay Low-Enriched Fuel

Commercial nuclear power plants typically use nuclear fuel that is enriched up to five weight percent in the isotope 235 U. However, recently several vendors have proposed new nuclear power plant designs that would use fuel with 235 U enrichments between five weight percent and 19.75 weight percent. Nuclear fuel with this level of 235 U enrichment is known as “high assay low-enriched uranium.” Once it has been irradiated in a nuclear reactor and becomes used (or spent) nuclear fuel, it will be stored, transported, and disposed of. However, irradiated high assay low-enriched uranium fuel differs from typical irradiated nuclear fuel in several ways, and these differences may have economic effects on its storage, transport, and disposal, compared to typical irradiated nuclear fuel. A previous report described these differences qualitatively (Price et al., 2024); this report builds on the previous report and provides quantitative estimates of the potential economic effects on storage, transport, and disposal of high assay low-enriched uranium spent fuel.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2021

Gas-phase stability of large lanthanide:diglycolamide clusters evaluated using collision-induced dissociation

Efficient utilization of long-term deep geologic storage repositories is critical for the large-scale deployment of nuclear energy. As the minor actinides (americium and curium) are the largest contributor to the decay heat of used nuclear fuel after a few hundred years, their removal from used fuel prior to disposal can significantly increase the amount of waste that can be stored in a given volume. The development of ligands that can effectively separate the minor actinides from other components of used nuclear fuel are crucial to efficient utilization of geological storage repositories. N,N,N’,N’-tetraoctyl diglycolamide (TODGA) is a promising extractant for the separation of lanthanides and the minor actinides from other components of used nuclear fuel. While the use of TODGA in f-element separations has been investigated in process-based formulations, gas-phase metal ion cluster experiments enable the study of covalent interactions in reprocessing systems absent from solvent effects. Exploring fundamental differences in lanthanide-ligand covalent interactions can impact the development and implementation of actinide-lanthanide separation systems in nuclear fuels reprocessing. In this study, lanthanide-TODGA clusters were synthesized in the gas-phase and identified using mass spectrometry fragmentation experiments. Large europium and samarium clusters were identified that contained up to 8 and 10 bound TODGA ligands, respectively; this was surprising due to the size and multidentate binding that is normal for TODGA. In addition, while smaller clusters showed evidence of sequential ligand fragmentation, larger clusters displayed the loss of neutral TODGA with applied collision voltage. Interestingly, the voltage required for this removal decreased as more TODGA ligands were bound to the metal, suggesting that the metal coordination sphere was becoming more saturated and TODGA ligands were more weakly bound as the clusters got larger.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2020

Radiation Chemistry Research for Improved Nuclear Fuel Cycles

Nuclear energy is a key component of a global, low-carbon energy future. One of the challenges facing large-scale deployment of nuclear power is the long-term disposition of used nuclear fuel. Due to the political and technical challenges of siting deep geologic storage facilities, reprocessing of used nuclear fuel is desirable to reduce the total volume and decay heat of waste requiring long-term storage, enabling efficient usage of geologic storage repositories. However nuclear fuel reprocessing is complicated by intense multi-component radiation fields that degrade solvent systems that are used for this purpose. Resulting radiolytic degradation can result in reduced performance over time, and generation of additional waste. Thus, an understanding of the radiation-induced chemistry of these reprocessing solvent systems is crucial to for the development of new, radiation-resistant processes for efficiently treating used nuclear fuel. Controlled irradiation experiments combined with high-performance chromatography and mass spectrometry have provided comprehensive knowledge of radiolytic degradation pathways and kinetics, which is needed to predict the effect of radiation-induced chemistry on the performance of the nuclear fuel reprocessing technology. This talk will give an overview of recent progress in research on the radiation chemistry of fuel reprocessing molecules conducted by the Idaho National Laboratory Center for Radiation Chemistry Research (CR2) in conjunction with the Molecular Mass Spectrometry and Chromatography group.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2022

Suppressed thermal conductivity in hyperstoichiometric uranium dioxide controlled by phonon lifetimes

Thermal transport in nuclear fuels used for nuclear energy applications is directly tied to performance and reliability. Uranium dioxide (UO 2 ), one of the most important nuclear fuels, can accumulate excess oxygen atoms as interstitial defects, which significantly impacts thermal transport properties. In this study, thermal conductivities and inelastic neutron scattering (INS) measurements on UO 2+ x were performed at low temperatures (2–300K). The thermal conductivity of UO 2+ x (x = 0, 0.03, 0.04, and 0.11) is significantly suppressed compared to UO 2 except near the Néel temperature T N = 30.8 K, where it is independent of x. INS measurements demonstrate that the heat capacities and phonon group velocities of UO 2 and UO 2.08 are similar, and the suppressed thermal conductivity results from smaller phonon lifetimes. These perceptions advance our understanding of thermal transport properties in advanced nuclear fuels and guide safe and economic utilization of nuclear energy.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2024

Economic Impacts of Irradiated High Assay Low-Enriched Uranium Fuel Management

Commercial nuclear power plants typically use nuclear fuel that is enriched to less than five weight percent in the isotope 235 U. However, recently several vendors have proposed new nuclear power plant designs that would use fuel with 235 U enrichments between five weight percent and 19.75 weight percent. Nuclear fuel with this level of 235 U enrichment is known as “high assay low-enriched uranium.” Once it has been irradiated in a nuclear reactor and becomes used (or spent) nuclear fuel, it will be stored, transported, and disposed of. However, irradiated high assay low-enriched uranium differs from typical irradiated nuclear fuel in several ways, and these differences may have economic effects on its storage, transport, and disposal, compared to typical irradiated nuclear fuel. This report describes those differences and qualitatively discusses their potential economic effects on storage, transport, and disposal.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2025

Chloride-Based Volatility for Waste Reduction and/or Reuse of Metallic-, Oxide- and Salt-Based Reactor Fuels

The objective of the chloride based volatility project (CBV) was to demonstrate the ability to separate uranium from used fuel to enable process improvements resulting in 10x reduction of waste volume, while maintaining safeguards standards and global backend costs at $\$$1/MW-hr. Current industrial practices perform separations of used fuel using solvent media in the form of aqueous and molten salt processes, resulting in contaminated process waste. The CBV approach utilized solid state chemistry with no solvent media and was successful in chlorinating uranium and fission product oxides that sublimed into the gas phase and were collected in targeted condensation zones based on temperature gradients of chlorinated products. Recovery of better than 95% of initial uranium in the form of UCl4 was demonstrated when simulated used nuclear fuel was used. Laser induced breakdown spectroscopy, LIBS, and ultraviolet-visible spectroscopy, UV-Vis, were combined into a high temperature flow cell design and utilized as process monitoring techniques to observed chlorinated products leave the reaction vessel in real time.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2025

Real-Time Automated pH Control within Batch Processes Relying on Raman pH Measurement

Nuclear fission is an energy source that can provide consistent power with very low associated carbon emissions. However, management of the used nuclear fuel is an important aspect of the application of nuclear power. Recycling of useful components from used fuel is an attractive option, but this involves chemical processing of the fuel. Possible chemical separation technologies that might be used in this regard are sensitive to solution pH. Raman spectroscopy is a promising technique for monitoring the pH of solutions in real time. Classical pH probes are too fragile to be used in the harsh environments encountered in nuclear fuel processing. Raman probes are robust and can withstand these harsh environments to track pH. Coupled with chemometric analysis, the demonstration of the use of Raman spectroscopy to track and predict the pH in carboxylate-buffered systems is made possible. Utilizing this spectroscopy in conjunction with Programmable Logic Controllers mimics industrial control systems used in many modern industrial settings. This showcases a pragmatic approach toward leveraging Raman spectroscopy and chemometric model outputs as inputs for a real-time control system. The model to predict pH created by chemometrics proved to be successful in tracking pH. The optimal pH for TALSPEAK extraction of lanthanides and actinides from aqueous solution is known to proceed in a narrow pH range of around pH = 2.8 ± 0.1. This study uses Raman optical monitoring and automated control to return and maintain solution pH within this range after acid or base perturbations move the solution pH well outside this region. Root-mean-square errors show that pH changes measured using Raman spectroscopy on the batch process solution are reliably measured and used to automatically correct and maintain solution pH. Measurement of solution pH tracks favorably with electrochemical pH probe comparison measurements. As a result, the ability to showcase Raman spectroscopy paired with chemometrics analysis acts as a durable, better alternative data source compared to traditional pH probes to optimize the separation efficiency in the used nuclear fuel processing.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

The Role of Pulse Radiolysis in Advanced Nuclear Fuel Cycles

The effects of ionizing radiation are ubiquitous throughout all aspects of a nuclear fuel cycle. The complexity and intensity of these effects are greatest during reactor operations and in the management of used nuclear fuel and waste. Radiation-induced processes typically promote the chemical transformation of molecules and materials with the formation of potentially detrimental degradation products and corresponding changes in physical and chemical properties, which ultimately impact the effectiveness and longevity of nuclear technologies. Consequently, a molecular-level understanding of radiation effects over multiple time, distance, and material domains is essential for the innovation and deployment of next generation nuclear technologies. Attaining this knowledge necessitates a firm grasp of radiation-induced reaction kinetics, for which pulsed electron radiolysis is the methodology of choice. Presented here are several recent studies from our group that demonstrate the critical role of pulsed electron radiolysis techniques in the advancement of our understanding of radiation-induced chemistry under advanced nuclear fuel cycle conditions. Research topics include late actinide redox chemistry, radiation robustness of used nuclear fuel reprocessing complexants, and the behavior of metal cations in high temperature molten salt media.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2025

Non–linear bonding trends in maleonitrile-1,2–dithiolate complexes of the transuranium actinides

The trivalent actinides are produced in the nuclear fuel cycle during power production and provide the largest long-term radiation dose in used nuclear fuel. It is ideal for these elements to be removed from used nuclear fuel for disposal and a necessity for fuel recycling. A key challenge to this is the similarity of chemical behavior of the trivalent actinides to the lanthanides that are also present as fission products in used fuel. Thus far, some of the most effective separations of actinides from lanthanides utilise chelating agents containing sulfur moieties such as dithiophosphinates that selectively bind to actinide ions because of a greater bond covalency relative to lanthanide ions. Typically, greater differences between actinide and lanthanide ions are observable the more ligands and chelators bonds have a covalent character. Here, a series of complexes of the trivalent actinides Np(III) through Cf(III) (excluding Bk(III)) with maleonitrile-1,2-dithiolate (mnt 2– ) are synthesized along with their lanthanide counterparts (La(III) – Nd(III), Sm(III) – Gd(III), Dy(III)), in order to characterize the nature of chemical bonds with these metal ions and a polarizable, non-innocent, sulfur-donor ligand. The metal-sulfur bonds in these complexes trend shorter than measured for lanthanides with equivalent ionic radii. However, particularly large deviations are observed in the neptunium and plutonium complexes in both structure and bonding, resulting in a nonlinear bond length trendline for the actinide series. Density Functional Theory (DFT) calculations with Quantum Theory of Atoms in Molecules (QTAIM) and Natural Bond Order (NBO) analyses indicate that for the neptunium and plutonium complexes, the presence of increased 5f-orbital participation, energy degeneracy of the metal and ligand orbitals, and the structure packing result in shortened M–S bonds. The stabilization of the energy of the 5f-orbitals and the decrease in f-contribution to bonding orbitals in the later actinides results in structural properties more similar to the lanthanide complexes.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2021

The Future of Nuclear Energy: Electrochemical Reprocessing of Fuel Takes Center Stage

Nuclear power plants use energy-dense fuel and provide dependable baseload energy without generating greenhouse gas emissions. Despite these advantages, the long-term management of used nuclear fuel (UNF) remains a key challenge due to its lifetime (hundreds of thousands of years) and radiotoxicity. The components of UNF that contribute the most to this challenge are the actinide elements. A potential solution to this issue is to separate these radioisotopes from the bulk of the UNF and recycle them as fuel in advanced nuclear reactors. These separations can be achieved using electrochemical reprocessing, which employs electrochemical conversion and electrodeposition in a high-temperature molten salt electrolyte medium to separate the actinides from UNF. In this work, we review the current status, fundamental challenges, and future prospects of electrochemical reprocessing as they relate to UNF recycling.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2026

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↗
DOE OSTI2022

Plan for Developing TRISO Fuel Processing Technologies

This Plan demonstrates the availability of technologies for processing TRISO used nuclear fuel for waste management and actinide recovery purposes. These technologies are judged to be at a very low level of technology readiness and as such they constitute a fertile research area for the DOE-NE’s Office of Materials and Chemical Technologies. Strategies to mature the technologies to a point where they can reasonably be considered in engineering alternatives analyses typically involve laboratory-scale tests using fuel simulant to characterize process streams and demonstrate key engineering features. Several criteria are available to help selecting candidate technologies for further maturation

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2026

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↗
DOE OSTI2021

Gas-Phase Stability of Large Lanthanide:Ligand Clusters Evaluated Using Collision-Induced Dissociation

Introduction In the reprocessing of f-elements present in used nuclear fuels, a variety of diglycolamides (DGA’s) are used as extractants for actinide partitioning. In particular, the Actinide-Lanthanide Separation (ALSEP) process typically utilizes either the N,N,N’,N’-tetraoctyl diglycolamide (TODGA) or N,N,N',N'-tetra-2-ethylhexyl diglycolamide (T2EHDGA) extractant ligands following the partitioning of uranium and plutonium from used nuclear fuel. To better understand fundamental interactions in these processes, covalent bonding of several f-elements with diglycolamides, primarily TODGA, is investigated in the gas phase using nanospray ionization and a quadrupole time-of-flight mass spectrometer. Further, analysis of the identity and relative strength of the cluster is enabled by MS2 isolation and collision induced dissociation. Methods Metal ion cluster analysis was completed using a Bruker (Billerica, MA, USA) mircOTOF-Q II quadrupole time-of-flight mass spectrometer with a CaptiveSpray nanospray ion source. Detection was accomplished using positive ionization mode. Metal: ligand solutions were assembled as 30 µM europium nitrate, samarium nitrate, cerium nitrate, or holmium nitrate and 3 µM DGA in acetonitrile or a 50:50 mixture of acetonitrile: isopropanol. Preliminary data The samarium cluster experiments yielded clusters with a samarium:TODGA ratio of up to 1:7 able to be isolated and evidence of greater ratios present in the mass spectrum. This is surprising, as metal clusters are not expected to have a coordination space able to accommodate this many TODGA ligands, due to its size and tridenticity. Collisional activation of [Sm(TODGA)3]3+ suggested loss of a TODGA radical cation, in addition to ligand fragmentation. In contrast, activation of clusters with higher Sm:TODGA ratios resulted in loss of entire ligands, with no evidence of fragmentation. A lower collision energy was required to remove ligands as the number of bound TODGAs increased, suggesting that in larger clusters, ligands are more delicately complexed to the metal. In addition, several clusters were observed with the composition [Sm(NO3)x(TODGA)n x]+3 x. With a single nitrate ion, clusters with up to six TODGAs were able to be isolated. In a similar pattern to the samarium clusters containing only TODGA, less collision energy was required to eliminate one or more TODGAs with increasing size. Clusters with composition [Sm(NO3)(TODGA)n-1]2+ appeared in lower abundance and were more collisionally stable than [Sm(TODGA)n]3+ clusters. With two nitrate ions, only clusters with a single TODGA were able to be isolated. Analogous europium experiments resulted in similar clusters. Ratios of up to 1:7 Eu:TODGA and clusters with one nitrate and up to five TODGAs were isolated. In clusters with two nitrate ions, only one or two TODGAs were observed to be bound. Similar to samarium, MS2 experiments with the Eu clusters suggested that larger clusters required less collision energy to eliminate TODGA. Europium clusters with the composition [Eu(NO3)(TODGA)n-1]2+ were observed in greater abundance and with greater stability than the equivalent cluster with the composition [Eu(TODGA)n]3+. Novel Aspect These are the first reported Ln:TODGA clusters, allowing us to begin to investigate intrinsic complexation of lanthanides with process-relevant ligands.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2021

Investigating Covalent Bonding in f-elements using Gas-phase Ion Chemistry

Introduction In the reprocessing of f-elements present in used nuclear fuels, a variety of diglycolamides (DGA’s) are used as extractants for actinide partitioning. In particular, the Actinide-Lanthanide Separation (ALSEP) process typically utilizes either the N,N,N’,N’-tetraoctyl diglycolamide (TODGA) or N,N,N',N'-tetra-2-ethylhexyl diglycolamide (T2EHDGA) extractant ligands following the partitioning of uranium and plutonium from used nuclear fuel. To better understand fundamental interactions in these processes, covalent bonding of several f-elements with diglycolamides, primarily TODGA, is investigated in the gas phase using nanospray ionization and a quadrupole time-of-flight mass spectrometer. Further, analysis of the identity and relative strength of the cluster is enabled by MS2 isolation and collision induced dissociation. Methods Metal ion cluster analysis was completed using a Bruker mircOTOF-Q II quadrupole time-of-flight mass spectrometer equipped with a CaptiveSpray nanospray ion source. Metal:ligand solutions were prepared as 30 µM europium nitrate, samarium nitrate, cerium nitrate, or holmium nitrate and 3 µM DGA in acetonitrile or a 50:50 mixture of acetonitrile: isopropanol. Cluster mass spectra and collision-induced dissociation experiments were conducted in positive mode. Preliminary data To examine the patterns and relative strength of lanthanide: DGA interactions, MS2 experiments were completed with each lanthanide species listed above. Preliminary analyses of samarium and europium TODGA clusters suggest several combinations of TODGA and nitrate forming. The samarium cluster experiments yielded Sm(TODGA)x clusters with a samarium:TODGA ratio of up to 1:7 able to be isolated and evidence of greater ratios present in the mass spectrum. This is surprising, as metal clusters are not expected to have a coordination space able to accommodate this many ligands as large as TODGA. MS2 experiments show that, at higher ratios and with sufficient collision energy, entire TODGA ligands are removed instead of being fragmented. These experiments show that a lower collision energy is required to remove ligands as the number of bound TODGA’s increases, suggesting that in larger clusters, ligands are more delicately complexed to the metal. In addition to Sm(TODGA)x, several clusters were observed with nitrate ions bound to the metal in addition to TODGA. With a single nitrate ion, clusters with up to six TODGA’s were able to be isolated. In a similar pattern to the samarium clusters with only TODGA, less collision energy is required to eliminate one or more TODGA’s with increasing size. MS2 experiments suggest clusters with one nitrate appear to be of an equivalent or greater stability to clusters which replace the nitrate with a TODGA, as more collision energy is required to remove a TODGA ligand. These species with one nitrate are also in a higher abundance than the equivalent TODGA only cluster. With two nitrate ions, only clusters with a single TODGA were able to be isolated. Analogous europium experiments resulted in very similar clusters. Ratios of up to 1:7 Eu:TODGA were able to be isolated, and clusters with one nitrate and up to five TODGAs were isolated. In clusters with two nitrate ions, one or two TODGA’s could also be bound to the metal. MS2 experiments suggested, similarly to samarium, that larger clusters required less collision energy to eliminate TODGA. Europium clusters with one nitrate are in greater abundance and are stronger than the equivalent cluster which replaces the nitrate with TODGA. Similar analysis with cerium and holmium is ongoing, as well as analysis with other DGA ligands to compare relative strengths of the lanthanide metals with various extractant ligands.

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

Application of sensitivity analysis in DYMOND/Dakota to fuel cycle transition scenarios

The ability to perform sensitivity analysis has been enabled for the nuclear fuel cycle simulator DYMOND through its coupling with the design and analysis toolkit Dakota. To test and demonstrate these new capabilities, a transition scenario and multi-parameter study were devised. The transition scenario represents a partial transition from the US nuclear fleet to a closed fuel cycle with small modular LWRs and fast reactors fueled by reprocessed used nuclear fuel. Four uncertain parameters in this transition were studied – start date of reprocessing, total reprocessing capacity, the nuclear energy demand growth, and the rate at which the fast reactors are deployed – with respect to their impact on four response metrics. The responses – total natural uranium consumed, maximum annual enrichment capacity required, total disposed mass, and total cost of the nuclear fuel cycle – were chosen based on measures known to be of interest in transition scenarios and to be significantly impacted by the varying parameters. Furthermore, analysis of this study was performed both from the direct sampling and through surrogate models developed in Dakota to calculate the global sensitivity measures Sobol’ indices. This example application of this new capability showed that the most consequential parameter to most metrics was the share of new build capacity that is fast reactors. However, for the cost metric, the scaling factor of the energy demand growth was significant and had synergistic behavior with the fast reactor new build share.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2022

Impact of f-element complexation on the radiolytic robustness of separations ligands

Impact of f-element complexation on the radiolytic robustness of separations ligands Gregory P. Horne, Makayla R. Baxter, Corey D. Pilgrim, Travis S. Grimes, Center for Radiation Chemistry Research, Idaho National Laboratory, P.O. Box 1625, Idaho Falls, ID, 83415, USA Cristian Celis Barros, Department of Chemistry and Biochemistry, Florida State University, Tallahassee, FL 32306, USA. E-mail: ccelisbarros@fsu.edu Andrew R. Cook, Department of Chemistry, Brookhaven National Laboratory, Upton, New York, 11973, USA Stephen P. Mezyk, Department of Chemistry and Biochemistry, California State University Long Beach, 1250 Bellflower Boulevard, Long Beach, California, 90840-9507, USA The effects of ionizing radiation are ubiquitous throughout all aspects of a nuclear fuel cycle. However, the complexity and intensity of these effects are greatest during the management of used nuclear fuel, owing to the presence of a wide spectrum of radionuclides from neutron capture and fission processes. With regards to used nuclear fuel (UNF) reprocessing, radiation-induced processes typically promote the destruction of active compounds (e.g., complexants and additives) with the concomitant formation of potentially detrimental degradation products and corresponding changes in physical and chemical properties, which ultimately impact the effectiveness and longevity of a given reprocessing system. Concerning UNF complexants, radiation chemistry studies have historically focused on their radiation robustness in the absence of the metal ions they were designed to selectively complex. This knowledge gap is worrisome as previous studies on aqueous phase complexants have demonstrated significant changes in radiolytic behavior upon metal ion complexation.1-4 More recently, the rate of reaction of the n-dodecane radical cation—believed to be the major organic phase radiation-induced transient species responsible for complexant radiolysis in n-dodecane based solvent systems—with hexa-n-octylnitrilo-triacetamide (HONTA) was shown to increase by an order-of-magnitude upon complexation of europium or americium.5 These findings have significant implications on the projected longevity of complexants in UNF reprocessing solvent systems. Consequently, a thorough understanding of metal ion complexation effects on the radiolytic integrity of UNF complexants is essential to evaluate their potential for process application. Presented here are two recent studies from the Idaho National Laboratory Center for Radiation Chemistry Research group that demonstrate the various impacts of f-element complexation (uranium, americium, and lanthanides) on the radiolytic integrity (gamma and electron pulse) of tributyl phosphate (TBP), N,N-di-(2-ethylhexyl)butyramide (DEHBA), N,N-di-2-ethylhexylisobutryamide (DEHiBA), and 2-ethylhexylphosphonic acid mono-2-ethylhexyl ester (HEH[EHP]) under UNF reprocessing conditions. References 1) Bhattacharyya and Kundu, Int. J. Radiat. Phys. Chem., 1971, 3, 1. 2) Kundu and Matuura, Int. J. Radiat. Phys. Chem., 1975, 7, 565. 3) Ilan and Czapski, Biochimica et Biophysica Acta, 1977, 498, 386. 4) Buettner, Doherty, and Patterson, Fed. Euro. Biochem. Soc., 1983, 158 (1), 143. 5) Toigawa, Peterman, Meeker, Grimes, Zalupski, Mezyk, Cook, Yamashita, Kumagai, Matsumura, Horne, PCCP, 2021, 23, 1343.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2020

Process Model Development and Experimental Investigation for Spent Fuel Disposal in Crystalline Rocks: FY20 Report.

The U.S. Department of Energy Office of Spent Fuel Waste Disposition (SFWD) established in fiscal year 2010 (FY10) the Spent Fuel Waste Science & Technology (SFWST) Program (formerly the Used Fuel Disposition Campaign - UFDC) program to conduct the research and development (R&D) activities related to storage, transportation and disposal of used nuclear fuel and high level nuclear waste. The Mission of the SFWST is: To identify alternatives and conduct scientific research and technology development to enable storage, transportation and disposal of used nuclear fuel and wastes generated by existing and future nuclear fuel cycles. Significant progress has been made in FY20 in both experimental and modeling arenas in evaluation of used fuel disposal in crystalline rocks, especially in model demonstration using field data. The work covers a wide range of research topics identified in the R&D plan.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗