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At least 163 records · Page 9

Systems Engineering Approach for Design and Implementation of a Gas Breech for Actinide Experiments at the JASPER Facility

The Joint Actinide Shock Physics Experimental Research (JASPER) Facility is located approximately 65 miles north of Las Vegas, Nevada at the Nevada National Security Site (NNSS). The primary mission is to conduct shock physics research on actinide materials in support of NNSA’s Stockpile Stewardship Program. JASPER experiment uses a two-stage light gas gun to accelerate projectiles into targets at velocities up to 8 km/s (17,000 mph). The first stage uses an ignited propellent to drive a piston to compress gas in the pump tube. At the second stage, the gas compression exceeds a specified pressure and a rupture valve at the end of the pump tube opens. This launches a projectile to impact the target. The target is housed inside the target assembly and the debris field is contained inside the primary target chamber (PTC). The PTC is placed inside the secondary confinement chamber (SCC) as an added protection against possible contamination. These major components are illustrated in Figure 1.JASPER is capable of generating and measuring data on the properties of radioactive chemical elements at high shock pressures, temperatures, and strain rates approximating the conditions in nuclear weapons by using a two-stage gas gun. The data is used to determine material equations-of-state and validate computer models of material response. The work advances predictive capability, thus ensuring confidence in the nuclear stockpile.

42 ENGINEERING↗

Characterization of actinide abundances and isotopic compositions by HR-ICP-MS

In this report, we present actinide isotopic and elemental data from fallout melt glass using high resolution inductively coupled plasma mass spectrometry (HR-ICP-MS). This is an analytical technique that requires minimal sample preparation. These data are directly compared to the results of high precision isotopic analyses and elemental assay by multi-collector (MC-) ICP-MS, which requires lengthy sample processing involving spiking and purifying aliquots of individual elements. The comparison shows broad overlap between the results of the two techniques. Thus, although the data obtained by HR-ICP-MS is of significantly lower precision, it is a viable method to obtain actinide elemental and isotopic data on a more rapid timeframe than traditional high-precision techniques.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Applications of Alternate Actinide Calibration on Inductively Coupled Plasma Mass Spectrometry (ICPMS) Analysis of H-Canyon Highly Enriched Uranium Legacy Material at the Savannah River Site (SRS)

The Savannah River National Laboratory (SRNL) uses Inductively Coupled Plasma Mass Spectrometry (ICPMS) to support numerous programs at the Savannah River Site (SRS). As part of an objective to prepare high assay low enriched uranium (HALEU), the SRS H-Canyon needed analysis of legacy uranyl nitrate that is stored at its Outside Facilities (HOF). With the application of a standard practice for alternate actinide calibration on ICP-MS, SRNL has successfully demonstrated its capability to characterize the uranium/actinide composition of the HOF tanks that are intended for consolidation prior to preparation of the HALEU. A comparison of the uranium analytical results between recently upgraded SRNL ICP-MS and Inductively Coupled Plasma Optical Emission Spectrometry (ICP-OES) instrumentation shows the alternate actinide calibration is a valid complementary method when used in conjunction with other analytical techniques (Davies-Gray Potentiometric Titration). The methods, instrumentation, and ongoing developments on ICP-MS at SRNL will be discussed.

Jones, Mark A.↗

Concepts for Actinide Recovery from TRISO Used Nuclear Fuel

The work described in this report has developed a preliminary conceptual flowsheet based on limited published literature for the head-end of a TRISO oxycarbide UNF reprocessing plant. The essential function of the head-end is to prepare the UNF for subsequent separation of actinides. The main steps of the conceptual TRISO UNF head-end reprocessing flowsheet are: 1. Fragmentation of the graphite moderator to expose the fuel particles. 2. Separation of fuel particles from fragmented graphite moderator by sieving and fluidization. 3. Fragmentation of the fuel particles to expose the fuel kernel. 4. Dissolution of the fuel kernel in nitric acid. Noteworthy at this step is the formation of organic acids (mainly oxalic and mellitic acids) from the carbon associated with the fuel and TRISO coatings. These acids can interfere with actinide separations and solvent extraction hydraulic performance and carbon dioxide gas generation. 5. Clarification of the dissolved fuel solution to separate the coating fragments. 6. Dissolver off-gas treatment with specific emphasis on managing generation of carbon dioxide gas containing carbon-14. The quantity of carbon dioxide is projected to be 100 to 1000 times greater than that arising from dissolving LWR UNF. Pre or post treatment of the exposed fuel kernels could be undertaken to mitigate the formation of organic acids but there still exists a significant off-gas treatment challenge. The literature on reprocessing uranium nitride UNF was reviewed but a flowsheet was not specifically developed since its scope and uncertainties are expected to be encompassed by the oxycarbide flowsheet. Overall, the predominant feature of processing TRISO UNF is carbon management to reduce waste volume and mitigate the formation of carbon dioxide and organic acids. This report recommends broad areas of research that will help to further define the head-end flowsheet.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Design, Construction, and Installation of In-Glovebox Pumped Actinide Molten Salt Loops

This report summarizes the work conducted in FY25 to construct and install pumped actinide-bearing molten salt loopsin a radiological glovebox. The establishment of such a capability will provide a platform in which technologies developed for Gen. IV molten salt reactors may be tested under relevant operating conditions. A review of convective molten salt systems is provided to frame Argonne’s pumped actinide loop relative to contemporary and historical systems. Moreover, the infrastructure needed to operate the system is detailed to provide additional context as to design metrics of the loops and supporting equipment. The pumps’ performance in water testing is outlined and used to inform operational activities planned in FY26. Finally, electrochemical experiments investigating fundamental reaction mechanisms governing reactive oxygen species that promote corrosion of molten salt media is also reported. In total, these combined loop installation and sensor development tasks will serve to aid in the future commercial deployment of molten salt reactors in the U.S.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Biologically Influenced Transport of the +3 Actinide Oxidation State from the WIPP Environment, Using Neodymium as an Analog

This report provides an update to a previously issued report on the bioassociation of the +3 actinide analog, neodymium, with Waste Isolation Pilot Plant (WIPP) microbial isolates (LCO ACP-32, Biologically Influenced Transport of the +3 Actinide Oxidation State from the WIPP Environment, Using Neodymium as an Analog ). Results contribute to updates for the biocolloid parameters for the 2026 Compliance Recertification Application (CRA-2026).

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Synthesis Roadmap for Actinide Chloride Salts

Molten salt reactors (MSRs) are among the main advanced nuclear reactor types at the forefront of development by industry, with the support of the US government, for the next fleet of nuclear reactors to support the demand for energy in the coming decades. MSRs are highly unique because they are cooled and typically also fueled by molten salt. This quality brings about safety benefits such as low-pressure operation and self-stabilization of the neutron flux, operational benefits such as high-temperature operation and the ability for online refueling, and fuel and waste management benefits thanks to the flexibility of post-processing of molten salts and reprocessing options that involve removal of fission products and actinide separation. In fact, domestic deployment of molten salt (or molten salt–cooled) reactors is an approaching reality: a handful of molten salt reactor developers are planning to operate demonstration-scale reactors, as a step toward commercial-scale power reactors, within the decade. For example, Natura Resources received a construction permit in September 2024 for the deployment of MSR-1, which is a graphite-moderated thermal spectrum reactor, at Abilene Christian University. Also, TerraPower, in a collaborative effort with Southern Company and Idaho National Laboratory (INL), received approval from DOE in 2023 to proceed with the construction of the Molten Chloride Reactor Experiment (MCRE), a homogeneous chloride fast reactor at INL, and has begun assembly of system components. There are several other examples of developers at different stages of development of their own unique MSR designs (Jenet et al., 2025). As developers are in the process of obtaining approvals for their designs, deploying demonstration-scale reactors, and planning for their commercial-scale power reactors, there is a critical supply chain need for the synthesis of fuel for these reactors that must be addressed. The challenge generally is three-fold: (1) the quantity of fueled salt needed for these reactors is extraordinarily high (>100s of kilograms), but demonstrations of scaled-up techniques for fueled salt synthesis are significantly more limited than demonstrations of lab-scale syntheses; (2) each developer has a unique reactor design, which means different actinide halide elements in different carrier salts must be synthesized; and (3) there is a need for particularly high-purity salt so as to ensure the long-term operability of these reactors with minimal degradation to salt-wetted components, which necessitates synthesis techniques with high levels of quality control, repeatability, and well-characterized precursor and reactant materials. It is crucial that this supply chain challenge be addressed by demonstrating synthesis techniques that are scalable, de-risked, and well-documented so that these technologies may be adopted and utilized by industry to support the fueling needs of MSRs that are to come online within the next 10 years. With this supply chain challenge clearly defined for the developing MSR industry, it is important to consider that addressing such a challenge is oftentimes complex and context-dependent. There is not necessarily a single synthesis technique that can be scaled up and adopted to address the needs of all MSR developers; the synthesis approach that may be viable for producing a desired fuel salt will be entirely dependent on the exact salt composition needed, the quantity needed, purity needed, the refueling and waste plans, and the availability of a carrier salt for the fuel. Therefore, it is important to consider more broadly what synthesis techniques are available and have been demonstrated to understand the benefits, challenges, and general nuances that should be considered when evaluating a particular route for efficient production of high-purity fuel salts at scale.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Low-Energy Electron Elastic Collisions with Actinide Atoms Am, Cm, Bk, Es, No and Lr: Negative-Ion Formation

The rigorous Regge-pole method is used to investigate negative-ion formation in actinide atoms through electron elastic total cross sections (TCSs) calculation. The TCSs are found to be characterized generally by negative-ion formations, shape resonances and Ramsauer-Townsend(R-T) minima, and they exhibit both atomic and fullerene molecular behavior near the threshold. Additionally, a polarization-induced metastable cross section with a deep R-T minimum is identified near the threshold in the Am, Cm and Bk TCSs, which flips over to a shape resonance appearing very close to the threshold in the TCSs for Es, No and Lr. We attribute these new manifestations to size effects and orbital collapse significantly impacting the polarization interaction. From the TCSs unambiguous and reliable ground, metastable and excited states negative-ion binding energies (BEs) for Am−, Cm−, Bk−, Es−, No− and Lr− anions formed during the collisions are extracted and compared with existing electron affinities (EAs) of the atoms. The novelty of the Regge-pole approach is in the extraction of the negative-ion BEs from the TCSs. We conclude that the existing theoretical EAs of the actinide atoms and the recently measured EA of Th correspond to excited anionic BEs.

Msezane, Alfred Z. (ORCID:0000000212485661)↗

Microbial Influence on the Mobility of +3 Actinides from a Salt-Based Nuclear Waste Repository

Biologically enhanced transport of radionuclides is one of several processes that can affect the performance of a nuclear waste repository. In this work, several microbial isolates from the Waste Isolation Pilot Plant (WIPP) were tested for their influence on the concentration of neodymium, as an analog for +3 actinides, in simple sodium chloride solutions and in anoxic WIPP brines. Batch sorption experiments were carried out over a period of 4–5 weeks. In many cases, the effect on neodymium in solution was immediate and extensive and assumed to be due to surface complexation. However, over time, the continued loss of Nd from the solution was more likely due to biologically induced precipitation and/or mineralization and possible entrapment in extracellular polymeric substances. The results showed no correlation between organism type and the extent of its influence on neodymium in solution. However, a correlation was observed between different test matrices (simple NaCl versus high-magnesium brine versus high-NaCl brine). Further experiments were conducted to test these matrix effects, and the results showed a significant effect of magnesium concentration on the ability of microorganisms to remove Nd from solution. Possible mechanisms include cation competition and the alteration of cell surface structures. This suggests that the aqueous chemistry of the WIPP environs could play a larger role in the final disposition of +3 actinides than the microbiology.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Study of actinide chemistry in saturated potassium fluoride solution

Study concerning the chemistry of actinides in saturated KF solution included work with neptunium, uranium, and americium. Solubilities, absorption spectra, oxidation-reduction reactions, and solid compounds which can be produced in KF solution were examined. The information is used for preparation of various materials from salts of the actinides.

Cohen, D.↗

Actinide crystal-liquid partitioning for clinopyroxene and Ca3/PO4/2

Coefficients for the partitioning of the actinide elements Th, U and Pu, which are used as indicators of r-process nucleosynthesis and the ages of meteorite and lunar samples, between diopsidic clinopyroxene, whitlockite and silicate liquid at 20 kbar are measured. Fission and alpha track radiography techniques are employed to detect element concentrations in synthetic crystals made using spiked starting materials, under the assumptions of equilibrium partitioning at the crystal-liquid interface and actinide zoning. Analysis of the data indicates results to be consistent with interface equilibrium except at high cooling rates. Th/U/Pu partition coefficients of about 0.002/0.002/O.06 are measured for clinopyroxene and 1.2/0.5/3.4 for whitlockite. The greater incorporation of Pu into the crystalline phases is attributed to the importance of trivalent Pu, and the similarity of its partition coefficient into clinopyroxene to that of the light rare earths supports the concept of Pu/rare earth dating.

Benjamin, T.↗

The abundance of the actinides in the cosmic radiation as measured on HEAO 3

The HEAO 3 detector of heavy cosmic-ray nuclei has observed one possible actinide nucleus and some 100 nuclei of the platinum-lead group of elements. The resulting upper limit of 3% for the abundance ratio of actinides to platinum-lead nuclides is significantly lower than previous results from other observations. This new limit is inconsistent with freshly synthesized, pure r-process sources for cosmic-ray nuclei in this charge interval but is consistent with a source having a composition similar to the solar system, or to aged r-process material. We observe no events with a charge greater than 96.

Binns, W. R.↗

Actinide abundances in ordinary chondrites

Measurements of actinide and light REE (LREE) abundances and of phosphate abundances in equilibrated ordinary chondrites were obtained and were used to define the Pu abundance in the solar system and to determine the degree of variation of actinide and LREE abundances. The results were also used to compare directly the Pu/U ratio with the earlier obtained ratio determined indirectly, as (Pu/Nd)x(Nd/U), assuming that Pu behaves chemically as a LREE. The data, combined with high-accuracy isotope-dilution data from the literature, show that the degree of gram-scale variability of the Th, U, and LREE abundances for equilibrated ordinary chondrites is a factor of 2-3 for absolute abundances and up to 50 percent for relative abundances. The observed variations are interpreted as reflecting the differences in the compositions and/or proportions of solar nebula components accreted to ordinary chondrite parent bodies.

Hagee, B.↗

Advances in Structure Prediction of Lanthanides and Actinides with Genetic Algorithms

Computationally guided materials discovery has advanced significantly in the past two decades. Recent developments of widely available genetic algorithm-based structure prediction software in the past 10+ years has led to increased use of this methodology in the discovery and design of new materials. Owing to the computational challenges of treating f-block elements and computationally expensive methods for structure prediction, the discovery of new phases of lanthanide and actinide materials has been particularly challenging. With advancements in the development of genetic algorithms for structure prediction and the continuing improvement of high-performance computing resources, genetic algorithms provide a tractable method to find new stable phases of materials at high pressure or to search a large phase space for unknown compounds. Genetic algorithms have already been applied to the successful identification of novel lanthanide and actinide materials, as well as the prediction of unusual material properties in new phases that make promising synthetic targets.

Shields, Ashley↗

Actinide Science for Post Detonation Nuclear Forensic Analyses

Actinide and fission product separations, analyses, and solid material syntheses are key to supporting the development and testing of new nuclear forensic science technologies and for training nuclear emergency responders to effectively respond to nuclear emergency events. In this presentation, nuclear forensic scientist Dr. Mathew Snow will discuss a variety of technologies developed at Idaho National Laboratory (INL) and around the world for these applications. The presentation will include discussions of new approaches to rapid, high-efficiency chemical separations, sample preparation and analysis techniques for field-deployable actinide analyses, and techniques recently developed at INL for producing solid nuclear fallout simulant materials. An overview of the challenges confronting researchers in these area, along with possible opportunities, will also be provided.

Nuclear Forensics↗

Exploring the speciation of actinide salts in the presence of contaminants related to molten salt reactors

Molten salt reactors (MSR) are up-and-coming Generation IV nuclear reactors with either coolant and/or radioactive fuel in molten salt form. Due to their improved safety, efficiency, affordability and convenient waste processing system, these reactors are considered a superior alternative to conventional ones. However, prior to commercial implementation, it is necessary to have an extensive understanding of the reactions occurring in the MSR. The safety parameters of the MSR are determined by the rheological properties such as density and viscosity of the molten salt and these properties are governed by the local structure of the molten salts. Due to the high operational temperatures of MSR's, corrosion plays an important role. Because of their influence, the container corrosion products become part of the fuel salt matrix. In this work, we are investigating how these corrosion products, e.g., Mo, Ni, Cr, would impact the speciation of the actinide metal centers. For the initial studies, lanthanides are used as a surrogate for actinides. Lanthanide chloride salts (LnCl3) are mixed with transition metals and excess of alkali or alkali earth metal salts or salt mixtures (LiCl, NaCl, KCl). These are added to an alumina crucible, placed in a quartz tube, and sealed under a vacuum. This is heated up to around 1000 °C and slowly cooled to a temperature above the melting point of the salt and at that temperature, the reaction is taken out of the furnace. The excess salt is removed, and the resulting product is analyzed using X-ray diffraction techniques, scanning electron microscopy, and spectroscopic methods such as Raman, UV-Visible, and FTIR spectroscopy.

37 - INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL C↗

ThH 5 : An Actinide–Containing Superhalogen Molecule

Thorium and its compounds have been widely investigated as important nuclear materials. Previous research focused on the potential use of thorium hydrides, such as ThH 2 , ThH 4 , and Th 4 H 15 , as nuclear fuels. Here, we report studies of the anion, ThH 5 , by anion photoelectron spectroscopy and computations. The resulting experimental and theoretical vertical detachment energies (VDE) for ThH 5 are 4.09 eV and 4.11 eV, respectively. These values and the agreement between theory and experiment facilitated the characterization of the structure of the ThH 5 anion and showed its neutral counterpart, ThH 5 to be a superhalogen. ThH 5 , which exhibits a C 4v structure with five Th–H single bonds, possesses the largest known H/M ratio among the actinide elements, M. Here, the adaptive natural density partitioning (AdNDP) method was used to further analyze the chemical bonding of ThH 5 – and to confirm the existence of five Th–H single bonds in the ThH 5 – molecular anion.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Measurements of effective actinides neutron capture cross sections in a cadmium-filtered epithermal neutron spectrum

In this work, a total of 20 actinide samples were irradiated in the Advanced Test Reactor (ATR) at Idaho National Laboratory (INL): 233 U (1), 235 U (1), 236 U (1), 238 U (1), 237 Np (2), 239 Pu (1), 240 Pu (1), 242 Pu (2), 244 Pu (2), 241 Am (2), 243 Am (2), 244 Cm (2), and 248 Cm (2). The samples were loaded in a basket containing a 1.1-mm thick cadmium filter. The presence of the filter drastically changes the neutron spectrum in the samples and accentuates the reaction rates in the resonance region. Isotopic ratios were determined using Multi-Collector Inductively Coupled Plasma Mass Spectrometry (MC-ICP-MS) that allowed inferring effective capture cross sections. Detailed best-estimate MCNP models of the experiment using ENDF/B-VII.0 nuclear data were developed to calculate the effective neutron cross sections and, subsequently, compare them with the cross sections inferred from experimental results.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗