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At least 37 records · Page 2

Electrorefiner Speciation and Phase Model for Prediction of Operation Lifetime

The Mk IV electrorefiner (ER) at Idaho National Laboratory has recovered uranium metal from used nuclear fuels for 27 years. Thus, large quantities of fission product chlorides more electropositive than uranium have accumulated in the ER salt, increasing the complexity of phase equilibria and salt speciation. Importantly, the melt temperature of the salt increases with ER operation and will ultimately exceed design limits without intervention. Methods to remove fission products from molten chloride salt are known, but their implementation at scale is not yet demonstrated. In this work, historical ER composition and differential scanning calorimetry (DSC) are utilized to develop coupled speciation and chloride salt solution thermochemistry models, which enable accurate present-day analysis of ER salt as well as forecast its future disposition. The developed thermochemical models are applicable to chloride salts generally and have been made available in the Molten Salt Thermal Properties Database – Thermochemical.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

A new inventory tracking method for Mark-V electrorefiner

Here, we discuss the current practice of assessing the Mark-V electrorefiner inventory and a proposed new way of tracking this inventory. The presented approach only involves the total mass measurement of the transferred materials and the consideration of metallic uranium phase in the inventory while the current practice involves the estimation/calculation of the salt phase mass in the transferred material mass and the calculation of the holdup. Without estimating the involved salt inventory in the incoming and outgoing material streams, the proposed method yields the salt inventory agreeing with the current mass tracking practice. The estimated holdup in the current mass tracking practice is entirely explained with the introduced metallic uranium phase in the proposed model. The current practice of closing out the special nuclear material inventory is revisited with the insight gained from the proposed model. Suggestions are given to achieve the bounded uncertainty of the inventory estimates with the emerging in-situ measurement technique on the molten salt density.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Retrieving Historical Electrorefining Data

Pyrochemical Operations began at Los Alamos National Laboratory (LANL) during 1962 (1). Electrorefining (ER) has been implemented as a routine process since the 1980’s. The process data that went through the ER operation was recorded but had never been logged in an online database. Without a database new staff members are hindered in their work by the lack of information. To combat the issue a database in Access was created to collect the historical data. The years from 2000 onward were entered and queries were created to analyze trends. These trends will aid engineering and operations staff to reach optimal performance for the startup of the new lines.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Roadmap for disposal of Electrorefiner Salt as Transuranic Waste.

The experimental breeder reactor (EBR-II) used fuel with a layer of sodium surrounding the uranium-zirconium fuel to improve heat transfer. Disposing of EBR-II fuel in a geologic repository without treatment is not prudent because of the potentially energetic reaction of the sodium with water. In 2000, the US Department of Energy (DOE) decided to treat the sodium-bonded fuel with an electrorefiner (ER), which produces metallic uranium product, a metallic waste, mostly from the cladding, and the salt waste in the ER, which contains most of the actinides and fission products. Two waste forms were proposed for disposal in a mined repository; the metallic waste, which was to be cast into ingots, and the ER salt waste, which was to be further treated to produce a ceramic waste form. However, alternative disposal pathways for metallic and salt waste streams may reduce the complexity. For example, performance assessments show that geologic repositories can easily accommodate the ER salt waste without treating it to form a ceramic waste form. Because EBR-II was used for atomic energy defense activities, the treated waste likely meets the definition of transuranic waste. Hence, disposal at the Waste Isolation Pilot Plant (WIPP) in southern New Mexico, may be feasible. This report reviews the direct disposal pathway for ER salt waste and describes eleven tasks necessary for implementing disposal at WIPP, provided space is available, DOE decides to use this alternative disposal pathway in an updated environmental impact statement, and the State of New Mexico grants permission.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Technical Feasibility of Direct Disposal of Electrorefiner Salt Waste

The experimental breeder reactor (EBR-II) used fuel with a layer of sodium surrounding the uranium-zirconium fuel to improve heat transfer. Disposing of this EBR-II used fuel in a geologic repository without treatment is not prudent because of the potentially energetic reaction of the sodium with water. In 2000, the US Department of Energy decided to treat the EBR-II sodium-bonded used fuel in an electrorefiner (ER), which produces a metallic waste, mostly from the cladding. The salt remaining in the ER contains most of the actinides and fission products. Two baseline waste forms were proposed for disposal in a mined repository; the metallic waste, which was to be cast into ingots, and the ER salt waste, which was to be further treated to produce a ceramic waste form. However, alternative disposal pathways for metallic and salt waste streams are being investigated that may reduce the complexity. For example, performance assessments show that both mined repositories in salt and deep boreholes in basement crystalline rock can easily accommodate the ER salt waste without treating it to form a ceramic waste form. Hence the focus of a direct disposal option, as described herein, is now on the feasibility of packaging the ER salt waste in the near term such that it can be transported to a repository in the future without repackaging. A vessel for direct disposal of ER salt waste has been previously proposed, designed, and a prototype manufactured based on desirable features for use in the hot cell. The reported analysis focused on the feasibility of transporting this proposed vessel and whether any issues would suggest that a smaller or larger size is more appropriate. Specifically, three issues are addressed (1) shielding necessary to reduce doses to acceptable levels; (2) the criticality potential and the ease which it can be shown to be inconsequential, and (3) temperatures of the containers in relation to acceptable cask limits. The generally positive results demonstrate that direct disposal of ER in the proposed packaging is feasible without the need to secure funding to modify the facility.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Final Design for Thermal/Epithermal eXperiments (TEX) with Chloride Absorbers to Provide Validation Benchmarks for Y-12 Electrorefining Facility

Uranium electrorefining operations at Y-12 require validation for chlorine absorption and reflection. Plutonium chloride solution operations at Los Alamos National Laboratory require chlorine absorption validation. The growing need for chlorine validation is evident to the wider criticality safety community, with multiple attendees at the recent TEX 2.0 meeting at Lawrence Livermore National Laboratory (May 2023) requesting validation for chlorine (Idaho National Laboratory (INL), Institute de radioprotection et de surete nucleaire (IRSN), Savannah River Nuclear Site (SRNS), LANL, and Y-12). Los Alamos National Laboratory has recently performed, and benchmarked, an experiment titled Chlorine Worth Study (CWS) for the internal operations at the lab, but due to the difficulties in precisely characterizing the material compositions of the chlorine absorbers it is advantageous to perform a complimentary study with a different chlorine-based absorber material. Furthermore, having a uranium-based vs plutonium-based experiment provides a separate and important validation basis for criticality safety and nuclear data evaluation. The original final design report for the study of chlorine absorption using the TEX-HEU experimental base was presented in 2022, but used the same chlorine-bearing materials that were found to be difficult to characterize in the LANL benchmark. A complete redesign of the experiment has been performed looking at alternative absorber materials in various forms to produce an experiment that is fully characterizable. This report presents five novel chlorine experiments using the TEX-HEU test bed which provides direct comparison to the Y-12 and INL/Terrapower application needs, utilizing sodium chloride (NaCl) absorber plates. The absorber plates will consist of granulated NaCl (≥99.5% pure), which will be fully encapsulated in aluminum tins, providing a simple but effective chlorine-based absorber material that can be completely characterized. Of the five configurations presented in this report, it is expected that two or three configurations will be down selected for the actual experiment, with the other configurations being alternates. Three of the configurations are in the standard configuration, where the absorber is placed directly on the HEU fuel plates, and two in the sandwich configuration, where the absorber is surrounded by polyethylene moderators to force additional neutron thermalization prior to reaching the absorber. There are two thicknesses of NaCl absorber plates: 3/16” and 1/4” active thicknesses (i.e. not including the encapsulation). Both variations of the absorbers have an active absorber radius of 6” and a total radius of 7.5” to match the diameter of the HEU plates, with the outer 1.5” being aluminum encapsulation. The high-density polyethylene (HDPE) moderators are of the thicknesses: 27/16”, 7/4”, 1/8”, 11/16”, and 3/4”. The final configurations have six (one sandwich and one standard configuration), eight (one sandwich and one standard configuration), and 18 total fuel layers (standard configuration). The standard and sandwich configurations were designed such that the differences in moderator thicknesses are 1” HDPE, which were already procured for the original CED-2. The proposed configurations were precisely tuned to closely match the sensitivity profiles and neutron spectra of the Y-12 upset cases and were also compared to the INL/Terrapower upset cases. The assessment of experimental uncertainties of the non-absorber components was predicted to be 0.00114 Δk eff . The assessment of uncertainties resulting from the absorbers was predicted to be 0.00029 Δk eff . This results in a total uncertainty of 0.00118 Δk eff . Many of the largest uncertainties, namely the moderator densities, may be reduced with precision dimensional inspection of the components. The 1” HDPE moderators as well as the HDPE reflectors from the original CED-2 were incorporated in the final designs presented here. Additional HDPE moderator plates must be fabricated to complete the configurations. NaCl absorber plates will by fabricated at LLNL. The total additional cost is expected to be $\$$54,250 for the remaining components. Precise inspection, including dimensional, mass, density, and impurity, is recommended for all components. LLNL estimates that these costs are around $\$$12,000. It is expected, based on previous TEX-HEU experiments, that three weeks of experimental facility time is needed to complete the experiments.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

System and method for electrorefining of silicon

The present disclosure provides methods and systems for electrorefining high-purity materials, for example, silicon. An exemplary system includes at least one cathode, an anode, and a reference electrode. At least one controller, for example a potentiostat, is used to control the potential difference between a reference electrode and a cathode or anode. The system can be operated in a single phase or multiple phase operation to produce high-purity materials, such as solar-grade silicon.

Tao, Meng↗

A Triple Bubbler System to Measure Density, Surface Tension, and Depth of Electrorefiner Molten Salt

In pyroprocessing of used nuclear fuel (UNF), uranium from the fuel is electrochemically dissolved at the anode and transported through a molten salt electrolyte to the cathode—where it is later recovered for reuse. As part of this process, special nuclear materials (SNM) dissolve into the molten salt electrolyte. Monitoring the mass of these materials, particularly plutonium, is important for material accountability and safeguards of the electrorefiner (ER) used in pyroprocessing. The mass of plutonium in the ER vessel is a function of the volume and density of the salt as well as the plutonium concentration. Measuring these parameters presents challenges due to the high temperature, radiation, and accessibility of the ER within a hotcell. Here, the main motivation for this work was to develop a method capable of measuring the density and depth (volume) of salt under the extreme operating conditions within the ER to enhance the SNM accountability and safeguards of pyroprocessing. In addition, these online measurements would be useful for monitoring level changes associated with removal of electrolyte from the ER and different unit operations associated with electrochemical reprocessing of used nuclear fuel.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Dechlorination of molten chloride waste salt from electrorefining via ion-exchange using pelletized ultra-stable H-Y zeolite in a fluidized particle reactor

Dechlorination of eutectic LiCl–KCl based electrorefner (ER) salt is reported via ion-exchange reaction with protonated ultrastable Y-type (USHY) zeolite bound into mechanically fuidized 45–250 μm diameter particles. Evidence of exchange of cations from the salt (Li + , K + , and fission product cations) into the zeolite lattice replacing H + ions was found based on a change in unit cell size, ICP-MS, XRD and TEM–EDS in addition to detection of HCl of gas. Ion exchange reaction was carried out at 625 and 650 °C, temperatures above the melting point of eutectic LiCl–KCl. Experiments were carried out to optimize zeolite drying temperature, estimate maximum ion-exchange capacity, and determine the thermal stability of USHY zeolite. The results indicate over 90% dechlorination can be achieved without zeolite structure collapse at 625 °C. Finally, this provides a promising route to stabilizing waste from radioactive chloride salts into dechlorinated waste forms for permanent geologic disposal.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Room Temperature Electrorefining of Rare Earth Metals from End-of-use Nd-Fe-B Magnets

Recovering rare earth elements (REE) from used permanent magnets, which contains about 30 wt.% of rare earth elements, has been persistent technological challenge. Current recycling methods relies on pyrometallurgical or hydrometallurgical processes which are energy- and chemical- intensive and not economically and environmentally viable for rare earth containing magnets. Enabling efficient and simplistic recovery and refining of REEs contained in End-of-Use (EoU) products, such as Neodymium-Iron-Boron (Nd-Fe-B) based magnets will play an important and complementary role in the total supply of REEs in the future. We designed a new electrochemical method and demonstrated a room temperature one-pot process that concurrently separates and electroplates REE from commercial Nd-Fe-B magnets. By establishing selective oxidation and reductive potential as electrochemical control parameter along with electrochemically compatible non-aqueous electrolyte system, we demonstrated selective electroleaching of lanthanides (Nd and Preseodymium (Pr)) from anode and concurrent plating as alloy at Pt cathode. The morphological and chemical evolution of the Nd-Fe-B magnets during electroleaching reveals the electrochemical stimuli and rate of dissolution depends on microstructural complexities of the Nd-Fe-B magnet. The concomitant electroplating process leads to Nd-Pr based alloy which can be used as raw metallic alloy for manufacturing new permanent magnet and other devices. Our study demonstrates a scalable separation and refining methodology, based on widely available organic electrolyte system and without any consumptive chemical use, for selective lanthanide recovery from waste magnets.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Evaluation of Iron‐Phosphate Glass–Ceramic Waste Form for Electrorefiner Salt Waste Simulant Dechlorinated With Phosphoric Acid

The importance of glass and glass–ceramic nuclear waste forms has been reaffirmed in recent years by the growing interest in nuclear power as a reliable energy source. Determination of processing methods for the disposal of halide-containing wastes will be essential for the advancement of nuclear technologies such as non-aqueous fuel reprocessing. Phosphate-based dechlorination and subsequent vitrification of radioactive salt waste into an iron-phosphate waste form have been identified as a potential processing scheme for electrochemical processing waste. The impact of H 3 PO 4 -based dechlorination of complex salt mixtures on the vitrification process and structure of the final iron-phosphate waste form has not yet been investigated. In this work, iron-phosphate glass–ceramics were made from simulant salt waste (48LiCl–33KCl–19NaCl mol%) dechlorinated with the H3PO4-based method. The glass-forming region was compared to that of traditionally prepared Na 2 O–Fe 2 O 3 –P 2 O 5 systems. For a candidate glass-forming composition, the processing scheme presented here was determined to favor Fe 3+ species. The O/P molar ratio was consistent for the candidate composition when dechlorinated at 400°C and 600°C in air and argon environments, indicating glass network connectivity was maintained despite variations in processing parameters. The results presented here validate processing schemes requiring iron-phosphate waste form synthesis following H 3 PO 4 -based dechlorination.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Final Design for Thermal/Epithermal eXperiments (TEX) with Absorbers to Provide Validation Benchmarks for Y-12 Electrorefining Facility

One of the main goals of the Thermal/Epithermal eXperiments (TEX) project is to use existing Nuclear Criticality Safety Program (NCSP) assets to create critical experiment plutonium and uranium test beds for materials important to criticality safety that have insufficient benchmark evaluations. The plutonium test bed experiments were completed in 2018 and are published in the 2020 edition of the International Criticality Safety Benchmark Evaluation Project (ICSBEP) Handbook. The uranium test bed assemblies were measured in 2020, with benchmark preparation underway.

42 ENGINEERING↗

Developments in Processing Criteria for Iron Phosphate Waste Form Design for Treating Electrorefiner Salt Wastes

This report describes work done under a Nuclear Energy University Partnership (NEUP) project that included a collaborative effort between Pacific Northwest National laboratory, University of Nevada Reno, University to Utah, and Missouri University of Science and Technology. In this project, the main goals were the following: (1) to assess H3PO4 dechlorination parameters for halide removal from salt simulants, (2) to evaluate crucible compatibility with iron phosphate glass melts, and (3) to evaluate waste form properties within a ternary system of P2O5 (added as H3PO4), Fe2O3 and fission product simulants.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

TEX-Chlorine: Highly Enriched Uranium with Chloride Absorbers to Provide Validation Benchmarks for Y-12 Electrorefining Facility

This report documents the final benchmark of the TEX-Chlorine (IER-499) Thermal Epithermal eXperiments (TEX) with highly enriched uranium with chlorine absorbers and high-density polyethylene reflectors and moderators. TEX-Chlorine is a variation of the TEX-HEU baseline assembly with the addition of sodium chloride absorber plates. This evaluation contains three experimental configurations that were performed on Comet at NCERC between July and August 2024. The three configurations, which were acceptable as benchmark cases, spanned from thermal (first two configurations) to fast (third configuration). All three cases were reviewed and accepted by the ICSBEP TRG in April 2025 and was submitted to the ICSBEP in August 2025 after receiving subgroup approval.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗