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All sourcesNASA NTRSDOE OSTI
DOE OSTI2018

AGR-3/4 Experiment Preliminary Mass Balance

AGR-3/4 was an experiment primarily aimed at studying fission product transport in graphite and graphitic materials. To accomplish this, 80 designed-to-fail (DTF) particles coated only with a thin pyrocarbon layer were incorporated among the roughly 7500 tristructural isotropic-coated driver fuel particles in each capsule. It was anticipated that intact DTF particles would behave like TRISO particles with SiC layer failures (releasing cesium and other metallic fission products to some extent, but retaining fission gases), and failed DTF particles would behave like TRISO particles with failed TRISO coatings (releasing both cesium and other metallic fission products and fission gases). The DTF particles provided a known source of fission products to migrate out into the fuel compact matrix and out into the surrounding concentric rings of graphite and graphitic matrix material for study. Post-irradiation examinations have focused on measuring the total releases of fission products from the fuel compacts (mass balance) and the spatial distribution of fission products in the rings. The total mass balance is an important parameter for comparison to fission product transport simulations of the AGR-3/4 experiment, and the spatial distribution within carbon rings is being used to derive fission product diffusion coefficients. To determine the fission product mass balance, each of the 12 irradiation capsules was disassembled, and their component parts analyzed via gamma counting and destructive leach or burn-leach methods. In “standard” capsules (Capsules 1, 3-5, 7-8, 10, and 12), inner rings, outer rings, sink rings, spacers, foils, felts, and through tubes were all analyzed for gamma-emitting fission products. Beta-emitting Sr-90 was measured as well, but because of the analysis program on the inner and outer rings, the Sr-90 inventory of the inner and outer rings is not yet available. “Fuel body” Capsules 2, 6, 9, and 11 were retained intact for future heating tests; thus, the inner and outer rings from these capsules were not measured. The most commonly detected radionuclide fission products were Ag-110m, Cs-134, Cs-137, Eu-154, Eu-155, and Sr-90. Sb-125 was also frequently detected in the sink rings and spacers; however, the zircaloy spacers used in Capsules 1 through 6 contained natural antimony that transmuted to Sb-125 and made it impossible to separate Sb-125 released from the fuel from that generated in the spacers. Summing the fission product inventory measured on each capsule component made it clear that the presence of 80 DTF particles in each capsule resulted in noticeably higher releases of cesium, europium, and strontium from AGR-3/4 fuel when compared to AGR-1 fuel which did not have DTF particles. Greater than 30 particles worth of Cs-134 was measured outside of the fuel compacts in Capsules 3-5, 7, 8, and 10. In Capsule 11 (an intact fuel body for which the inner and outer rings were not measured), 26 particle equivalents of Cs-134 was measured outside of the outer ring. Based on experience from AGR 1, it is very unlikely that any driver particles failed during the irradiation; therefore, this cesium is assumed to be overwhelmingly dominated by release from DTF particles.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2019

Fabrication and Irradiation Test Plan for Fully Ceramic Microencapsulated Fuels

The objective of this work is to irradiate fully ceramic microencapsulated (FCM) fuel in the High Flux Isotope Reactor (HFIR) to (1) facilitate irradiation of novel fuel concepts and (2) validate potential fuel performance. The FCM fuel used in this study is composed of either uranium nitride (UN) or two phase uranium oxide and uranium carbide (UCO) kernels, each of which are coated with a tristructural-isotropic (TRISO) coating layer and compacted into a silicon carbide (SiC) matrix. The TRISO layers and matrix provide multiple barriers to fission product release. Five particles are placed into the matrix and, combined, are considered a single “pellet”. This fuel concept is a candidate accident-tolerant fuel (ATF) for use in light water reactors (LWRs) and advanced reactor concepts. The potential benefits of the FCM fuel concept include greater burnup, improved fuel reliability, and improved thermal performance. The UN particles used in this fuel concept are intended to enhance heavy metal loading to achieve sustainable LWR cycle lengths. These kernels were developed and produced under the Advanced Fuels Campaign (AFC) at Oak Ridge National Laboratory (ORNL) beginning in FY15, and coating parameters for UN were completed in FY16. Production of very high-density TRISO-coated UN kernels was completed more recently in FY18. The experiment described herein is being conducted to provide basic data on the irradiation performance of these fuel pellets at relevant LWR temperatures. This report presents the irradiation test plan for this novel fuel concept.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2019

Additional Confirmatory LBL Analysis of AGR-5/6/7 Compacts and Over-Coated Particles

Fuel compacts for the Advanced Gas Reactor Fuel Development and Qualification (AGR) Program’s AGR-5/6/7 irradiation test in the Idaho National Laboratory (INL) Advanced Test Reactor (ATR) were fabricated by BWX Technologies Nuclear Operations Group (BWXT NOG) located in Lynchburg, Virginia. Two compact packing fractions (PFs) were produced - nominally, 40% PF and 25% PF - in which the tristructural-isotropic (TRISO)-coated particle volume was targeted to be approximately 40% and 25% of the total compact volume, respectively. The TRISO coatings were deposited using a 150 mm diameter fluidized-bed chemical vapor deposition (CVD) furnace on spherical kernels that were nominally 425 μm in diameter. The kernels were from kernel composite Lot J52R-16-69317, which contained low-enriched uranium (15.5% 235 U) in a mixture of uranium carbide and uranium oxide (UCO). Kernels were coated with four concentric CVD layers: a porous carbon buffer layer that was nominally 100 μm thick, an inner pyrolytic carbon (IPyC) layer that was nominally 40 μm thick, a silicon carbide (SiC) layer that was nominally 35 μm thick, and an outer pyrolytic carbon (OPyC) layer that was nominally 40-μm-thick. Coated particle composite J52R-16-98005 was overcoated (OC) with a graphite/resin blend, and these OC TRISO particles were pressed to form cylindrical compacts that were nominally a half inch in diameter and one inch long.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2012

PIE on Five Irradiated AGR-1 Compacts

Post-irradiation examination (PIE) is in progress on coated particle fuel compacts from the first Advanced Gas Reactor irradiation experiment (AGR-1). PIE has been completed on five compacts at the Oak Ridge National Laboratory (ORNL). Three compacts (Compacts 6-1-1, 4-4-2, and 5-2-3) were examined in the as-irradiated condition and two compacts (Compacts 6-4-3 and 3-3-2) were subjected to safety testing at 1600°C, followed by post-safety testing examination similar to the PIE performed on the as-irradiated compacts. All compacts were subjected to a standard set of analyses that included the following: (1) detection of exposed fission products by Deconsolidation-Leach-Burn-Leach (DLBL), (2) measurement of gamma-emitting fission product inventory using the Irradiated Microsphere Gamma Analyzer (IMGA), and (3) microstructural examination by x-ray tomography and materialography. The equipment and methods used are reported in detail in ORNL/TM-2012/233, AGR-1 Irradiated Compact 6-1-1 PIE Report, and have been summarized in the next section of this report. This report also provides a brief summary of the results of the completed PIE. Preliminary trends are discussed in this report, but final conclusions will require the support of additional data and further analysis. A separate report is being generated for each AGR-1 compact after PIE is complete that describes in detail the examinations performed and fully documents the data obtained. A final AGR-1 PIE summary report will compile all available data and provide a more comprehensive analysis of the AGR-1 fuel performance. In general, it was observed that the tristructural isotropic (TRISO) coated particles remained intact during irradiation and subsequent safety testing to 1600°C. No significant gaseous 85 Kr release was detected during the irradiation or high temperature safety testing, which would be indicative of simultaneous failure of all three outer layers of the TRISO coating. Only three particles with defective SiC layers were detected in the five compacts included in this summary. These particles were detected because they released a significant fraction of their cesium inventory, which was generally well retained. Two particles from Compact 5-2-3 released cesium during irradiation and one particle from Compact 3-3-2 released cesium during safety testing. However, it is evident that some fission products were released through intact SiC during irradiation. Most of these fission products were trapped in the compact matrix, where they could be analyzed by PIE. In terms of fractional release, the main fission products detected outside intact SiC were silver, palladium, and europium. The main impact of irradiation on the microstructure of the TRISO-coating layers was densification and shrinkage of the buffer layer, which often led to buffer fracture and subsequent enhanced swelling of the kernel. Some inner pyrocarbon (IPyC) layers were cracked by the radiation-induced changes in the buffer layer, and on rare occasion these cracks propagated into the SiC. In the two particles that released cesium during irradiation, these SiC cracks penetrated through the entire layer. The particle from Compact 3-3-2 that released cesium was not directly related to irradiation damage. Its SiC layer was determined to be porous as a result of a fabrication defect that occurs when a particle is over-fluidized in the coater, causing it to pick up carbon soot on the surface of the IPyC prior to SiC deposition. This porous SiC layer remained sufficiently intact during irradiation to retain cesium, but finally cracked during high temperature testing. Analysis of fission products remaining in the coated particles showed that the retention of silver varied dramatically from particle-to-particle within each compact. Examination with the IMGA determined that some particles contained a level of 110m Ag equivalent to that calculated to have been generated over the three-year irradiation period, while other particles contained too little to be detected by the gamma analysis. The mechanism for silver release is still being investigated. Attempts to correlate the varied release behavior to obvious radiation-induced changes in the coating layers have not been successful. Scanning electron microscopy (SEM) has provided some evidence that particles with higher silver release also show greater penetration of palladium silicide into the SiC layer, and this should be studied further.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2020

A White Paper: Disposition Options for a High-Temperature Gas-Cooled Reactor

The high-temperature gas-cooled reactor (HTGR) is a uranium-fueled, graphite-moderated, gas-cooled nuclear reactor design concept capable of producing very high core outlet temperatures. Both types of HTGR have the tristructural isotropic (TRISO) fuel kernel at the heart of the fuel design. For the prismatic block-type HTGR, the TRISO particles are overcoated with a resinated graphitic matrix and pressed into fuel compacts, which are then heat treated and placed in the fuel channels of the prismatic-block-shaped fuel assemblies. For the pebble-bed-type HTGR, the TRISO particles are dispersed in a graphitic-matrix sphere, which is the basic unit for the reactor core. Despite having very different fuel designs, both types of HTGR are graphite-moderated, gas-cooled, thermal reactors using many of the same materials. As a result, both prismatic-block-type and pebble-bed-type HTGRs have similar radioactive waste streams, all of which require safe and secure storage and eventual disposition. Modern HTGR designs are based on a long and rich operating history of several different graphite-moderated, gas-cooled, thermal reactors. Several of these reactors have been shut down, the fuel has been placed in safe storage, and they have undergone some degree of decommissioning. As such, there is significant experience in the management of the spent nuclear fuel (SNF) and radioactive wastes associated with operating these reactors. This white paper will, (1) identify the definitions and regulations that apply to the safe and secure management, storage, and disposal of radioactive waste; and (2) identify the key radioactive waste streams from HTGRs and their characteristics. Idaho National Laboratory (INL) has significant experience in the management of SNF from HTGR predecessors. This experience should form the basis for the management and disposition efforts of the radioactive waste from any new HTGR-type small modular reactor, or microreactor intended for deployment at the INL site.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2022

Safety Testing of AGR-5/6/7 Compacts 2-2-2 and 2-2-4

Compacts 2-2-2 and 2-2-4 from the Advanced Gas Reactor (AGR) Fuel Development and Qualification Program’s final irradiation campaign (AGR-5/6/7) were each separately subjected to a thermal soak at 1600°C for 300 h under flowing helium to simulated conditions experienced during a postulated high-temperature gas-cooled reactor (HTGR) depressurization conduction cooldown event. The safety testing of the fuel compacts’ performance under accident conditions was conducted in the Oak Ridge National Laboratory (ORNL) Core Conduction Cooldown Test Facility (CCCTF), which utilizes a stand-alone hot cell at the Irradiated Fuels Examination Laboratory (IFEL). The CCCTF heats fuel to temperatures up to 1900°C in a non-oxidizing environment while continuously monitoring the sweep gas for radioactive 85 Kr to detect release levels associated with hermetic failure of the tristructural-isotropic (TRISO) coating surrounding each fuel kernel. In addition, certain metallic radionuclides that escape the fuel compact are collected on deposition cups that are periodically exchanged with a new cup to obtain information on the overall retention behavior of the TRISO coating layers. Because cesium can diffuse through intact pyrocarbon layers, abnormal degradation of the silicon carbide (SiC) layer in the absence of holistic TRISO coating failure is indicated by release of 134 Cs at levels equivalent to an individual particle inventory in the absence of significant 85 Kr release (Hunn et al. 2014). Additional description of the CCCTF system is provided in Appendix A.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2023

An Assessment of Applying Pyroprocessing Technology to Advanced Pebble-Type Fuels

With an expected increased demand for high-assay low enriched uranium (HALEU) to supply advanced reactors, the possibility of recovering actinides from various used nuclear fuels (UNF) is being reassessed. Pebble-type fuels such as tristructural isotropic (TRISO) fuel are intended to be directly disposed after use, but the HALEU remaining in each pebble is a resource with increasing value. An economically feasible recovery strategy would maximize the amount of HALEU recovered for reuse in new fuel without increasing the waste volume relative to the direct disposal of used TRISO fuel. We are evaluating the technical feasibility of recycling TRISO or pebble fuels to recover actinides for reuse as new fuel for advanced reactors by using pyrochemical methods.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2023

Complete Survey of Fuel Candidates for Microreactor Purposes

This report summarizes various fuel types that may be applicable to several microreactor concepts, which are defined as (1) very high temperature reactors (VHTR), (2) sodium fast reactors (SFR), (3) system for nuclear auxiliary power (SNAP) reactors, (4) gas fast reactors (GFR), and (5) molten salt reactors (MSR). The fuel systems that were assessed include: uranium mononitride (UN), uranium monocarbide (UC), uranium dioxide (UO 2 ), uranium oxycarbide (UCO) Tristructural Isotropic (TRISO), UN TRISO, mixed oxide (MOX), metallic fuels, and metal hydrides. While UCO TRISO has undergone significant testing through the advanced gas reactor (AGR) program, the very high cost necessitates consideration of other fuel types. UN and UC were identified as fuels that should receive further investigation due to their thermophysical and mechanical properties. Minimal irradiation performance data shows that these fuels are good candidate fuels for microreactors.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2023

An Assessment of Applying Pyroprocessing Technology to Advanced Pebble-Type Fuels

With an expected increased demand for high-assay low enriched uranium (HALEU) to supply advanced reactors, the possibility of recovering actinides from various used nuclear fuels (UNF) is being re-assessed. Pebble-type fuels such as tristructural isotropic (TRISO) fuel are intended to be directly disposed after use, but the HALEU remaining in each pebble is a resource with increasing value. An economically feasible recovery strategy would maximize the amount of HALEU recovered for reuse in new fuel without increasing the waste volume relative to the direct disposal of used TRISO fuel. We are evaluating the technical feasibility of recycling TRISO or pebble fuels to recover actinides for reuse as new fuel for advanced reactors by using pyrochemical methods.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2023

Survey of Uranium Nitride and Mixed Oxide Fuels for Microreactor Applications

Different fuel systems are being proposed for use in microreactors including TRISO fuel and metallic U-Zr based fuel. TRISO fuel is considered the main fuel option for most of the industry teams. Given the need for compact size core and potential for long fuel life of a microreactor, high density fuels such as metallic and nitride fuels are potential options. Of interest here is the uranium nitride (UN) option, which can allow for higher fissile material content and higher thermal conductivity compared to conventional uranium oxide fuel, and also has higher melting temperature compared to metallic fuel. Meanwhile, the current availability is limited for high assay low enriched uranium (HALEU) that is needed for high density fuels, which motivates the consideration of using Pu as a potential replacement for HALEU until adequate production capacity is in place. Current Pu availability is mainly attributed to the inventory of excess weapons Pu rather than through reprocessing of spent nuclear fuel. This inventory of excess Pu can be used in both metallic and oxide fuel systems to replace HALEU. Of interest here, the oxide form, that is the mixed oxide form of PuO 2 and UO 2 (MOX). In this report, the options of using UN or MOX, in both pellet and TRISO fuel forms, in microreactors are evaluated in relation to their properties, fuel performance and irradiation data, as well as fabrication. Gaps related to those areas are identified for both fuel systems, to guide future activities by DOE programs such as the advanced fuels campaign (AFC), to enable their use in microreactors.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2024

Evaluation of XCT for Matrix Density Measurement of Particle Fuel Forms

Particle fuel forms generally consist of a dispersion of fuel, such as tristructural isotropic (TRISO) particles, within a refractory matrix (e.g., graphite or silicon carbide). The density of matrix materials for particle fuel forms is of interest for modeling fuel form strength and thermal properties and may be specified as a quality control parameter, depending on reactor design. Some of the uncertainty associated with traditional, manual approaches can be eliminated by performing x-ray computed tomography (XCT) on the fuel forms and applying image processing methods to generate a precise count of the number of particles. This also removes the need to include determination of particle count within each individual fuel form during fabrication. Unfortunately, reconstruction artifacts from high-Z uranium-bearing kernels prevent accurate measurement of individual particle volumes using this approach, so the use of mean particle mass and volume are still necessary for computation of average fuel form matrix density. This method of using XCT to count particles in individual fuel form for determination of average matrix density was applied to three archived compacts from the Advanced Gas Reactor Fuel Development and Qualification (AGR)-1 campaign, four archived compacts with uranium carbide/uranium oxide (UCO) TRISO from the AGR-2 campaign, and three archived UO 2 -TRISO compacts from the AGR-2 campaign. The resulting density values were compared with those previously reported, showing slight changes due to uncertainties in the previously used number of particles in each of these cylindrical, graphite matrix compacts.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2024

Summary of Leach-Burn-Leach Round-Robin Test Results

Tristructural isotropic (TRISO) coated particle fuel is of interest to multiple member states associated with the Generation IV International Forum (GIF). Qualification and acceptance testing of TRISO fuel includes the determination of particle defect fractions and impurities in the as-fabricated TRISO fuel particle and/or composited fuel form, which are typically determined using burn-leach (BL) or leach-burn-leach (LBL) analysis methods. A round-robin test focusing on LBL analysis was undertaken by the GIF Very High Temperature Reactor System Fuel and Fuel Cycle Project Management Board. Participating in this LBL round-robin test were research staff from the Institute of Nuclear and New Energy Technology (INET) in the People’s Republic of China, the Korean Atomic Energy Research Institute (KAERI) in the Republic of Korea, and Oak Ridge National Laboratory (ORNL) in the United States of America. The motivation of this LBL benchmarking exercise was to explore consistency in results generated by LBL and to elucidate the potential influence of variations in the procedures used by the participating members on the accurate determination of the measured fuel properties.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2024

Assessment and validation of NEAMS tools for high-fidelity multiphysics transient modeling of microreactors: Application of NEAMS codes to perform multiphysics modeling analyses of micro-reactor concepts

The NEAMS Multiphysics Applications team aims at providing assessment of code useability and functionality for microreactor design and analyses, together with demonstration of their capabilities to properly capture the steady-state and time-dependent behavior of different microreactor concepts. In FY-24, significant progress was achieved in improving multi-physics models of several microreactors systems: HP-MR, GC-MR and KRUSTY. These efforts focused on solving more complex multiphysics problems enabled by enhanced tools capability, verifying and validating results obtained, providing feedback to developers for suggested improvements, and sharing these models to facilitate user training. A series of new multiphysics transients were completed on the HP-MR (using Griffin/BISON/Sockeye) with core startup transient, control drum inadvertent rotation accident, and hydrogen leakage from hydride moderator (also including SWIFT). On the GC-MR, a new full-core model was developed and analyzed through a series of new multiphysics (Griffin/BISON/SAM) transients to simulate moderator leakage (also including SWIFT), flow blockage and coolant depressurization. Additional and updated TRISO failure analyses were completed on the HP-MR unit-cell and GC-MR assembly models leveraging improved TRISO modeling capabilities. The amount of SiC failure following accidental transients at end-of-life was null. However, GC-MR assembly TRISO analysis highlighted Pd penetration rate can be problematic and may require design changes on the studied microreactor concept. The neutronics discrepancies observed on the KRUSTY model in previous years were resolved using hybrid set of Monte Carlo/Deterministic cross-sections. The multiphysics (Griffin neutronics / BISON thermal-mechanics) 15₵ insertion transient simulation displayed good agreement when comparing with experimental data. Initial modeling of the 30 ₵ reactivity insertion also displays promising results. Such close agreement provides important validation data that can be leveraged by the NEAMS program and by microreactor vendors to support licensing of their technology. Finally, important experience was gathered with the NEAMS tools leading to several user feedback shared with tools developers, especially with regards to MOOSE mesh generator and Griffin. This project led to many publications demonstrating modeling capabilities, and to three models shared on the Virtual Test Bed.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2025

Benchmark Gap Assessment for the Manufacturing of High-Assay Low-Enriched Uranium Fuels

This document develops basic critical conditions for spheres—moderated and unmoderated, as well as reflected and unreflected—in consideration of nuclear criticality safety of a potential fuel production facility producing high-assay low-enriched uranium (HALEU) fuel of several different types like tristructural-isotropic (TRISO), uranium metal and alloys, oxide and non-metallic forms. In addition to spherical arrangements, TRISO particle manufacturing process–specific equipment is modeled as it would be for the criticality safety analysis. The objective is to develop representative systems that can then be used for comparison with existing benchmarks. SCALE/TSUNAMI is used to assess the similarity index between these systems to assess validation gaps for possible fuel production applications of proposed advanced reactors. Several different fuel types were evaluated, including TRISO, uranium metal, uranium molybdenum, uranium zirconium, uranium dioxide, uranium nitride, uranium hydride, U-ZrH, and uranium chloride. This selection of fuel types covers a breadth of proposed reactor types, as well as intermediate steps in the production and fabrication of the fuel

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2025

Destructive PIE and Safety Testing of Six AGR-5/6/7 Capsule 2 Compacts

This study evaluates fission product retention and particle failure mechanisms in AGR-5/6/7 Capsule 2 uranium carbide and uranium oxide (UCO) tristructural isotropic (TRISO) fuel under high-temperature gas reactor accident-relevant conditions using high-temperature safety tests and destructive postirradiation examination. Three Capsule 2 compacts were held isothermally at 1600°C for approximately 300 hours and one compact at 1800°C for approximately 300 hours; two additional compacts were examined in the as-irradiated state. Post-test deconsolidation–leach–burn–leach (DLBL) quantified nuclide inventories in matrix and particles. Individual particles were surveyed for radioisotope inventories, and microanalytical approaches resolved microstructural evolution and fission product distributions within the coating layers. At 1600°C, no krypton was detected above the minimum detectable limit, and cesium releases were far below a single particle equivalent, indicating the absence of full TRISO failure or SiC failures. Silver releases were limited and primarily reflected depleted postirradiation inventories, consistent with prior compact-level exams indicating substantial in-pile 110mAg loss. At 1800°C, cumulative 134Cs release of approximately 2.5 particle equivalents and delayed 85Kr totaling approximately 0.53 particle equivalents were consistent with one full TRISO failure and two SiC failures. Europium and strontium releases were roughly one order of magnitude higher than at 1600°C and comparable to AGR-1/AGR-2 high-temperature tests, with sustained late-hold rates indicating diffusion through intact coatings coupled with matrix depletion. Overall, AGR-5/6/7 Capsule 2 UCO fuel demonstrated fission product retention during safety testing consistent with prior AGR campaigns, while distinctive in-pile 110mAg depletion and measurable 1600°C europium loss motivate targeted follow-on studies.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2025

Application of Raman Spectroscopy to Determine Uranium Content in ADUN Solution

The work presented in this report is part of the ongoing efforts to address the nuclear material control and accounting needs for advanced reactor fuel fabrication facilities. This work was supported by the Materials Protection, Accounting, and Control Technologies (MPACT) program under the US Department of Energy Office of Nuclear Energy‘s Nuclear Fuel Cycle and Supply Chain program. The activities and engagements under the MPACT program are designed to support a robust US civilian nuclear energy enterprise. In the work described in this report, we supported MPACT objectives by developing measurement techniques that could be used for material accounting and process monitoring and by working with industry partners to identify existing gaps and areas for improvement. Oak Ridge National Laboratory has been working with commercial tristructural isotropic (TRISO) fuel fabricators such as Standard Nuclear to develop technology for rapid and cost-effective uranium content assessment. This work has focused on demonstrating advanced measurement techniques (e.g., Raman spectroscopy) that can be used for rapid, reliable, and cost-effective routine measurements of uranium content in feed solutions and liquid waste streams as well as for monitoring in-line process measurements and product streams. Specifically, this report explores techniques for accurately determining uranium content in acid-deficient uranyl nitrate (ADUN) solutions and detecting low uranium concentrations in ammonia solutions. Developing such measurement techniques will benefit TRISO fuel fabrication facilities, facilities involved in other parts of the fuel cycle that require online monitoring of aqueous solutions, and potentially molten salt fuel reactors. This work supports developing Raman spectroscopy procedures to determine uranium concentrations in ADUN solutions, which are used as feedstock in the sol–gel process for creating TRISO fuel. Some additional benefits of using Raman spectroscopy for uranium quantification in fabrication facilities include enabling online monitoring of the chemical process, which would provide near real-time feedback; eliminating the need for sample transfers, preparation, or dilution; providing nondestructive measurements; and user friendliness. In this fiscal year, FY25, we determined the identity of the unknown Raman band at approximately 853 cm−1 that was discovered in ADUN Raman spectra in FY24, created calibration curves and determined uranium concentrations of two ADUN solutions, and compared the Raman results to results obtained from inductively coupled plasma mass spectrometry and Davies–Gray titration. Furthermore, we have identified focus areas for experimentation in future fiscal years. A key result is that the accuracy of using Raman can provide accuracy comparable to destructive analysist techniques, With a well-developed calibration curve, using standards and a large number of samples (more than five samples), uncertainty on the order of 1%–3% is achievable. Given that the uncertainties achieved by Raman spectroscopy were on the order of the uncertainties achieved using ICP-MS, we conclude that with a well-developed procedure Raman spectroscopy can be used to determine uranium concentrations in ADUN solutions for NMC&A applications. The benefits of such an approach are that the time and effort will be less than that of comparable destructive analysis techniques, with approximately the same level of technical expertise. This will be attractive to operators of fuel fabrication facilities as it will lower costs and improve efficiencies.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2025

Destructive PIE and Safety Testing of Six AGR-5/6/7 Capsule 2 Compacts

This study evaluates fission product retention and particle failure mechanisms in AGR-5/6/7 Capsule 2 uranium carbide and uranium oxide (UCO) tristructural isotropic (TRISO) fuel under high-temperature gas reactor accident-relevant conditions using high-temperature safety tests and destructive post-irradiation examination. Three Capsule 2 compacts were held isothermally at 1600°C for approximately 300 hours and one compact at 1800°C for approximately 300 hours; two additional compacts were examined in the as-irradiated state. Post-test deconsolidation–leach–burn–leach (DLBL) quantified nuclide inventories in matrix and particles. Individual particles were surveyed for radioisotope inventories, and microanalytical approaches resolved microstructural evolution and fission product distributions within the coating layers. At 1600°C, no krypton was detected above the minimum detectable limit, and cesium releases were far below a single particle equivalent, indicating the absence of full TRISO failure or SiC failures. Silver releases were limited and primarily reflected depleted post-irradiation inventories, consistent with prior compact-level exams indicating substantial in-pile 110m Ag loss. At 1800°C, cumulative 134 Cs release of approximately 2.5 particle equivalents and delayed 85 Kr totaling approximately 0.53 particle equivalents were consistent with one full TRISO failure and two SiC failures. Europium and strontium releases were roughly one order of magnitude higher than at 1600°C and comparable to AGR-1/AGR-2 high-temperature tests, with sustained late-hold rates indicating diffusion through intact coatings coupled with matrix depletion. Overall, AGR-5/6/7 Capsule 2 UCO fuel demonstrated fission product retention during safety testing consistent with prior AGR campaigns, while distinctive in-pile 110m Ag depletion and measurable 1600°C europium loss motivate targeted follow-on studies.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2026

Microreactor Core Transportation Cask Model Description for Criticality Safety Validation Basis Assessment (Rev. 2)

Criticality safety analyses are completed on transportation casks used for microreactor whole core shipment to provide examples of models and analyses to industry, regulators, and nuclear community at large to be used in verification and validation analyses of similar applications. The microreactors considered are based on a Gas-Cooled Microreactor (GCMR) and a Heat-Pipe Microreactor (HPMR), both utilize HALEU fuel in the form of TRISO particles and various other design options considered in industry microreactor designs. Variant design options of GCMR and HPMR were also investigated to provide a wider application range for each technology. Criticality safety analyses for the GCMR and HPMR packages were performed using the CSAS6 sequence of SCALE 6.3.2 with the ENDF/B-VII.1-based continuous energy neutron libraries. Different scenarios were investigated, including normal operation and water flooded conditions to represent nominal and hypothetical accident scenarios. Sensitivity and similarity analyses are also performed using the TSUNAMI sequence of SCALE 6.3.2, and the similarity analysis uses all the experiments from the ICSBEP Handbook with High Enriched Uranium (HEU), Intermediate and mixed Enriched Uranium (IEU) and Low Enriched Uranium (LEU) systems. Many ICSBEP experiments were found marginally similar, with similarity index (ck) values greater than 0.8, to the GCMR and HPMR cask models, especially in flooded conditions that may be more constraining due to reduced reactivity margins. Some experiments using TRISO fuel particles and graphite moderator, including the recent THETA and Deimos experiments from LANL, together with some IRPhEP experiments, were also used for the similarity analyses. These TRISO-fueled and graphite moderated experiments behaved similarly to the GCMR models, with maximum ck value greater than 0.9, but they are less similar to the HPMR models. This observation indicates that additional critical experiments might be needed to further validate the criticality safety models, especially for heat-pipe based microreactor transport packages and for non-flooded transportation configurations.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗