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DOE OSTI2023

Behavior of contaminants and simulant fission products in the advanced chlorination process

The University of Tennessee, Knoxville and Oak Ridge National Laboratory have completed proof-of principle testing on an advanced sulfur-based zirconium and aluminum chlorination process for the recovery of Zr or Al from spent fuel claddings and purification of the products. This process could be used to recover hafnium-free nuclear-grade zirconium for reuse or disposal as low-level waste. Testing showed that even non-optimized reaction protocols could produce zirconium product streams from simulated irradiated fuel with purities >90%. The chlorination process was tested on representative fission product species that would be found in Advanced Test Reactor fuel (ATR). First, fission product generation was determined through modeling and simulation of the ATR. The generation of fission products was used to selected contaminants and potentially volatile fission product simulants for laboratory testing. The goal is to identify which species may react with the sulfur-chlorine reagents and be transported into the advanced chlorination off-gas.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2024

BISON Simulated and Experimental Fission Product Release Comparisons from Reradiated AGR-3/4 Compacts During High Temperature Heating Tests

The fuel performance modeling code BISON was used to predict the release of fission products iodine-131 (131I), xenon-133 (133Xe), and krypton-85 (85Kr) from four re-irradiated AGR-3/4 fuel compacts containing tristructural isotropic (TRISO) coated particles during high-temperature isothermal heating tests. The AGR-3/4 fuel compacts were irradiated in the Advanced Test Reactor (ATR) as part of the third and fourth series of planned experiments to support the Advanced Gas Reactor (AGR) Program. They were subsequently stored and re-irradiated in the Neutron Radiography (NRAD) reactor for approximately five days and then stored for another five to eight days before being subjected to isothermal heating tests in the Fuel Accident Condition Simulation (FACS furnace) for 200 to 300 hours at temperatures between 1000°C and 1600°C to evaluate fission product release at elevated temperatures. New nuclide-specific fission product source term models for the three nuclides of interest were developed using the reactor multiphysics code Griffin and implemented into BISON to support this work. The new source term models were incorporated into coupled compact- and particle-scale BISON simulations, which predict spatially- and temporally-resolved radionuclide generation, radioactive decay, transport, and release throughout the entire irradiation history, including the initial ATR irradiation, NRAD re-irradiations, FACS heating tests, and intermediate periods spent in storage. The experimentally measured fission product release from the heating tests were compared to modeling release predictions calculated by BISON to evaluate how well the code compares to experimental results. Overall, the experimental measured and BISON predicted comparative release results varied but generally agreed to within 5 particle equivalents. Comparative release results identified general observations to take into consideration to help refine future models and reduce uncertainties associated with both the measurement results and predictive results. This includes developing new uranium oxycarbide (UCO) specific kernel diffusivities for the three isotopes examined to more accurately reflect the material properties of the fuel form. Deriving new diffusivities will aid in producing a more informed BISON model

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2023

Catalyzed oxidation of nuclear graphite by simulated fission products Sr, Eu, and I

The influence of three fission products Sr, Eu, and I on the oxidation of IG-110 nuclear graphite was studied in the temperature range of 400 to 1000 °C. Sr and Eu were introduced as chlorides, and I was introduced as NaI. The temperature dependence of both CO 2 and CO production during the graphite oxidation measured with mass spectroscopy and infrared spectrometry shows that the introduction of these three compounds to graphite significantly decreases the onset temperature for the oxidation of graphite. Among the three compounds, NaI is the most active towards the oxidation reaction, characterized by a significant decrease of the onset temperature from approximately 650 to 400 °C before and after its introduction to graphite. Separate measurements of CO 2 and CO concentration at varying temperatures enable the calculation of the activation energy for the formation of CO 2 and CO. The activation energies for the oxidation of pure and fission product-impregnated graphite samples decrease in the following order: standard IG-110 graphite, EuCl 3 -impregnated IG-110, SrCl 2 -impregnated IG-110, and NaI-impregnated IG-110. This trend indicates that the three compounds catalyze the oxidation of graphite at temperatures relevant to the operation of high-temperature gas-cooled reactors. Furthermore, it is found that the three compounds can also affect the molar ratio of reaction products CO 2 and CO, and the rates of the graphite oxidation. At temperatures higher than about 850 °C, the impregnated samples exhibit lower CO 2 : CO ratios than the pure graphite. Different from EuCl 3 and NaI, the introduction of SrCl 2 decreases the graphite oxidation rates at temperatures higher than about 770 °C. Their catalytic mechanism can be understood based on a redox cycle of the intermediate active species, promoting the dissociation of molecular oxygen and transfer to the carbon.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2024

237 Np Fission Spectrum Cumulative Fission Product Yield Measurement Using Godiva IV Critical Assembly

Precise integral measurement of fast neutron-induced fission product yields for various actinides is of high interest for applied nuclear science. The goal of this effort is to improve uncertainties in fission product yield values of 237 Np. Fission was induced in a NpO 2 (NO 3 ) target using the Godiva IV critical assembly in burst mode. The irradiated sample was transferred to a high-resolution γ-ray detection setup within 50 minutes. γ-ray list mode data was collected from 50 minutes to 1 week after the irradiation. γ-ray spectroscopy was performed to analyze the time dependent γ-ray yields using an automated peak search algorithm to identify isotopes by their decay γ-ray energy and half-life. Finally, the initial activity for each isotope identified was used to calculate their fission product yield.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2024

239 Pu Fission Spectrum Cumulative Fission Product Yield Measurement Using Godiva IV Critical Assembly

Precise integral measurement of fast neutron-induced fission product yields for various actinides is of high interest for applied nuclear science. The goal of this effort is to improve uncertainties in fission product yield values of 239 Pu. Fission was induced in a pure 239 Pu (>99%) target using the Godiva IV critical assembly in burst mode. Further, the irradiated sample was transferred to a high-resolution γ-ray detector within 45 minutes. γ-ray list mode data was collected from 45 minutes to 1 week after the irradiation. γ-ray spectroscopy was performed to analyze the time dependent γ-ray yields using an automated peak search algorithm to identify isotopes by their decay γ-ray energy and half-life. The initial activity for each isotope identified was used to calculate their fission product yield.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2021

Thermochemically-informed mass transport model for interdiffusion of U and Zr in irradiated U-Pu-Zr fuel with fission products

A new formulation for redistribution of constituents in metallic U-Pu-Zr nuclear fuel is presented that can incorporate the contributions from fission products. The formulation is based on the thermodynamic driving forces derived from the generalized chemical potential that includes effects of composition and temperature. As a result, the redistribution model can readily account for the composition changes due to the generation of fission products while using only a limited set of transport coefficients. The thermodynamic model for the metallic fuel and thermochemistry solver Thermochimica were coupled with the nuclear fuel performance code BISON to implement the redistribution model. The simulations reproduce an experimentally observed Zr-depletion zone in the mid-radius region of an irradiated fuel slug. The generation of fission products during burnup is shown to have a stabilizing effect on the fuel chemistry, slowing the rate of U-Zr interdiffusion and reducing the size of the Zr-depleted zone. Here, the overall objective of the work is to advance predictive capabilities of fission product behaviour in U-Zr metallic fuel in the context of fuel performance and safety.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2022

Energy Dependent Fission Product Yields

Since 2011, the LLNL-LANL-TUNL collaboration has undertaken experimental measurements of the energy evolution of the chain fission product yields (FPY) from neutron-induced fission of 235 U, 238 U, and 239 Pu using quasi-monoenergetic neutrons produced at the TUNL 10 MV Van de Graaff accelerator. Our method relies on direct, post-irradiation γ-ray spectroscopy of γ-rays emitted by fission products in actinide targets, with multiple γ-ray spectra taken continuously for a period from a half-hour to three months from the end of irradiation. The main experimental results of this study have been published for eight incident neutron energies of En = 0.58, 1.37, 2.37, 3.6, 4.6, 5.5, 8.9 and 14.8 MeV [1–4]. For each incident energy, approximately 16 cumulative FPYs were determined, nearly all being high-yield fission products, i.e., those occurring in the peaks of the mass distributions. As will be described in this report, our FPY analysis has been significantly improved in every step of the process, reducing the overall systematic uncertainties compared to previously published data.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2020

Analysis of fission product distribution and composition in the TRISO layers of AGR-2 fuel

The Advanced Gas Reactor Fuel Qualification and Development Program's second irradiation experiment focuses on the performance of fuel particles produced in an industrial-scale coating system. Ongoing post-irradiation examination efforts include exploration of tristructural-isotropic (TRISO)-coated particle fuel in the as-irradiated state and subjected to elevated temperatures to simulate accident conditions (safety testing). Scanning electron microscopy (SEM) analysis with energy dispersive x-ray spectroscopy (EDS) was used to show the distribution of fission products within the TRISO layers. The SEM analysis showed a variation of fission product distribution within the TRISO layers based on irradiation temperature, burnup, individual particle fission product inventory retention, safety testing history and kernel composition. Finally, a key observation is that particles which likely experienced higher temperature showed a greater diversity and distribution of fission products and actinides in the IPyC and SiC layers, implying that temperature is a dominant variable influencing the transport of radionuclides in TRISO particles.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2021

Fission product distribution in irradiated safety-tested and as-irradiated AGR-2 TRISO particles

In this work, two tristructural isotropic (TRISO)-coated nuclear fuel particles were examined by electron probe microanalysis (EPMA) as part of the Advanced Gas Reactor program. The compacts’ average irradiation temperatures ranged from approximately 1260 to 1290 °C. One particle was examined in the as-irradiated condition, while the other was subject to 1600 °C post-irradiation safety testing. This study was undertaken to test a newly-developed EPMA technique to determine fission product masses in TRISO particles on a layer-by-layer basis, and to compare fission product distributions between an as-irradiated and safety-tested particle. Fission product concentration profiles were collected along two radii in each particle, with measured concentrations used to compute the fission product mass in each TRISO particle layer. These measured masses were then compared to those predicted from ORIGEN modeling calculations. Data collected from these measurements show that for these two particles, masses determined via EPMA were within ± 20% of the calculated masses for the rare-earth elements, Mo, Zr, Cs, I, and Pd. Elements that tend to be less homogeneously distributed include Sr, Te, Eu, Ag, and possibly Ba. Measured Ag masses differed by more than 40% from the calculated mass. Lanthanides other than Eu remain primarily within the fuel kernel in the as-irradiated particle but in the safety-tested particle these element masses were divided approximately equally between the kernel and kernel periphery. In both particles, the majority of Sr and Eu accumulated in the carbon-rich kernel periphery, although in the safety-tested particle, Sr and Eu accumulated farther from the fuel kernel than occurred with irradiation alone. A greater mass fraction of mobile elements, such as Cs and I accumulated in the buffer and IPyC in the safety-tested particle as compared to the as-irradiated particle. When fully developed and tested, this mass balance approach to TRISO particle analysis has the potential to provide insight into fuel behavior.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2023

Fission product yields from the 238 U ( n,f ) reaction at E n = 4.6 MeV

Here, we present cumulative fission product yields from the 238 U (n, f) reaction at an incident energy of 4.6 MeV for fission products with half-lives from less than one second to several hours. We employed direct γ-ray spectroscopy to measure unseparated fission products with a conventional neutron activation analysis and a cyclic activation technique using the RApid Belt-driven Irradiated Target Transfer System (RABITTS). Yields were determined for 78 isotopes and isomers, covering the mass range 84 ≤ A ≤ 148 and the charge range from 33(As) ≤ Z ≤ 58(Ce). Our experimental cumulative yields are compared to the literature and evaluated data at E n ≈0.5 MeV from ENDF/B-VIII.0 and JEFF-3.3 libraries and with theoretical models using the GEF and FREYA codes at E n =4.6 MeV.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2021

Fission Product Transport in TRISO Particles and Pebbles

This document demonstrates completion of the goals described in the technical narrative of the FOA project titled: ”Modeling and Simulation Development Pathways to Accelerating KP-FHR Licensing” regarding fission product transport in the Kairos-proposed fuel pebble by INL and Kairos Power. Showcased in this report are code developments and simulations in BISON that extend the state of the art in computation and understanding of fission product transport in a TRISO fuel particle and pebble. These enhancements lay the foundation for making predictions of fission product transport that can be used as input in the fuel licensing process. This was achieved by installing existing fuel material models originally used in PARFUME, developing a new failure probability method that is efficient and multi-dimensional, employing material homogenization, and expanding verification and validation simulations to demonstrate the efficacy of the work. All this work is leveraged to spotlight the main deliverable; a three-dimensional model and corresponding demonstration simulation of a pebble, which will serve as the starting point for models used to predict fission product release.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2023

Fission Product Transport in TRISO Particles and Pebbles

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2023

Property Measurements of NaCl-UCl 3 and LiF-NaF-KF Molten Salts Doped with Surrogate Fission Products

Knowing thermophysical and thermochemical property values of salts over the expected range of operating temperatures is essential to modeling and simulation efforts that support the commercialization of molten salt reactor (MSR) technologies. Salt properties being measured at Argonne include thermal transitions, phase behavior, heat capacity, density, surface tension, volumetric thermal expansion, thermal diffusivity, thermal conductivity, and viscosity. The properties of several salts of interest including NaCl-UCl 3 and LiF-NaF-KF (FLiNaK) have been measured at Argonne and reported previously. These property measurements are suitable for use in evaluating reactor performance during startup and the early operating life of the reactor. The physical and chemical behavior of the fuel salt is altered by the buildup of fission products and the resulting changes in heat transfer and other properties must be understood by reactor developers. This report summarizes melting behavior, heat capacity, and thermal diffusivity values that were measured for mixtures of FLiNaK and NaCl-UCl 3 salts that have been doped with surrogate fission products. Additional heat capacity measurements were also performed on a separate mixture of FLiNaK without dopants. Measured properties are suitable for incorporation into the Molten Salt Thermal Properties Database–Thermochemical (MSTDB–TC) and the Molten Salt Thermal Properties Database–Thermophysical (MSTDB–TP) to support the development of MSRs. Salts were prepared by doping eutectic mixtures of NaCl-UCl 3 and FLiNaK with surrogate fission products. These salts were prepared for use in salt spill experiments being performed at Argonne and were subsequently used for thermal property measurements. Thermal transitions and heat capacities were measured by using differential scanning calorimetry (DSC) and thermal diffusivity was measured by using laser flash analysis (LFA) at temperatures spanning the typical MSR operating range. The measured property values of the doped salts were compared to measured property values of salts without fission products to quantify the effects of the doped fission products.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2023

Removal of fission product tellurium and iodine from recently irradiated HEU using copper metal

Gamma detection of select fission products or activation products such as 153 Sm and 239 Np in a fission sample is difficult due to gamma interferences from radiotellurium and radioiodine. To aid in the detection of these difficult-to-detect nuclides, the radiotellurium and radioiodine were removed using Cu metal turnings. This method is highly effective at the removal of the interfering radionuclides removing > 98% of the radiotellurium and radioiodine. A mechanistic study was conducted. Determining the deposition mechanism, using a number of techniques including XANES and electrochemistry providing an understanding of the electrochemical path for the Te deposition. Initial work focused on the use of stable Te, further expanding into activated TeO 2 , and a fresh fission sample. Importantly, this method presents a rapid method for the direct detection of select fission products that could have a significant impact on nuclear related fields including nuclear forensics.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

DOE OSTI2025

A machine learning approach to quantify degradation of nuclear fuels and the effects of fission products

Nuclear fuel performance is critically dependent on understanding the evolution of fuel properties under operational conditions, a complex challenge driven by chemical changes and substantial radiation damage during fission. Traditionally, property evolution has been determined via empirical data collected following irradiation. However, these empirical correlations are limited in their applicability beyond the specific conditions in which they were obtained. This study explores a novel approach to address this challenge by applying materials informatics to develop a machine learning random forest (ML-RF) model that captures the effects of fission products on fuel compounds. The model predicts formation enthalpy (ΔH f ) by leveraging extensive quantum materials property data and correlating it with material descriptors such as composition, atomic and site features, and crystal lattice properties. This ML-RF model enables rapid interpolation across the compositional and structural spaces covered by the training data, thus supporting high-throughput screening and energetic ranking of candidate phases. The model demonstrates the ability to predict ΔH f with a mean absolute error (MAE) of approximately 0.1 to 0.2 eV/atom across a wide range of compounds, including key nuclear fuel systems (U-O, U-N, U-C, U-Si, and U-Mo). For example, it was used to assess shifts in stoichiometry for UO 2 (O/M) and UN (N/M) fuels, revealing their distinct tendencies in chemical potential variation and enabling preliminary convex hull analyses. Furthermore, the model provides insights into how individual fission products affect fuel properties. Results indicate that larger fission products (e.g., Nd, Pu, Ce) have a more pronounced impact on UO 2 , while lighter ones (e.g., Zr) strongly influence UN. Here, the model developed in this work can be used to support the Accelerated Fuel Qualification approach by facilitating preliminary evaluations prior to extensive materials modeling and experimentation. To this end, the trained model has been made available to the fuel community to support ongoing fuel development efforts.

Accelerated fuel qualification↗

DOE OSTI2023

Machine learning methods for fission product identification from Bragg curves

A fission time projection chamber (fission-TPC) was developed to provide precise neutron-induced fission measurements for several major actinides. As fission fragments lose energy in one of the gas volumes of the fission-TPC, energy loss information is captured and may be used to determine fission product yields as the stopping power of an ion is dependent on the atomic number. The work presented here demonstrates the ability to apply machine learning techniques for Bragg curve classification. A set of one million energy loss curves for 24 different fission-fragment elements was generated using common stopping power software. A ResNet architecture optimized for 1D data was used to train, test, and validate a model for light and heavy fission fragments using the simulated data. The resultant classification accuracy for the light and heavy fragments indicates that this could be a viable method for elemental classification of data from the fission-TPC.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2025

Monitoring Methods for Early Detection of Inadvertent Fission Product Release at the Advanced Test Reactor

Isotope effluent data obtained during three instances of experiment failures at the Advanced Test Reactor (ATR) are analyzed to provide an overview of the methods used to detect initial signs of unintended fission product release. The data is contextualized with the operational experience, including means of identification and subsequent mitigation strategies, gained during these events. General trends as well as variations in isotopic behavior between the three failures are explored. Background on the Real Time Monitor, a High Purity Germanium detector, and other fission product monitoring systems utilized at the Advanced Test Reactor is also provided. The presented analysis was used to establish administrative action levels which are currently utilized by ATR for early detection of experiment fission product release. Early identification provides time to make programmatic decisions before approaching safety and environmental limits.

21 - SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLAN↗

DOE OSTI2020

Precision γ-ray branching ratio measurements for long-lived fission products of importance to nuclear-security applications (TAMU Annual Report 2020)

Continuing with our effort of precisely measuring the branching ratios for long-lived fission products we have collected and measured two radiopure ¹⁵⁶Eu samples. The samples were collected on thin (40 μg/cm²) carbon-foil backings using a low-energy mass-separated beam of A = 156 fission products from CARIBU at Argonne National Laboratory. During collection, a HPGe detector was used to continuously monitor the implantation rate by detecting the characteristic γ rays emitted following the β decay of the shorter-lived fission products. The first sample had measured activity of 375 Bq while the second one had an activity of 700 Bq. The implanted samples were then shipped to Texas A&M University for measurement of the subsequent decay.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗