AGR-3/4 Fission Product Transport Analysis Results
Analysis results for AGR 3/4 fission product transport
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
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Experimental confirmation of first-principles thermal conductivity in Zirconium-doped ThO 2
The degradation of thermal conductivity in advanced nuclear fuels due to the accumulation of fission products and irradiation-induced defects is inevitable, and must be considered as part of safety and efficiency analyses of nuclear reactors. Here, this study examines the thermal conductivity of a zirconium-doped ThO 2 crystal, synthesized via the hydrothermal method using a spatial domain thermoreflectance technique. Zirconium is one of the soluble fission products in oxide fuels that can effectively scatter heat-carrying phonons in the crystalline lattice of fuel. Thus, thermal property measurements of zirconium-doped ThO 2 single crystals provide insights into the effects of substitutional zirconium doping, isolated from extrinsic factors such as grain boundary scattering. The experimental results are compared with first-principles calculations of the lattice thermal conductivity of ThO 2 , employing an iterative solution of the Peierls-Boltzmann transport equation. Additionally, the non-perturbative Green's function methodology is utilized to compute phonon-point defect scattering rates, accounting for local distortions around point defects, including mass difference changes, interatomic force constants, and structural relaxation. The congruence between the predicted results from first-principles calculations and the measured temperature-dependent thermal conductivity validates the computational methodology. Furthermore, the methodologies employed in this study enable systematic investigations of thermal conductivity reduction by fission products, potentially leading to the development of more accurate fuel performance codes.
36 - MATERIALS SCIENCE↗
Deconsolidation and Leach Burn Leach of Seven As Irradiated AGR 5/6/7 TRISO Fuel Compacts from Capsules 2, 3, 4, and 5
Seven as-irradiated Advanced Gas Reactor (AGR) 5/6/7 compacts underwent destructive post-irradiation examination via deconsolidation-leach-burn leach at Idaho National Laboratory (INL). The selection of the compacts extended the upper and lower limits of time-average volume-average (TAVA) temperature for compacts that had gone through deconsolidation-leach-burn leach so far. The measured inventories of fission products and actinides in the compact matrix and outer pyrolytic carbon were reported. Results indicated unexpectedly higher rates of fuel kernel leaching compared to compacts from AGR-1 and AGR-2. These failure rates were attributed to damage during post-irradiation sample handling, rather than irradiation itself. AGR-5/6/7 compacts have little or no matrix coverage for some particles at the top and bottom ends of cylindrical fuel compacts, making them more fragile. Sixty particles were randomly sampled from each compact, and the gamma results were reported. Three SiC shells from were identified, one of which showed signs of chemical attack in the high-irradiation temperature compact.
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Evaluation of an Accident Tolerant Fuel Leak in the Advanced Test Reactor
Accident Tolerant Fuels (ATF), which are nuclear fuel sources designed to withstand operational irregularities and incidents, have been a topic of interest in the nuclear industry for several decades. Interest in ATF technology surged following the 2011 accident at Fukushima Daiichi in Japan. At the Advanced Test Reactor (ATR), one of Idaho National Laboratory’s (INL) four operating nuclear reactors, the ATF program is a collaborative effort between the national laboratory and various stakeholders within the nuclear industry. This program focuses on the research and development of novel fuel compositions, cladding, and component materials with enhanced accident-resistant properties. During one of ATR’s 60-day operating cycles in 2024, the reactor experienced five unplanned shutdowns. Following the fifth shutdown, radiation monitors detected an increase in radiation levels coming from the loop piping. Subsequent water samples confirmed the cause was a leak of fission products from the ATF experiment, designated as ATF-2C. The source of the leak was identified as the instrumented section of the test train. The primary discussions in this presentation are 1) the design of the ATF test train, 2) the operating parameters leading up to and following the detection of the leak, and 3) the quantification and characterization of the released fission products.
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Multi-element isotopic analysis of hot particles from Chornobyl
Microscopic fuel fragments, so-called “hot particles”, were released during the 1986 accident at the Chornobyl nuclear powerplant and continue to contaminate the exclusion zone in northern Ukraine. Isotopic analysis can provide vital information about sample origin, history and contamination of the environment, though it has been underutilized due to the destructive nature of most mass spectrometric techniques, and inability to remove isobaric interference. Recent developments have diversified the range of elements that can be investigated through resonance ionization mass spectrometry (RIMS), notably in the fission products. The purpose of this study is to demonstrate the application of multi-element analysis on hot particles as relates to their burnup, particle formation in the accident, and weathering. The particles were analysed with two RIMS instruments: resonant-laser secondary neutral mass spectrometry (rL-SNMS) at the Institute for Radiation Protection and Radioecology (IRS) in Hannover, Germany, and laser ionization of neutrals (LION) at Lawrence Livermore National Laboratory (LLNL) in Livermore, USA. Comparable results across instruments show a range of burnup dependent isotope ratios for U and Pu and Cs, characteristic of RBMK-type reactors. Results for Rb, Ba and Sr show the influence of the environment, retention of Cs in the particles and time passed since fuel discharge.
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Multiexciton quintet state populations in a rigid pyrene-bridged parallel tetracene dimer
The multiexciton quintet state, 5 TT, generated as a singlet fission intermediate in pairs of molecular chromophores, is a promising candidate as a qubit or qudit in future quantum information science schemes.
36 MATERIALS SCIENCE↗
Chemical Modeling of the Capture of Radioiodine Species
Iodine is a common fission product resulting from the transmutation of uranium fuel in nuclear power reactors. The short-lived radioactive isotope, 131 I, with a half-life of around eight days, would be a particular health concern if released into the environment. Capture materials, such as activated carbon, are used routinely in nuclear power plants and medical isotope production facilities to remove this hazard during normal operations to reduce emissions to acceptable levels. Iodine, unlike other common fission products such as noble gases, is challenging because of the wide range of molecular forms and oxidation states (from +VII in IF 7 to -I in iodide) that it displays, which can interconvert both in the gas phase and in the solution phase for example. The work in this project is focused on three computational tasks. In the first, we consider the binding of iodine-containing molecules of varying oxidation states to the major component of activated carbon – pristine graphene-like sheets. The second task focused on molecular binding and possible chemical transformations resulting from the reaction of molecular iodine with chemical functional groups on the edge of the graphene sheets or surface defects in the sheet itself. The final task was associated with radiolytic breakdown of 131 I to 131 Xe in iodine containing molecules and investigated the resulting molecular fragmentation process both in the gas phase and on the graphene-like surface. For each of the tasks, the intent was to learn about the thermodynamics and kinetics of the chemical transformations and use the calculations to provide parameters for input into kinetic models describing these processes for interpretation of experimental data in future work.
07 ISOTOPE AND RADIATION SOURCES↗
Embedded acoustic sensing and monitoring techniques for small modular reactors
The goal of this project was to study the applicability of specific innovative instrumentation techniques for assessing parameters needed for safe small modular reactor operation and safeguarding of nuclear material. Small modular reactor core designs are currently being developed to provide energy more effectively and efficiently than in the past because they can be built as modules at fabrication sites and then transported to a power-producing facility. However, these modules and/or the final core will often be sealed and not accessible again until disposal. Instead of instruments that access the core directly, during and after operation, to monitor flux/dose and structural integrity, as current power plants use, new sensors need to be designed that can be built into the reactor initially to determine operating history, structural integrity through operation of the system, and nuclear material accountancy after shutdown and before disposition of the core. Embedded sensors already exist that can provide neutron flux, gamma dose, and temperatures, but techniques to expand upon these for assessing structural health and material inventory in the system over time need to be developed. Structural health assessments include the detection and imaging of cracks in the components that could eventually cause radioactive fission products to be released.
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Design Report on the MiniFuel Instrumented Test Apparatus for Understanding Radiation Effects
Most nuclear fuels irradiations at Oak Ridge National Laboratory (ORNL) over the past decade have been conducted using MiniFuel—a static capsule design employing subscale fuel specimens to collect separate-effects irradiated fuel performance data. Irradiation conditions for MiniFuel experiments are predicted pre-test using reactor physics, and thermal models are verified post-irradiation via SiC dilatometry and various spectrometry methods. Relevant fuel performance parameters are also observed post-irradiation in a hot cell, thereby providing a single data point for each parameter representing the cumulative effects of the irradiation conditions. Substantially more data can be harvested from a single test and within a shorter duration by instrumenting irradiation vehicles and measuring desired quantities in situ. This report presents the design and analysis of the MiniFuel INstrumented Irradiation Test Apparatus for Understanding Radiation Effects (MINITAURE)—an instrumented test rig based on the separate-effects MiniFuel concept that aims to capture fission gas release (FGR) and thermal conductivity degradation of fuel specimens during irradiation in the High Flux Isotope Reactor (HFIR). MINITAURE will be integrated with the Materials Irradiation Facility (MIF) located in the HFIR building outside the reactor containment. The MIF will act as the instrumentation and control center for the experiment, enabling real-time feedback from in situ sensors and control of irradiation temperatures via a gas delivery system. Two unique capsule designs were developed to capture each phenomenon: the thermal conductivity capsule, which uses a thermopile method to estimate fuel specimen thermal conductivity, and the fission gas release capsule, which will have continuous flowing gas communication to high-purity germanium detectors that are housed in the MIF for monitoring FGR. This report details the reactor physics and heat transfer modeling activities that were used to inform the experiment design and predict capsule performance. It also describes out-of-pile activities conducted to stand up this new capability and verify the measurement techniques. Modeling efforts to date have demonstrated the feasibility of the in situ measurement techniques and supported the development of the MINITAURE assembly configuration. Out-of-pile testing of the thermal conductivity measurement shows promise in capturing relative changes in thermal conductivity. However, significant errors exist in the measured absolute value, posing a need for further refinement.
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Utilizing Advanced Statistics to Determine Anomalistic Conditions in Pebble-Bed Reactors
Pebble-bed reactors (PBRs) utilize hundreds of thousands of fuel pebbles, which continuously circulate through the core, in lieu of traditional fuel assemblies to generate fissions and produce power. The use of unmarked fuel pebbles presents a challenge for international safeguards verification that nuclear material is not being diverted. To ensure pebble diversion is not taking place, new methods for accounting for and monitoring the pebbles should be examined to determine an appropriate methodology for performing bulk accountancy with pebbles. Here, this work examines the use of statistical methods for determining if the reactor is within a declared range of operation by examining the statistical distribution of pebble burnup as they are discharged from the core. Using this methodology, we created a model that detects diversion over 95% of the time, over multiple diversion pathways, if the reactor core maintains a constant power density during the diversion process and only falsely labels a diversion case nominal 2% of the time. For a diversion scenario where the reactor is maintained at a constant power, the statistical analysis can correctly identify if diversion is occurring over 80% of the time; however, nearly 20% of specific diversion pathways are mislabeled nominal. These results provide a basis and framework for exploring the further use of statistical methods to determine where these methods could be most useful and where additional methods, such as machine learning, could be used to capture if diversion is occurring in pebble-bed reactors.
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Enabling Load Following Capability in the Transatomic Power MSR
This project is dedicated towards designing a fuel processing system that enables liquid-fueled molten salt reactors (MSR) to load follow by removing the dissolved xenon in the fuel salt. As one of the Gen-IV nuclear reactor concepts, the molten salt reactor receives increasing development interests in the recent years. One distinguishing feature of the liquid-fueled molten salt reactor is its improved ability to operate in a load-following mode by including the unique online fission product removal system. Load-following means that the reactor changes its power output based on the demand on the grid. Most of the current operating nuclear reactors have limited load-following ability and operate as the base load on the grid. Due to the rapid increase of solar energy, the requirement on load-following capacity is significantly increased because of the varying power output of the solar panels, yet the traditional load-following capacity is expected to decrease as the decarbonization of the grid continues. Therefore, the ability to perform load-following operation for the nuclear reactors will greatly enhance the resilience of the grid and make nuclear energy more economically competitive. This load-following feature is included in many commercial molten salt reactor designs, such as the designs by Transatomic Power, Terrestrial Energy, and Flibe Energy. Unfortunately, detailed analysis of the fuel processing system for commercial scale MSRs is still lacking, as well as how the fuel processing quantitively impacts the load-following operation. Moreover, experimental data for many of the underlying physics of fuel processing is limited. This project aims to pave the way for the fuel processing technology to advance to the commercial stage by performing combined experimental and simulation research. During the project period, four interconnected aspects of the development of the fuel processing system in liquid-fueled molten salt reactors are investigated. These aspects are the simulation and analysis of the fission product removal system, the fuel cycle simulation, the coupled reactor neutronics and thermal hydraulics transient simulation, and the gaseous fission product removal experiment. Multiphase CFD simulations are performed for components of the processing systems, and simplified air-water experiments are carried out to provide validation data. It is concluded that the CFD simulation can satisfactorily predict the system level performance of the components, and engineering models are constructed based on this success. Fuel cycle analysis is performed for two representative MSR design, the MSBR and the Transatomic Power MSR. Open-source code SaltProc is developed to incorporate the unique fuel processing system of the MSRs. It is concluded that the removal of xenon is essential for load-following operation in thermal spectrum MSR and Molten Salt Breeder Reactor. For the Transatomic Power MSR, the xenon poisoning effect is negligible due to its relatively fast neutron spectrum, though the overall fuel cycle economics still benefits from the removal of xenon. Coupled reactor neutronics and thermal hydraulics transient simulation is performed specifically for the Transatomic Power MSR. It is concluded that the reactor core design could perform power ramping fast enough to satisfy load-following operation. Combining the findings from each aspect, it is concluded that the load-following operation of a thermal neutron MSR is dependent upon the removal of xenon, which could be achieved for a commercial sized reactor using continuous inert gas sparging in a separate system with reasonable dimensions.
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
β — -delayed fission in the coupled quasiparticle random-phase approximation plus Hauser-Feshbach approach
Beta-delayed neutron emission and β-delayed fission (βdf) probabilities were calculated for heavy, neutronrich nuclei using the Los Alamos coupled quasiparticle random-phase approximation plus Hauser-Feshbach (QRPA + HF) approach. In this model, the compound nucleus is initially populated by β decay and is followed through subsequent statistical decays taking into account competition among neutrons, γ rays, and fission. The primary output of these calculations includes branching ratios along with neutron and γ -ray spectra. Here, we find a relatively large region of heavy nuclides where the probability of βdf is near 100%. For a subset of nuclei near the neutron drip line, delayed neutron emission and the probability of fission are both large, which leads to the possibility of multichance βdf (mc-βdf). We comment on prospective neutron-rich nuclei that could be probed by future experimental campaigns and provide a full table of branching ratios in ASCII format in the Supplemental Material for use in various applications.
73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
Analysis of SCALE Criticality and Sensitivity Calculations for Reflected HEU Cylinders
The SCALE code package offers multiple nuclear data libraries and sensitivity and uncertainty (S/U) methods supporting and derived from Monte Carlo (MC) transport. The CSAS and TSUNAMI-3D sequences use KENO MC, utilizing either continuous-energy (CE) cross sections or multigroup (MG) cross section libraries. TSUNAMI-3D has two CE calculational methods: the iterated fission probability (IFP) method, and the Contribution-Linked eigenvalue sensitivity/Uncertainty estimation via Tracklength importance CHaracterization (CLUTCH) method. Previous work has shown poor agreement between CLUTCH and confirmatory direct perturbation calculations in specific applications (e.g., fissionable and polyethylene reflectors). The HEU-MET-FAST-084 (HMF-084) International Criticality Safety Benchmark Evaluation Project evaluation consists of 27 cylindrical highly enriched uranium metal cores with 14 unique reflector materials of 0.5 and 1 in. thicknesses. Included in this list of reflector materials are natural uranium and polyethylene. This work utilized SCALE 6.2.4 models of the HMF-084 evaluation, with additional non-physical configurations to test both the MG bias and CLUTCH functionality across a variety of reflector material thicknesses. The evaluation’s use of concentric cylinders allowed for examination of several MG self-shielding methods: infinite homogenous, cylindrical, and spherical. The results indicate that the use of polyethylene reflectors with CLUTCH is not fundamentally impossible but sensitive to geometry. The poor performance of CLUTCH with fissionable reflectors was reaffirmed. The 2 in. and greater polyethylene-reflected calculations demonstrate the necessity of using the 302-group library for fast systems. The nickel MG bias was substantial, as discussed in a companion paper, as were cobalt and iron.
73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
Interplay between Mixed and Pure Exciton States Controls Singlet Fission in Rubrene Single Crystals
Singlet fission (SF) is a multielectron process in which one singlet exciton S converts into a pair of separated triplet excitons T. SF is widely studied as it may help overcome the Shockley−Queisser efficiency limit for semiconductor photovoltaic cells. To elucidate and control the SF mechanism, great attention has been given to the identification of intermediate states in SF materials, which often appear elusive due to the complexity and fast time scales of the SF process. Here, we apply 14 fs-1 ms transient absorption techniques to high-purity rubrene single crystals to disentangle the intrinsic fission dynamics from the effects of defects and grain boundaries and to identify reliably the fission intermediates. Our data demonstrates that above-gap excitation directly generates a hybrid vibronically assisted mixture of singlet state and triplet-pair multiexciton [S/TT], which rapidly (<100 fs) and coherently branches into pure singlet or triplet excitations. The relaxation of [S/TT] to S is followed by a relatively slow and temperature-activated (48 meV activation energy) incoherent fission process. The SF competing pathways and intermediates revealed here unify the observations and models presented in previous studies of SF in rubrene and offer alternative strategies for the development of SF-enhanced photovoltaic materials.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Standardizing a Renewed Fission Product Yield Library and Related Covariances (Part II)
A complete library of independent fission product yields including covariance information was generated by a sequential Bayesian methodology whose prior information consisted of independent fission product yields and branching ratios of the possible decay modes reported in the recently released ENDF/B-VIII.0 nuclear data library. The Bayesian procedure consisted in the adjustment of independent fission product yields to match the set of stable and long-lived cumulative yields reported in the ENDF/B-VIII.0 nuclear data library which, in this work, were considered as legacy values together with their uncertainties. According to the χ 2 -metric, the results obtained by this methodology show a systematic improvement in the agreement with legacy reported cumulative yields for the entire adjusted independent fission product yield library.
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
Understanding TRISO Coated Particle Neutron Irradiation Behavior:Evolution of Advanced Micro Analysis and Electron Microscopy Approaches
Objectives and motivation• Provide data for fuel qualification in support of reactor licensing• Establish a domestic commercial TRISO fuel fabrication capability Approach • Focus is on developing and testing UCO TRISO fuel –Develop fuel fabrication and QC measurement methods, first at lab scale and then at industrial scale –Perform irradiation testingover a range of conditions (burnup, temperature, fast neutron fluence) –Perform post-irradiation examination and safety testingto demonstrate and understand performance during irradiation and during accident conditions –Develop fuel performance modelsto better predict fuel behavior –Perform fission product transport experiments to improve understanding and refine models of fission product transport
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AGR-2 Compact 6-4-1 Post-Irradiation Examination Results
The Advanced Gas Reactor (AGR) Fuel Development and Qualification Program was established to perform research and development on tristructural isotropic (TRISO)-coated particle fuel to support deployment of a high-temperature gas-cooled reactor (HTGR). The work continues as part of the Advanced Reactor Technologies (ART) TRISO Fuel Program. The overarching goal of the program is to provide a baseline fuel qualification data set to support licensing and operation of an HTGR. To achieve these goals, the program includes the elements of fuel fabrication, irradiation, post-irradiation examination (PIE) and safety/heating testing, fuel performance modeling, and fission product transport (INL 2017). Several fuel irradiation experiments have been performed at the Advanced Test Reactor (ATR) at Idaho National Laboratory (INL), and additional irradiations are planned. These experiments are intended to provide data on fuel performance under irradiation, support fuel fabrication process development, qualify fuel for operating and accident conditions, provide irradiated fuel for accident testing, and support development of fuel performance and fission product transport models.
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Fusion Materials Semiannual Progress Report for the Period Ending June 30, 2025
This is the seventy-eighth in a series of semiannual technical progress reports on fusion materials science activity supported by the Fusion Energy Sciences Program of the U.S. Department of Energy. It covers the period ending June 30 th , 2025. This report focuses on research addressing the effects on materials properties and performance of exposure to the neutronic, thermal and chemical environments anticipated in the chambers of fusion experiments and energy systems. This research is a major element of the national effort to establish the materials knowledge base for an economically and environmentally attractive fusion energy source. Research activities on issues related to the interaction of materials with plasmas are reported separately. The results reported are the products of a national effort involving a number of national laboratories and universities. A large fraction of this work, particularly in relation to fission reactor irradiations, is carried out collaboratively with international partners, e.g., Japan and the UK. The purpose of this series of reports is to provide a working technical record for the use of program participants, and to provide a means of communicating the efforts of fusion materials scientists to the broader fusion community, both nationally and worldwide. This report has been compiled by Stephanie Melton, Oak Ridge National Laboratory. Her efforts, and the efforts of the many persons who made technical contributions, are gratefully acknowledged.
70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗