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DOE OSTI2025

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.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2020

Fission Product Gas Monitoring During Fuel Drying Operations - 20094

The goal of the project was to devise and implement a method of accurately qualifying any noble gas emitted during fuel drying operations (part of the dry fuel storage process) in order to provide the data needed to validate the off-site dose calculations. The imputes of the project was the NRC publishing Information Notice 18-01, 'Noble Fission Gas Releases During Spent Fuel Cask Loading Operations' in February 2018. The information notice describes some industry events that occurred during vacuum drying operations as part of a dry fuel campaign. The solution was devised by Fort Calhoun Station staff in partnership with Mirion Technologies technical staff. The monitoring was accomplished by directing all the effluent from the fuel storage cask vacuum drying machine through a sample chamber containing a compact ISOCS characterized CZT based gamma spectrometer connected to a Mirion Data Analyst. This resulted near real-time quantification of the radionuclides of concern. (authors)

07 ISOTOPE AND RADIATION SOURCES↗

DOE OSTI2020

Advances in Resin Management Using 3R-Scan - 20154

The most important factor underlying optimal waste management is developing a clear picture of the radioactivity content of the waste and its impact on waste disposal cost. For over 35 years since the publishing of 10CFR61, waste characterization has relied on sampling the final waste product after formation. In the days following 10CFR61, the cost of final disposal was marginal with only a small impact on the overall costs. Constraints were added by provisions of the Low Level Waste Policy Act of 1985 leading to increasingly limited access to those disposal sites that remained available. In addition, Nuclear Regulatory Commission (NRC) pressure promoting waste volume reduction led to disposal costs inevitably rising. Despite this, characterization practices in monitoring of waste generation for activity content still center on the same dated processes. This results in a disposal classification on the basis of endpoint sampling without consideration of the homogeneity of the waste mixture. It can also disregard consideration of the representativeness of the single or small sample base. As a minimum effort, a formalized sampling program of a fixed grouping of waste streams can be implemented that could account for more than 95% of all of the activity carried in solid waste products. The sample results for each radionuclide could then be trended as time passes to develop reasonable scaling factors for difficult to measure radionuclides. This process, identified in NRC guidance, has been rigorously followed by a relatively small number of facilities. The trended scaling factors serve to improve accuracy by identifying anomalous results that could otherwise go undetected. Direct monitoring of the accumulation of activity in process streams generating solid radwaste, including demineralizers and filter streams, is a more precise approach. Nearly all of these streams are monitored by plant chemistry on a regular schedule to maintain water quality. This paper discusses viable options for developing the basis for characterization through process monitoring of the accumulation of activity at the point of generation. Special focus is on resin bed tracking and how process knowledge of these streams can be brought together to form a consistent and precise solid waste radioactivity inventory. Some of the specific points covered in this paper include the merger of the fission product release computer program, 3R-STAT, with the radwaste sample analysis computer program, SCAN4 to create 3R-SCAN, the importance of individual waste stream influences on the overall source term, and the use of historic sample data to develop scaling factors using an automated process. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI1992

Nuclear Safety [Vol. 33, No. 1, January-March 1992]

Nuclear Safety is a review journal that covers significant developments in the field of nuclear safety. Its scope includes the analysis and control of hazards associated with nuclear energy, operations involving fissionable materials, and the products of nuclear fission and their effects on the environment. Primary emphasis is on safety in reactor design, construction, and operation; however, the safety aspects of the entire fuel cycle, including fuel fabrication, spent-fuel processing, nuclear waste disposal, handling of radioisotopes, and environmental effects of these operations, are also treated. Table of Contents for this issue follows. GENERAL SAFETY CONSIDERATIONS: 1 Technical Note: A New Approach to Fission Reactor Safety, Yu. V. Petrov; 5 Erratum; ACCIDENT ANALYSIS: 6 Analysis and Modeling of Fission Product Release from Various Uranium-Aluminum Plate-Type Reactor Fuels, R. P. Taleyarkhan; CONTROL AND INSTRUMENTATION: 23 Applications of a Surveillance and Diagnostics Methodology Using Neutron Noise From a Pressurized-Water Reactor, R. T. Wood, L. F. Miller, and R. B. Perez; DESIGN FEATURES: 36 Westinghouse Advanced Passive 600 Plant, B. A. McIntyre and R. K. Beck; 47 System 80+™ PWR Safety Design, C. W. Bagnal, R. A. Matzie, and R. S. Turk; ENVIRONMENTAL EFFECTS: 58 The MATS Experiments—Mesoscale Atmospheric Transport Studies at the Savannah River Site, A. H. Weber, S. Berman, R. J. Kurzeja, and R. P. Addis; 75 Book Review: Environmental Radioactivity in the European Community 1984-1985-1986, C. A. Little; WASTE AND SPENT FUEL MANAGEMENT: 76 Activities Related to Waste and Spent Fuel Management, M. D. Muhlheim and E. G. Silver; OPERATING EXPERIENCES: 87 Aging Assessment of BWR Control Rod Drive Systems, R. H. Greene; 100 Reactor Shutdown Experience, Compiled by J. W. Cletcher; 103 Selected Safety-Related Events, Compiled by G. A. Murphy; 110 Operating U.S. Power Reactors, Compiled by M. D. Muhlheim and E. G. Silver; RECENT DEVELOPMENTS: 129 General Administrative Activities, Compiled by M. D. Muhlheim and E. G. Silver; 139 Reports, Standards, and Safety Guides, D. S. Queener; 143 Proposed Rule Changes as of Sept. 30 1991; ANNOUNCEMENTS: 128 Harvard School of Public Health Announces Short Courses; 128 16th Biennial ANS Topical Meeting on Reactor Operating Experience: Present and Future Technologies—Applying Lessons Learned (Call for Papers); 147 The Authors; 150 Indexes to Nuclear Safety, Volume 32; 154 Errata.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2025

Development of an In Situ Fission Gas Release Instrument for Fuel Sample Irradiations in the High Flux Isotope Reactor

Experimental measurement of gaseous fission product release with respect to temperature and burnup is a critical aspect of understanding nuclear fuel performance, validating predictive models, and qualifying new fuels. To measure this phenomenon in real-time, Oak Ridge National Laboratory has developed an instrument for measuring in situ fission gas release from small-scale fuel samples irradiated in the High Flux Isotope Reactor (HFIR). The instrument uses a continuous flow of Heover the fuel samples to sweep gaseous fission products from a sealed capsule in the HFIR Be reflector to an instrument station adjacent to the reactor. The instrument station houses two high-purity germanium (HPGe) detectors that measure decay gamma rays from fission products passing through a room temperature dwell chamber placed over the detector crystal. The sealed capsules in the reactor are designed to modulate fuel sample temperatures between 700 and 1,100°C by changing the Ar/He gas mixture surrounding the capsules during irradiation. N-type thermocouples are incorporated into the capsule housing to record real-time fuel temperatures. The capsules are heated primarily by prompt gamma rays emitted from the HFIR core with minimal heat contributions from fission in the fuel samples to minimize temperature gradients in the specimens for separate-effects characterization of the material. This paper describes modeling of time-dependent nuclear heating and fission product formation in fuel samples, thermal characteristics of the in-core capsules, and expected gaseous fission product gamma spectra at the HPGe instrument station.

Mulligan, Padhraic L [ORNL] (ORCID:000000025826540↗

DOE OSTI2020

An Overview of Neutron Irradiated SiC Layer Behavior using Micro-and Nano-Characterization Techniques

The complexity of fission product distribution and composition within the SiC layer of tristructural isotropic (TRISO) coated particles, irradiation effects on the SiC structure as well as the variable nature of metallic fission product release, has led to the exploration of multiple micro- and nano-characterization techniques. The fine scale of the fission product precipitates necessitates unique learnings and application of electron microscopic techniques with irradiated fuel during the Advanced Gas Reactor (AGR)-1 experiment analysis. A summarized discussion on the specific advanced techniques with associated method development for TRISO coated particles is provided followed by the down selected techniques currently considered to provide the highest impact. Techniques considered are electron probe micro-analyzer (EPMA), scanning transmission electron microscopy (STEM), and Precession electron diffraction (PED). SiC grain boundary characteristics are evaluated due to the mobility of specific fission products through grain boundaries. PED was performed for understanding the role of grain boundary character on fission product transport. One set of comparative analyses between AGR-1 and AGR-2 particles leads to a finding that the AGR-1, high-Ag-retention particle, had statistically more coincidence site lattice (CSL)-related grain boundaries (but fewer low-angle grain boundaries), compared to the AGR-2 particle. This implies that CSL-related grain boundaries may have a direct influence on Ag retention. However, precipitates were found on a relatively small fraction of CSL-related grain boundaries in both particles. In another set of comparison between AGR-1 and AGR-2 particles that were subjected to safety testing, there is significant differences in average SiC grain boundary distributions, but the fission product distributions on these grain boundaries are very similar.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2021

Micro- and Nano-techniques for the Study of Fission Product Precipitation in SiC Layer

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2020

Simplified Approach for Scoping Assessment of Non-LWR Source Terms

This report describes a structure to aid in evaluation of release mitigation strategies across a range of reactor technologies. The assessment performed for example reactor concepts utilizes previous studies of postulated accident sequences for each reactor concept. This simplified approach classifies release mitigation strategies based on a range of barriers, physical attenuation processes, and system performance. It is not, however, intended to develop quantitative estimates of radiological release magnitudes and compositions to the environment. Rather, this approach is intended to identify the characteristics of a reactor design concepts release mitigation strategies that are most important to different classes of accident scenarios. It uses a scoping methodology to provide an approximate, order-of-magnitude, estimate of the radiological release to the environment and associated off-site consequences. This scoping method is applied to different reactor concepts, considering the performance of barriers to fission product release for these concepts under sample accident scenarios. The accident scenarios and sensitivity evaluations are selected in this report to evaluate the role of different fission product barriers in ameliorating the source term to the environment and associated off-site consequences. This report applies this structure to characterize how release mitigation measures are integrated to define overall release mitigation strategies for High Temperature Gas Reactors (HTGRs), Sodium Fast Reactors (SFRs), and liquid fueled Molten Salt Reactors (MSRs). To support this evaluation framework, factors defining a chain of release attenuation stages, and thus an overall mitigation strategy, must be established through mechanistic source term calculations. This has typically required the application of an integral plant analysis code such as MELCOR. At present, there is insufficient evidence to support a priori evaluation of the effectiveness of a release mitigation strategy for advanced reactor concepts across the spectrum of events that could challenge the radiological containment function. While it is clear that these designs have significant margin to radiological release to the environment for the scenarios comprising the design basis, detailed studies have not yet been performed to assess the risk profile for these plants. Such studies would require extensive evaluation across a reasonably complete spectrum of accident scenarios that could lead to radiological release to the environment.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

DOE OSTI2023

Determination of Average Burnup in AGR-3/4 Compacts 1-4 and 7-4

The Advanced Gas Reactor (AGR) Fuel Development and Qualification Program third and fourth irradiation experiments (AGR-3/4), originally planned as separate tests, were combined in one test train for irradiation in the Advanced Test Reactor (ATR) at Idaho National Laboratory (INL). The irradiation test began on December 14, 2011, and ended on April 12, 2014 (Collin 2016). The originally planned AGR-3 and AGR-4 irradiation experiments were both focused on obtaining data on fission product transport to support the improvement of modeling. The AGR-3 experimental plan was focused on gaseous and metallic fission product release from the kernels and diffusion in the coatings during irradiation and post-irradiation safety testing. The AGR-4 experimental plan was focused on diffusivities and sorptivities in the compact matrix and reactor graphite. These two goals were combined in the AGR-3/4 irradiation, which consisted of 12 independently monitored capsules that each contained four AGR-3/4 compacts in a single stack surrounded by an inner ring of matrix or graphite and an outer ring of graphite. Two capsule types were used: a standard capsule and a so-called fuel body, in which the outer graphite ring included a floor and cap that fully enclosed the fuel. The fuel body design supported post-irradiation safety testing of the intact fuel and ring assembly to provide data on fission product transport and release from the matrix and graphite at accident temperatures.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2020

Radial Deconsolidation and Leach-Burn-Leach of AGR-3/4 Compact 1-4 and 10-4

The Advanced Gas Reactor (AGR) Fuel Development and Qualification Program third and fourth irradiation experiments (AGR-3/4), originally planned as separate tests, were combined in one test train for irradiation in the Advanced Test Reactor at Idaho National Laboratory (INL). The irradiation test began on December 14, 2011 and ended on April 12, 2014 (Collin 2016). The originally planned AGR-3 and AGR-4 irradiation experiments were both focused on obtaining data on fission product transport to support the improvement of modeling. The AGR-3 experimental plan was focused on gaseous and metallic fission product release from the kernels and diffusion in the coatings during irradiation and postirradiation safety testing. The AGR-4 experimental plan was focused on diffusivities and sorptivities in the compact matrix and reactor graphite (Petti et al. 2005). These two goals were combined in the AGR-3/4 irradiation, which consisted of twelve independently monitored capsules that each contained four AGR-3/4 compacts in a single stack surrounded by an inner ring of matrix or graphite and an outer ring of graphite. There were two capsule types: a standard capsule and a “fuel body”, in which the outer graphite ring included a floor and cap that fully enclosed the fuel (Stempien et al. 2018a). The fuel body design supported post-irradiation safety testing of the intact fuel and ring assembly to provide data on fission product transport and release from matrix and graphite at accident temperatures (Demkowicz 2017).

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2021

Radial Deconsolidation and Leach-Burn-Leach of AGR-3/4 Compacts 8-4 and 7-4

The Advanced Gas Reactor (AGR) Fuel Development and Qualification Program’s third and fourth irradiation experiments (AGR-3/4), originally planned as separate tests, were combined into one test train for irradiation in the Advanced Test Reactor at Idaho National Laboratory (INL). The irradiation test began on December 14, 2011, and ended on April 12, 2014 (Collin 2016). The originally planned AGR-3 and AGR-4 irradiation experiments were both to be focused on obtaining fission product transport data to support improvements in modeling. The AGR-3 experimental plan was focused on gaseous and metallic fission product release from the kernels and diffusion in the coatings during irradiation and postirradiation safety testing. The AGR-4 experimental plan was focused on diffusivities and sorptivities in the compact matrix and reactor graphite (Petti et al. 2005). These goals were combined in the AGR-3/4 irradiation experiment, which consisted of twelve independently monitored capsules that each contained four AGR-3/4 compacts in a single stack surrounded by an inner ring of matrix or graphite and an outer ring of graphite. There were two capsule types: a standard capsule and a fuel body, in which the outer graphite ring included a floor and cap to fully enclose the fuel (Stempien et al. 2018a). The fuel body design supported post-irradiation safety testing of the intact fuel and ring assembly to obtain data on fission product transport and release from matrix and graphite at accident temperatures (Demkowicz 2017).

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

DOE OSTI2022

Radial Deconsolidation and Leach-Burn-Leach of AGR-3/4 Compacts 1-3, 4-3, 10-1, and 10-2

The Advanced Gas Reactor (AGR) Fuel Development and Qualification Program’s third and fourth irradiation experiments (AGR-3/4), originally planned as separate tests, were combined into one test train for irradiation in the Advanced Test Reactor at Idaho National Laboratory (INL). The irradiation test began on December 14, 2011 and ended on April 12, 2014 (Collin 2016). The originally planned AGR-3 and AGR-4 irradiation experiments were both focused on obtaining data on fission product transport to support modeling improvement. The AGR-3 experimental plan was focused on gaseous and metallic fission product release from the kernels and diffusion in the coatings during irradiation and post-irradiation safety testing. The AGR-4 experimental plan was focused on diffusivities and sorptivities in the compact matrix and reactor graphite (Petti et al. 2005). These two goals were combined in the AGR-3/4 irradiation, which consisted of twelve independently monitored capsules that each contained four AGR-3/4 compacts in a single stack surrounded by an inner ring of matrix or graphite and an outer ring of graphite. There were two capsule types: a standard capsule and a fuel body in which the outer graphite ring included a floor and cap that fully enclosed the fuel (Stempien et al. 2018a). The fuel body design supported post-irradiation safety testing of the intact fuel and ring assembly to provide data on fission product transport and release from matrix and graphite at accident temperatures (Demkowicz 2017)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2024

Investigation of Frozen Chemistry for Molten Salt Reactors (MSRs)

Understanding accident progression and the potential/conditions for fission product release from fuel is necessary to evaluate safety for any nuclear reactor system. Molten Salt Reactors (MSRs) under development need such analysis to support safety evaluations. Fission product chemistry specific to MSR concepts is a critical area that introduces distinct considerations relative to the current state-of-knowledge in reactor safety, primarily developed for water-moderated nuclear reactor systems. In Light Water Reactor (LWR) systems, it is necessary to capture the chemical interaction of fission products with the reactor evironment, containment and confinement systems. The overall effects at this point are relatively well understood for the purposes of performing safety evaluations. A key insight from LWR studies is that fission product chemical behavior can be reasonably captured by modeling approaches where the chemistry is "frozen". These modeling approaches assume that radionuclide reaction and speciation can be represented by chemical classes, each with characteristic transport behavior that is invariant under a broad range of thermochemical conditions. However, radionuclides can exhibit a range of behavior in the liquid salt-melt phase of the coolant used in MSRs. Radionuclides, salt, and the metal containment surfaces (i.e. pipes) can co-exist in dynamic equilibrium that could evolve with small system mass changes. A detailed investigation to the degree the equilibrium state can dynamically evolve with changes in the conditions of the molten salt mixture has not been previously conducted. It is currently not well understood where frozen chemistry assumptions are valid. Expanding the state-of-knowledge in this regard is relevant to better assessing the range of chemical effects that should be incorporated as part of MSR safety assessments. This investigation used the Oak Ridge Isotope GENeration (ORIGEN) module of the Standardized Computer-Analysis for Licensing Evaluation (SCALE) code to generate simulated radionuclide inventories for the MSR Experiment (MSRE) and then modeled reactor chemical speciation using the Molten Salt Thermodynamic Database – Thermochemical (MSTDB-TC) coupled with Thermochimica. The effect of composition variation during decay of fission product inventory in a molten salt over a period of 500 days prolonged post- at multiple temperatures was studied. Mass fractions for fluorine and berilium were varied in order to probe the effects of free fluorine control. Finally, speciation of fluoride reactors were showed by comparing MSRE readionuclide inventories with a FLiBe based molten salt breeder reactor (MSBR). The results showed that fission product mass change has little effect on phase mass changes and vapor pressures for fluoride species, but differ with varying carrier and fuel salt compositions. However, iodine species were found to have a vapor pressure not only dependent on temperature, but also the free fluorine potential, releasing iodine when the free fluorine potential is equal to the iodine inventory. This observation, however, arose under free fluorine potentials that are very unlikely to be realized in typical molten salt mixtures. Despite this observation, temperature was found to be the dominant parameter that drove phase change and fission product species vapor pressure. The results indicate that the current frozen chemistry approach is adequate for MSR analysis.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

DOE OSTI2022

Westinghouse Accident Tolerant Fuel Phase 2B with Higher Enriched and Higher Burnup Add-On Project Final Technical Report Deliverable Volume 1

The Westinghouse Electric Company LLC (Westinghouse) accident tolerant fuel (ATF) program funded by Westinghouse and the US Department of Energy (DOE) utilized chromium (Cr) coated zirconium alloy cladding with doped UO 2 (ADOPT(TM)) and uranium silicide (U 3 Si 2 ) high density/high thermal conductivity fuel for its lead test rod (LTR) program with irradiation beginning in 2019. ADOPT is a Cr 2 O 3 +Al 2 O 3 doped UO 2 pellet with increased oxidation resistance and density, and increased resistance to fission gas release. Due to the issues with U 3 Si 2 fuel reaction in pressurized water reactor (PWR) environments, uranium nitride (U 15 N) has been substituted for U 3 Si 2 as a long-term fuel option. Cr coated cladding with ADOPT fuel is the near-term Westinghouse EnCore fuel product. The long-term EnCore ® fuel product is SiGA ® SiC/SiC composite cladding with high density/high thermal conductivity UN fuel. In 2020, the higher burnup and higher enriched and (HBHE) program was integrated into the ATF program. The objective of this expanded program is to extend ATF burnups to at least 75 MWd/kgU to economically facilitate 24-month cycles in PWRs. The ATF program now includes ADOPT fuel with enrichments >5% 235 U. Over the past several years, Westinghouse has tested the Cr coated zirconium (Zr) and silicon carbide (SiC) claddings in Westinghouse Churchill autoclaves and the Massachusetts Institute of Technology (MIT) reactor. Additionally, the Cr coated cladding has been tested in the Advanced Test Reactor (ATR) at Idaho National Laboratory (INL) and in LTR programs at the Doel 4 and Bryon 2 commercial reactors. High temperature tests at the state-of-the-art Westinghouse facilities in Churchill, PA and at Karlsruhe Institute of Technology (KIT) have been carried out to determine the time and temperature limits for the Cr coated zirconium claddings. These tests indicate that Cr coated Zr cladding can take temperatures up to about 1500°C for short periods of time without becoming totally oxidized. The main issue is the formation of the Cr-Zr eutectic at 1333°C resulting in the migration of this eutectic inward with the formation of ZrCr 2 which rapidly oxidizes to ZrO 2 on the outside of the tube. The Cr coated Zr cladding also delays the bursting of the tube, reduces the burst area, and reduces hydriding and embrittlement of the Zr which is a major benefit for reducing fuel fragmentation, redistribution, and dispersal (FFRD), the major licensing issue faced by HBHE. The manufacturing parameters for the SiC have been found to have a significant effect on the corrosion rate of the SiC in light water reactor (LWR) conditions and significant improvements have been made in the yield, quality, and oxidation resistance of the SiC cladding by identifying and tightening manufacturing process parameters. Current autoclave results for SiC composite claddings indicate that a corrosion rate of fewer than 2 micrometers per year can be achieved which meets corrosion requirements under normal operating conditions. High temperature steam oxidation tests at the state-of-the-art Westinghouse facilities in Churchill, PA and at Karlsruhe Institute of Technology (KIT) have been carried and determined that SiC cladding can withstand temperatures up to about 1800°C to 1900°C before excessive corrosion reactions begin, and that the SiC will not balloon and burst. ADOPT fuel pellets were incorporated into the Westinghouse ATF program because of their increased density and oxidation resistance. A topical report supporting the use of ADOPT pellets has been submitted to the NRC and will be approved shortly. ADOPT pellets have been a product in Europe for over 15 years. The additives work to make larger grain sizes which appear to reduce fission gas release during transients as well as increase the density of the pellet. Fuel rod and assembly design in preparation for the lead test rod (LTR) and lead test assembly (LTA) programs is underway as well as licensing efforts with the Nuclear Regulatory Commission (NRC). Finally, accident analyses coupled with economic evaluations for both operating savings as well as fuel savings have been initiated. Modular Accident Analysis Program 5 (MAAP5) calculations indicate that both Cr coated cladding and SiC composite cladding can increase the time to fuel rod loss of geometry for up to two hours longer than current Zr based cladding in a station blackout scenario. This additional time is due to the much higher oxidation resistance of the SiC and Cr coated cladding. These two hours can be used to implement additional response options instituted through the Diverse and Flexible Mitigation Capability (FLEX) program by reactor operators. Both ATF cladding options also reduce hydrogen production which dramatically reduces primary system and containment pressure and the risk of fission product release beyond containment in the unlikely event of an accident. The lower pressure in the system allows more time to feed cooling water to the core, resulting in the avoidance of fuel melting. The coping time is extended indefinitely if the modest water flow provided by FLEX continues. Experimental work on methods to rapidly fabricate SiC composite structures with high density and reduce the fabrication price of SiC fibers while maintaining a high level of performance is needed. Methods for mitigating or stopping the Cr-Zr eutectic are also needed to further improve the oxidation resistance of Cr coated Zr. Minimal (<1%) swelling of U 3 Si 2 and subsequent fission gas release has been demonstrated up to 20 MWd/kgU. Irradiation experiments with U 3 Si 2 fuel in ATR to determine these properties at 40 MWd/kgU were completed but post irradiation examinations were not done since U 3 Si 2 has been replaced by UN. UN has three issues that are being addressed. The first is increasing the oxidation resistance so that there is not excessive reaction up to ~1500°C. While UN increases the pellet density and additives to the UN postponed the temperature at which rapid oxidation occurred by ~100°C to 200°C, this is not enough, and pellet coating options are now being pursued. The second is developing a method to manufacture that does not require the multi-step process of UF 6 to UO 2 to UC to UN. Efforts are underway looking at UF 6 to UN 2 to UN and UF 6 to UF 4 to UN 2 to UN reactions. Finally, an economically acceptable process for potentially enriching the 15 N content of the nitrogen used to make UN to >95% 15N was identified though not experimentally validated. In addition to the work supported by the DOE, research and testing activities are being carried on in a world-wide effort funded by many countries such as Sweden, United Kingdom, Belgium, Netherlands, Spain, Germany, Japan, and France. This work is being facilitated through the Westinghouse led Collaboration for Advanced Research on Accident Tolerant Fuel (CARAT) program. Annual meetings were organized in 2018 and 2019 by Westinghouse as a venue for presentation of this work and to provide for the cross-fertilization of ideas among the many outstanding researchers in the ATF area. No meetings were held in 2020 and 2021 due to the COVID-19 related restrictions on traveling and gatherings. Since SiC, coated cladding, and high-density fuel options are not currently used in the nuclear industry; support from the government and industry members is needed to further the significant effort of setting new standards. The same is true for the Nuclear Regulatory Commission (NRC) which must review and approve the commercial use of these new fuels since all current regulations are oriented toward Zr/UO 2 fuel. Several meetings have been held with the NRC to generate a fast-track approach to licensing ATF using a combination of atomic modeling, in-rod sensors, and in-reactor testing. This approach was memorialized in an “Accelerated Fuel Qualification White Paper” prepared by the Accelerated Fuel Qualification Working Group lead by General Atomics.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2022

Westinghouse Accident Tolerant Fuel Phase 2B with Higher Enriched and Higher Burnup Add-On Project Final Technical Report Deliverable Volume 2

The Westinghouse Electric Company LLC (Westinghouse) accident tolerant fuel (ATF) program funded by Westinghouse and the US Department of Energy (DOE) utilized chromium (Cr) coated zirconium alloy cladding with doped UO 2 (ADOPT(TM)) and uranium silicide (U 3 Si 2 ) high density/high thermal conductivity fuel for its lead test rod (LTR) program with irradiation beginning in 2019. ADOPT is a Cr 2 O 3 +Al 2 O 3 doped UO 2 pellet with increased oxidation resistance and density, and increased resistance to fission gas release. Due to the issues with U 3 Si 2 fuel reaction in pressurized water reactor (PWR) environments, uranium nitride (U 15 N) has been substituted for U 3 Si 2 as a long-term fuel option. Cr coated cladding with ADOPT fuel is the near-term Westinghouse EnCore ® fuel product. The long-term EnCore fuel product is SiGA ® SiC/SiC composite cladding with high density/high thermal conductivity UN fuel. In 2020, the higher burnup and higher enriched and (HBHE) program was integrated into the ATF program. The objective of this expanded program is to extend ATF burnups to at least 75 MWd/kgU to economically facilitate 24-month cycles in PWRs. The ATF program now includes ADOPT fuel with enrichments >5% 235 U. Over the past several years, Westinghouse has tested the Cr coated zirconium (Zr) and silicon carbide (SiC) claddings in Westinghouse Churchill autoclaves and the Massachusetts Institute of Technology (MIT) reactor. Additionally, the Cr coated cladding has been tested in the Advanced Test Reactor (ATR) at Idaho National Laboratory (INL) and in LTR programs at the Doel 4 and Bryon 2 commercial reactors. High temperature tests at the state-of-the-art Westinghouse facilities in Churchill, PA and at Karlsruhe Institute of Technology (KIT) have been carried out to determine the time and temperature limits for the Cr coated zirconium claddings. These tests indicate that Cr coated Zr cladding can take temperatures up to about 1500°C for short periods of time without becoming totally oxidized. The main issue is the formation of the Cr-Zr eutectic at 1333°C resulting in the migration of this eutectic inward with the formation of ZrCr 2 which rapidly oxidizes to ZrO 2 on the outside of the tube. The Cr coated Zr cladding also delays the bursting of the tube, reduces the burst area, and reduces hydriding and embrittlement of the Zr which is a major benefit for reducing fuel fragmentation, redistribution, and dispersal (FFRD), the major licensing issue faced by HBHE. The manufacturing parameters for the SiC have been found to have a significant effect on the corrosion rate of the SiC in light water reactor (LWR) conditions and significant improvements have been made in the yield, quality, and oxidation resistance of the SiC cladding by identifying and tightening manufacturing process parameters. Current autoclave results for SiC composite claddings indicate that a corrosion rate of fewer than 2 micrometers per year can be achieved which meets corrosion requirements under normal operating conditions. High temperature steam oxidation tests at the state-of-the-art Westinghouse facilities in Churchill, PA and at Karlsruhe Institute of Technology (KIT) have been carried and determined that SiC cladding can withstand temperatures up to about 1800°C to 1900°C before excessive corrosion reactions begin, and that the SiC will not balloon and burst. ADOPT fuel pellets were incorporated into the Westinghouse ATF program because of their increased density and oxidation resistance. A topical report supporting the use of ADOPT pellets has been submitted to the NRC and will be approved shortly. ADOPT pellets have been a product in Europe for over 15 years. The additives work to make larger grain sizes which appear to reduce fission gas release during transients as well as increase the density of the pellet. Fuel rod and assembly design in preparation for the lead test rod (LTR) and lead test assembly (LTA) programs is underway as well as licensing efforts with the Nuclear Regulatory Commission (NRC). Finally, accident analyses coupled with economic evaluations for both operating savings as well as fuel savings have been initiated. Modular Accident Analysis Program 5 (MAAP5) calculations indicate that both Cr coated cladding and SiC composite cladding can increase the time to fuel rod loss of geometry for up to two hours longer than current Zr based cladding in a station blackout scenario. This additional time is due to the much higher oxidation resistance of the SiC and Cr coated cladding. These two hours can be used to implement additional response options instituted through the Diverse and Flexible Mitigation Capability (FLEX) program by reactor operators. Both ATF cladding options also reduce hydrogen production which dramatically reduces primary system and containment pressure and the risk of fission product release beyond containment in the unlikely event of an accident. The lower pressure in the system allows more time to feed cooling water to the core, resulting in the avoidance of fuel melting. The coping time is extended indefinitely if the modest water flow provided by FLEX continues. Experimental work on methods to rapidly fabricate SiC composite structures with high density and reduce the fabrication price of SiC fibers while maintaining a high level of performance is needed. Methods for mitigating or stopping the Cr-Zr eutectic are also needed to further improve the oxidation resistance of Cr coated Zr. Minimal (<1%) swelling of U 3 Si 2 and subsequent fission gas release has been demonstrated up to 20 MWd/kgU. Irradiation experiments with U 3 Si 2 fuel in ATR to determine these properties at 40 MWd/kgU were completed but post irradiation examinations were not done since U 3 Si 2 has been replaced by UN. UN has three issues that are being addressed. The first is increasing the oxidation resistance so that there is not excessive reaction up to ~1500°C. While UN increases the pellet density and additives to the UN postponed the temperature at which rapid oxidation occurred by ~100°C to 200°C, this is not enough, and pellet coating options are now being pursued. The second is developing a method to manufacture that does not require the multi-step process of UF 6 to UO 2 to UC to UN. Efforts are underway looking at UF 6 to UN 2 to UN and UF 6 to UF 4 to UN 2 to UN reactions. Finally, an economically acceptable process for potentially enriching the 15 N content of the nitrogen used to make UN to >95% 15 N was identified though not experimentally validated. In addition to the work supported by the DOE, research and testing activities are being carried on in a world-wide effort funded by many countries such as Sweden, United Kingdom, Belgium, Netherlands, Spain, Germany, Japan, and France. This work is being facilitated through the Westinghouse led Collaboration for Advanced Research on Accident Tolerant Fuel (CARAT) program. Annual meetings were organized in 2018 and 2019 by Westinghouse as a venue for presentation of this work and to provide for the cross-fertilization of ideas among the many outstanding researchers in the ATF area. No meetings were held in 2020 and 2021 due to the COVID-19 related restrictions on traveling and gatherings. Since SiC, coated cladding, and high-density fuel options are not currently used in the nuclear industry; support from the government and industry members is needed to further the significant effort of setting new standards. The same is true for the Nuclear Regulatory Commission (NRC) which must review and approve the commercial use of these new fuels since all current regulations are oriented toward Zr/UO 2 fuel. Several meetings have been held with the NRC to generate a fast-track approach to licensing ATF using a combination of atomic modeling, in-rod sensors, and in-reactor testing. This approach was memorialized in an “Accelerated Fuel Qualification White Paper” prepared by the Accelerated Fuel Qualification Working Group lead by General Atomics.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2021

Measurement of Fission Product Concentration Profiles in AGR-3/4 TRISO Fuel Graphitic Matrix and Nuclear Graphites

The third Advanced Gas Reactor (AGR) irradiation experiment, AGR-3/4, was designed to investigate the migration of fission products in fuel compact graphitic matrix and reactor graphite components. Using destructive methods, radial fission product concentration profiles were measured for gamma-emitting fission products (e.g., Ag-110m, Cs-134, and Eu-154) and beta-emitting Sr-90 in irradiated graphitic and graphite components from six different AGR-3/4 irradiation capsules. These new measured concentration profiles can now be compared to non-destructive measurements and fission product transport simulations and will be used to derive new diffusivities and sorptivities to support refinement of fission product transport models and high-temperature gas-cooled reactor (HTGR) source-term analyses. Each capsule in the AGR-3/4 experiment had four fuel compacts in the middle of two concentric rings of graphitic matrix material, PCEA graphite, or IG-110 graphite. In addition to the approximately 1898 tristructural isotropic (TRISO) coated particles in each compact, there were 20 designed to fail (DTF) particles coated only in pyrocarbon so that they released fission products into the surrounding cylindrical rings of carbonaceous materials. Destructive sampling of the rings involved machining/milling material from around the circumference of the rings, collecting that material, and performing radiochemical analyses on it. Milling operations were performed in multiple steps or segments, and each segment was generally 0.508 mm (0.020 in) thick. Knowing the radial position at which each segment was milled, the volume of the milled material at each segment, and the fission product content in each segment, the radial fission product concentrations were constructed for select isotopes in each ring. Ag-110m profiles had the most variation. Some profiles were peaked at an inner or outer surface. Some were peaked at the middle of the ring wall thickness. Some increased radially outward, and some decreased radially outward. These types of variations and the fact that the measured profiles do not generally compare favorably with the transport model employed for AGR-3/4 may adversely impact the ability to extract reasonable transport parameters for this isotope. In many cases, the Cs-134 profiles decreased somewhat linearly in the outward radial direction, and in cursory comparisons, the shapes of these profiles appeared similar to those from model predictions. The step changes in concentration across the inner-outer ring gap were generally consistent with the model predictions as well. In some cases, there were local maxima in concentration at the outer surface of the rings. This suggests that fission products could have transported in the small gaps between the inner ring and the outer ring and between the outer ring and the sink ring such that some portion of a given fission product can bypass diffusion through the ring itself. The analysis of the small nubs on the outer surfaces of some of the outer rings revealed fission product concentrations in the nubs that were often higher than in the outermost segments of the rings. This further supports the hypothesis that short-circuit, gap transport occurred, causing relatively high surface concentrations on the outer surfaces of the rings. Eu-154 and Sr-90 profiles tend to have very similar shapes, suggesting that they transport via the same mechanisms. The observed profiles were indicative of a transport process where the isotopes are sorbed on the inner surface of the ring, but diffusion into the ring from that surface is quite slow. Some elevated concentrations of Sr-90 (relative to Eu-154) on the outer surface of a ring suggested that rapid, gas-gap transport of gaseous precursor Kr-90 and volatile Rb-90 could have occurred prior to their decaying to Sr-90. Overall, the Eu 154 and Sr-90 profiles were still very similar, which indicates that the transport of short-lived Sr-90 precursors is not a major effect. In some capsules, the qualitative Sr-90 behavior across the ring gaps was consistent with the model (using the available legacy Sr-90 transport parameters), but in other capsules the model was inconsistent with the measurements and seems to underestimate the amount of Sr-90 in the outer rings. The total ring Sr-90 inventories were estimated for all the rings that were subject to physical sampling. These results will be used to adjust the predicted particle and/or compact releases used in the AGR-3/4 fission product transport model. Given the different irradiation temperatures among the capsules and the rings, it was not possible to discern fundamental differences in the transport of isotopes within the different carbon materials, i.e., graphitic matrix, IG-110, or PCEA. It may be possible to do this in the course of determining transport from the concentration profiles in future work.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2022

AGR Program TRISO Fuel Topical Report Dialog

AGR Program Overview and Current Activities Fission Product Transport Data Short-Lived Fission Product Release Fuel Performance Margin Data Oxidation Testing Data

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2022

Ultra-low-level measurements of airborne fission products from the Fukushima Daiichi reactor accident using high volume collection systems at Savannah River National Laboratory

For this study, ultra-low-level measurements of radionuclides in air have been conducted at the Savannah River National Laboratory (SRNL) to determine the atmospheric concentration of fission products released following the Fukushima Daiichi reactor accident on March 11, 2011. Air filter samples were acquired from two high-volume collection systems (a traditional filter-based system and an electrostatic precipitator-based system) to monitor airborne radionuclide concentrations in the period covering from 2 weeks to 3 years after the disaster. The world-wide spread of low-level concentrations of airborne fission products from the Fukushima event provided a unique opportunity to demonstrate SRNL's electrostatic particle collection technology and other improvements in environmental monitoring developed at the Savannah River Site (SRS). Detecting and analyzing the release allowed a comprehensive test of SRS systems for monitoring environmental radioactivity. Gamma-ray-emitting fission products ( 131,132 I, 134,136,137 Cs, and 129,132 Te) and cosmogenic isotopes ( 7 Be and 22 Na) in air were detected and quantified by high-resolution gamma-ray spectroscopy at concentrations as low as 0.07 μBq per standard cubic meter (SCM) (50 mBq total 137 Cs), while plutonium content was quantified by thermal ionization mass spectrometry (TIMS) at concentrations as low as 6.5 × 10 –21 g/SCM (3.0 fg 239+240 Pu). Isotope concentrations measured at SRNL from gamma-ray spectroscopy were compared to independent measurements from Chapel Hill, NC, located approximately 370 km (230 mi) NE of SRNL. Meteorological modeling was also used to predict radionuclide transport from the location of release to both measurement locations.

63 RADIATION, THERMAL, AND OTHER ENVIRON. POLLUTAN↗