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The Advanced Reactor Terminology Graphite Research and Development program is currently measuring irradiated material property changes in several grades of nuclear graphite to predict behavior and operating performance within the core of these new high temperature reactor designs. The Advanced Graphite Creep (AGC) experiment, consisting of six irradiation capsules, will generate the irradiated graphite performance data for the Very High Temperature Reactor operating conditions. All six capsules in the experiment conducted at Idaho National Laboratory will be irradiated in the Advanced Test Reactor, disassembled in the Hot Fuel Examination Facility, and examined at the Idaho National Laboratory Research Center. This is the disassembly report describing the disassembly, shipment, post irradiation inspection, and storage of the graphite specimens contained within the AGC 4 irradiation test series capsule (the fourth irradiation capsule of the series). AGC 4 was irradiated in the Advanced Test Reactor (ATR) East Flux Trap (EFT) during ATR Cycle 157D, 158A, 162A, 162B, 164A, 164B, 166A, and Cycle 166B. Approximately 3.6 dpa was achieved. Desired experiment temperatures were exceeded by at least 100C during the second Cycle of irradiation due to the insertion of the KJRR experiment. The capsule was removed from the ATR and transferred to the Hot Fuel Examination Facility on May 15, 2020 and eventually unloaded into the Hot Fuel Examination Facility (HFEF) Decon Cell through Penetration 2D on February 26, 2021. It was moved to the HFEF Main Cell Window 3M for disassembly on March 15, 2021. Disassembly and specimen extraction began March 18, 2021, and packaging of the graphite specimens was completed on April 16, 2021. Several anomalies were noted, specifically that the radiological dose rates were nominally an order of magnitude higher than that of the previous AGC experiments. This report summarizes the disassembly of the AGC 4 experiment.

The Three Mile Island, Unit Two (TMI-2) pressurized water reactor core underwent a significant meltdown in 1979 due to an untimely combination of maintenance problems that led to a loss of feedwater, followed by a series of operational misunderstandings and errors. Primary coolant discharging through a malfunctioning valve represented what was analyzed as a “small-break” loss-of-coolant accident (LOCA) and ultimately became a full core meltdown. The melted core recovery process required the development of a wide array of tools. After approximately three years of water management and other cleanup actions, the first views of the core revealed a much higher degree of damage than previously expected. Approximately 62 metric tons of the core had melted, leaving only 42 of the 177 fuel assemblies standing with fuel rods intact. The core to be recovered was composed of loose, gravel-like and granular particulate material and a central solidified mass of formerly molten fuel. Molten fuel had also penetrated some of the pressure vessel internals and resolidified below the main core support structure. Robotic tools that had been designed for the task were of limited effectiveness due to the range of material types and phases.

The Three Mile Island, Unit Two (TMI-2) pressurized water reactor core underwent a significant meltdown in 1979 due to an untimely combination of maintenance problems that led to a loss of feedwater, followed by a series of operational misunderstandings and errors. Primary coolant discharging through a malfunctioning valve represented what was analyzed as a “small-break” loss-of-coolant accident (LOCA) and ultimately became a full core meltdown. The melted core recovery process required the development of a wide array of tools. After approximately three years of water management and other cleanup actions, the first views of the core revealed a much higher degree of damage than previously expected. Approximately 62 metric tons of the core had melted, leaving only 42 of the 177 fuel assemblies standing with fuel rods intact. The core to be recovered was composed of loose, gravel-like and granular particulate material and a central solidified mass of formerly molten fuel. Molten fuel had also penetrated some of the pressure vessel internals and resolidified below the main core support structure. Robotic tools that had been designed for the task were of limited effectiveness due to the range of material types and phases.

The Advanced Reactor Terminology Graphite Research and Development program is currently measuring irradiated material property changes in several grades of nuclear graphite to predict behavior and operating performance within the core of these new high temperature reactor designs. The Advanced Graphite Creep (AGC) experiment, consisting of six irradiation capsules, will generate the irradiated graphite performance data for the Very High Temperature Reactor operating conditions. All six capsules in the experiment conducted at Idaho National Laboratory will be irradiated in the Advanced Test Reactor, disassembled in the Hot Fuel Examination Facility, and examined at the Idaho National Laboratory Research Center. This is the disassembly report describing the disassembly, shipment, post irradiation inspection, and storage of the graphite specimens contained within the AGC 4 irradiation test series capsule (the fourth irradiation capsule of the series). AGC 4 was irradiated in the Advanced Test Reactor (ATR) East Flux Trap (EFT) during ATR Cycle 157D, 158A, 162A, 162B, 164A, 164B, 166A, and Cycle 166B. Approximately 3.6 dpa was achieved. Desired experiment temperatures were exceeded by at least 100C during the second Cycle of irradiation due to the insertion of the KJRR experiment. The capsule was removed from the ATR and transferred to the Hot Fuel Examination Facility on May 15, 2020 and eventually unloaded into the Hot Fuel Examination Facility (HFEF) Decon Cell through Penetration 2D on February 26, 2021. It was moved to the HFEF Main Cell Window 3M for disassembly on March 15, 2021. Disassembly and specimen extraction began March 18, 2021, and packaging of the graphite specimens was completed on April 16, 2021. Several anomalies were noted, specifically that the radiological dose rates were nominally an order of magnitude higher than that of the previous AGC experiments. This report summarizes the disassembly of the AGC 4 experiment.

The DOE SNF Working Group ASNF Subgroup and the U.S. Nuclear Waste Technical Review Board have identified knowledge gaps regarding the management of aluminum-clad spent nuclear fuel (ASNF).[1, 2] The objectives of this research are to observe, sample and analyze the nature of aluminum surface corrosion and corrosion layer chemistry relevant to the ASNF performance over the duration of the dry storage segment of the fuel life cycle. The primary goal is to build an understanding of ASNF behavior, from reactor service and wet storage through drying and dry storage, with parallel testing of surrogate materials. The premise is that residual water affiliated with the aluminum oxide from corrosion during reactor service and wet storage, continues to influence ASNF performance during dry storage, and that even after successful drying the surface conditions of ASNF have yet to be satisfactorily characterized. The initial scope collected and analyzed specimens from irradiated non-fuel components of aluminum-clad Advanced Test Reactor (ATR) fuel elements that are routinely removed at the end of reactor service life. Techniques have been developed for remote material sampling from ATR elements from vented dry storage at the Irradiated Fuel Storage Facility (IFSF). These techniques involve 1) nipping off a small corner of the aluminum near where the end box had been removed and 2) scraping the exterior (non-fueled) plate surface to collect an oxide sample. This second effort targets ATR elements expected to have seen the longest residence in storage, both in the CPP-603 pool (with poor water quality) and in dry storage at IFSF, within the fuel handling scheduled to consolidate ATR at IFSF and receive the remaining inventory at CPP-666. Follow on work has been proposed to nip corners and collect scrapings immediately following ATR fuel drying, before placement in dry storage. Sample analysis will use multiple techniques to understand the chemical composition and morphology of the surface oxides. A simultaneous effort is progressing to develop surrogate materials to enable rigorous controlled experiments. Consistently produced, these surrogate materials can then be used to demonstrate limitations inherent to remote sampling and to validate performance models under relevant constraints. The combined efforts will substantiate ASNF performance and fuel management decisions regarding drying and packaging over a more complete range of life cycle conditions. [1] DOE Spent Nuclear Fuel Working Group, Aluminum-Clad Spent Nuclear Fuel: Technical Considerations and Challenges for Extended (>50 Years) Dry Storage, DOE/ID RPT#: 1575, prepared by Aluminum-Clad SNF Sub Working Group, June 2017. [2] U.S. Nuclear Waste Technical Review Board, Management and Disposal of U.S. Department of Energy Spent Nuclear Fuel, A Report to the United States Congress and the Secretary of Energy, December 2017, p. 143.

Milestone report on sampling of long-term dry-stored ATR spent fuel elements. It describes tooling, sample acquisition methods and analysis of the aluminum oxide samples by scanning electron microscopy, thermogravimetric analysis, X-ray diffraction and transmission electron microscopy. The observations provide input to projections on controls necessary for maintaining the integrity of the fuel during extended interim storage.

Aluminum samples taken from discarded irradiated Advanced Test Reactor fuel element end boxes (upper and lower adapter ) were characterized to determine the chemical composition and hydration state of the surface oxides. The samples were analyzed using scanning electron microscope imaging and chemical identification, x-ray diffraction to evaluate crystalline morphology, and thermogravitational analysis to determine mass loss by dehydration. The samples were acquired from the discarded fuel element components stored in the ATR fuel handling canal and transferred to the Materials and Fuels Complex for analysis. The measurements indicate that the samples have limited oxide thickness, indicating that little corrosion has occurred beyond the initial passive layer that was intentionally formed prior to irradiation. The presence of minimal aluminum oxyhydroxide suggests that there will be minimal risk to store these fuels in air with limited risk for alteration of the base passive layer. These observations will be compared against samples that will be taken of the same type of fuel that has been in dry storage for more than 10 years.

This report documents the commercial spent nuclear fuel currently in storage at Idaho National Laboratory with a specific focus on the potential research and development (R&D) opportunities for this material. Commercial spent nuclear fuel is stored in dry casks on the INL site at the Idaho Nuclear Technology and Engineering Center (INTEC, formerly the Idaho Chemical Processing Plant or ICPP). This spent fuel was part of the DOE-industry cooperative dry cask demonstration project that began in 1983 and from historical fuel testing and treatment activities that had been performed at the Test Area North (TAN)-607 facility. Most of the fuel is “low burnup,” but given that it was removed from the respective reactors between 1970 and 1985, it was representative for its time. The majority of the fuel is of the 15×15 Westinghouse PWR variety, though additional fuel types (e.g., TN-BRP) and configurations are also stored. Potential R&D opportunities identified are (1) the REA-2023 cask, (2) the TN-BRP cask, and (3) the Castor V/21 cask. Fuel from the TN-24P may be an alternative to the intact assemblies in the Castor V/21. Specifically, the REA-2023 cask contains 9 rods that have been exposed to air since 2005. These rods have a detailed pre-loading characterization and thus any changes in corrosion or geometry can most likely be attributed to the storage environment. In addition, similar rods to the nine in REA-2023 reside in the Castor V/21 cask whose environment has been maintained with inert nitrogen. The Castor V/21 cask also contains intact PWR assemblies that could be used to perform limited confirmation of the pyroprocessing approach. An alternative to the use of the Castor assemblies for pyroprocessing is the consolidated fuel that is stored in the TN-24P, which would not require removal from the assembly grid since it has already been packaged in accessible two-piece shell strongback containers. The TN-BRP cask contains a number of Gd-doped, low burnup assemblies that could be of use to validate code packages used to justify burnup-up credit for boiling water reactors (BWRs). The INL dry casks are stored on the CPP-2707 pad at INTEC, adjacent to the CPP-603 Irradiated Fuel Storage Facility, which incorporates a dry hot cell that has the potential to receive a full scale commercial cask of the types identified. Several evaluations have been made regarding this task, including full scale mockup testing of the physical clearances required to remove and handle fuel assemblies and components. A proposed schedule of 14 months and cost of $5.3 million was the outcome of analysis performed by Fluor Idaho and is included as Appendix A & B. In addition to the spent fuel at INL, there is also a full-scale mockup assembly that was fabricated for the Protypical Consolidation Demonstration Project to validate fuel rod consolidation approaches. The assembly was fabricated by Westinghouse as a 15 x 15 PWR, using Zircaloy-4 tubing and steel end fittings in accordance with product specifications. The only departure from specification is the use of copper metal in lieu of uranium oxide pellets to achieve a weight that is within 10% of the standard.

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

Destructive post-irradiation examination was performed on AGR-1 fuel Compact 4-1-1, which was irradiated to a final compact-average burnup of 19.4% FIMA (fissions per initial metal atom) and a time-average, volume-average temperature of 1072°C. The analysis of this compact focused on characterizing the extent of fission product release from the particles and examining particles to determine the condition of the kernels and coating layers. The work included deconsolidation of the compact and leach-burn-leach analysis, visual inspection and gamma counting of individual particles, metallurgical preparation of selected particles, and examination of particle cross-sections with optical microscopy, electron microscopy, and elemental analysis. Deconsolidation-leach-burn-leach (DLBL) analysis revealed no particles with failed TRISO or failed SiC layers (as indicated by very low uranium inventory in all of the leach solutions). The total fractions of the predicted compact inventories of fission products Ce-144, Cs-134, Cs-137, and Sr-90 that were present in the compact outside of the SiC layers were <2×10^-6, based on DLBL data. The Ag-110m fraction in the compact outside the SiC layers was 3.3×10^-2, indicating appreciable release of silver through the intact coatings and subsequent retention in the OPyC layers or matrix. The Eu-154 fraction was 2.4×10^-4, which is equivalent to the inventory in one average particle, and indicates a small but measurable level of release from the intact coatings. Gamma counting of 61 individual particles indicated no particles with anomalously low fission product retention. The average ratio of measured inventory to calculated inventory was close to a value of 1.0 for several fission product isotopes (Ce-144, Cs-134, and Cs-137), indicating good retention and reasonably good agreement with the predicted inventories. Measured-to-calculated (M/C) activity ratios for fission products Eu-154, Eu-155, Ru-106, Sb-125, and Zr-95 were significantly less than 1.0. However, as no significant release of these fission products from compacts was noted during previous analysis of the AGR-1 capsule components, the low M/C ratios are most likely an indication of a bias in the inventories predicted by physics simulations of the AGR-1 experiment. The distribution of Ag-110m M/C ratios was centered on a value of 1.02 and was fairly broad (standard deviation of 0.18, with values as high as 1.42 and as low as 0.68). Based on all data gathered to date, it is believed that silver retention in the particles was on average relatively high, but that the broad distribution in values among the particles represents significant variation in the inventory of Ag-110m generated in the particles. Ceramographic analysis of particle cross-sections revealed many of the characteristic microstructures often observed in irradiated AGR-1 particles from other fuel compacts. Palladium-rich fission product clusters were observed in the IPyC and SiC layers near the IPyC-SiC interface of three Compact 4-1-1 particle cross-sections. In spite of the presence of fission product clusters in the SiC layer, no significant corrosion or degradation of the layer was observed in any of the particles examined.