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Contributions to the mechanistic understanding of the microstructural evolution in irradiated U-Mo dispersion fuel

Here, advanced microstructural characterization techniques, such as scanning electron microscopy (SEM) and scanning transmission electron microscopy - energy dispersive x-ray spectroscopy (STEM-EDS), were used to interpret the fuel microstructure evolution and fission products behavior in U-Mo dispersion fuel irradiated in the Advanced Test Reactor (ATR) as part of the European Mini-Plate Irradiation Experiment (EMPIrE) test. The larger as-fabricated fuel grain size achieved by heat-treating the U-Mo powder resulted in slower high burnup structure (HBS) development and reduced fission gas porosity. Slower HBS kinetics was observed at the fuel kernels’ periphery, which contained smaller and less fission gas bubbles at all fission densities (FDs) investigated and was attributed to a locally reduced damage density and fission products concentration, as corroborated with Monte Carlo simulations. The non-refined grains at the fuel kernel periphery hosted a perfectly ordered fission Gas Bubble Superlattice (GBS) up to 6.3 × 10 21 fissions/cm 3 . Nano-scale STEM-EDS analysis presented in this study provided useful information on the GBS characteristic morphology and evolution in U-Mo fuel. The concentration of fission gas in the GBS progressively increased with FD, pointing to an evolution of the nanobubble pressure status with irradiation. A possible connection between the GBS collapse and HBS onset is proposed for which there exists a threshold in the misorientation of the refined sub-grains above which the GBS stability during irradiation is no longer preserved, resulting in the GBS collapse.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

High-temperature steam oxidation study of irradiated FeCrAl defueled specimens

Post irradiation examinations (PIE) were performed on irradiated iron-chromium-aluminum (FeCrAl) specimens. These FeCrAl specimens were fabricated at the US Department of Energy's Oak Ridge National Laboratory (ORNL). The experimental setup involved subjecting FeCrAl cladding, along with UO 2 pellets, to irradiation in the Idaho National Laboratory Advanced Test Reactor (ATR). In parallel, the FeCrAl alloy tubing without UO 2 pellets was irradiated at ORNL's High Flux Isotope Reactor (HFIR). After irradiation, the ATR-irradiated rodlet was transported to an ORNL hot cell, where it was sectioned into multiple samples for the PIE and severe-accident testing. The sectioning process revealed that the fuel was not bonded to the cladding and could be easily detached from sectioned cladding slices. Microstructural analysis of the fuel cross sections demonstrated no significant interaction between the fuel and the cladding. Additionally, high-temperature steam oxidation tests on defueled cladding segments showed minimal oxygen uptake even at 1200 °C. Here, the ATR-irradiated specimens began to exhibit signs of enhanced oxidation upon reaching a temperature of 1300 °C. Furthermore, enhanced oxidation was observed on the inner surface of the ATR-irradiated FeCrAl specimen, which had been subjected to 1300 °C for a duration of 1 min. By contrast, high-temperature steam oxidation experiments indicated that the HFIR-irradiated FeCrAl cladding provided good thermal stability when exposed to 1300 °C for up to 4 h. Comparative analysis encompassing the oxidation behavior of the ATR-irradiated fueled FeCrAl, HFIR-irradiated unfueled FeCrAl, and unirradiated FeCrAl suggests that the fuel–cladding interaction, although not visible via standard microscale electron microscopy measurements, may accelerate the deterioration of FeCrAl cladding in beyond-design-basis accident scenarios.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

FAST irradiations and initial post irradiation examinations – Part I

The Advanced Fuels Campaign Fission Accelerated Steady-state Test (FAST) at Idaho National Laboratory (INL) completed its first irradiation cycle within the Advanced Test Reactor (ATR). The test focused on the irradiation of alloy fuel forms for use in sodium fast reactors. Tests included the use of fuel additives (Sn, Sb, and Pd) for reducing the gettering of lanthanide fission products, zirconium liners to mitigate fuel-cladding chemical interaction, and annular fuel geometry for sodium-free fuel designs. The first cycle of FAST testing was completed and a series of rodlets were removed for the initial post irradiation examination (PIE) of FAST rodlets. The rodlet irradiation conditions was evaluated using Monte Carlo N-Particle (MCNP) for as-run power history and COMSOL for temperature analysis. These rodlets include a set of low burnups (~2.5 % heavy metal [%FIMA]) control rodlets and a helium bonded annular rodlet (4.7 %FIMA). Initial non-destructive PIE has been completed and includes, visual inspection, neutron radiography and gamma scanning of the FAST rodlets. Radiography confirmed the integrity of the experiments as well as showing the complete filling of the annulus in the annular fuel at a modest burnup (4.7 %FIMA) and potential slumping of the cooler rodlets at lower burnup. Precision gamma scanning indicated mostly usual fission product behavior with the exception of the ceasium in the He-bonded annular fuel. Future destructive PIE will be necessary in order to fully understand the effects of accelerated irradiation on U-Zr metallic fuel behavior.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Modeling and simulation study for the design of the Fuel Interrogation and Examination using Submersible Tomography Analysis Mk II instrument

Here, the design of a submersible, gamma-ray tomography system for imaging irradiated nuclear fuel is described. The system—named Fuel Interrogation and Examination using Submersible Tomography Analysis (FIESTA) Mk. II—is a variation on a previous Mk. I I design, which was developed to non-destructively image fuel capsules irradiated in the Advanced Test Reactor at the Idaho National Laboratory. The FIESTA system uses a combination of transmission computed tomography and emission computed tomography to image the restructuring and fission product migration at different points of burnup. Changes made to FIESTA Mk. I reflect the revised design requirements and a need to reduce background noise, largely originating from downscattered photons from fuel and transmission source. The computational design and radiation transport simulations are described.

46 - INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AN↗

Sensitivity study of coupled chemical-CFD simulations for analyzing aluminum-clad spent nuclear fuel storage in sealed canisters

We report the United States Department of Energy (DOE) manages over 50 Metric Tons Heavy Metal (MTHM) of aluminum-clad spent nuclear fuel. One main source for DOE’s Aluminum-clad spent nuclear fuel (ASNF) inventory is the advanced test reactor (ATR) at the INL site, which makes this fuel of particular interest for storage scenarios. Road-ready and final disposition packaging configurations for the ATR fuel dictates storage within helium-backfilled, sealed DOE standard canisters. The conditions within these sealed canisters for extended (greater than50 year dry) storage is of interest. To further this goal, a three-dimensional (3D) multi-physics computational fluid dynamics (CFD) model is developed of the sealed DOE standard canisters. This 3D CFD model is one-way coupled with bulk gas radiolysis reactions considering sealed canisters with inert gas and possible trace amounts of air and water vapor. This study looks at the evolution of the thermal history of the canisters over a 50 year time period with a coupling to the chemical reactions occurring from radiolytic breakdown of residual water. A sensitivity study is then carried out over the parameters of the model including the fuel decay heat, residual water content, sealed pressure, canister external temperature, and canister emissivity. In pure helium, hydrogen generation rates are low, under 10 ppm, but hydrogen generation rates are affected greatly by the presence of even 1% residual air, increasing by 50-plus-fold, and nitric acid generation with residual air also occurs ranging from 500 to 4000 ppm after 50 years. The fuel decay heat and the residual water content show the most importance in the generation of hydrogen gas in pure air, and for nitric acid with a residual air condition. External temperature, canister emissivity and sealed pressure all show minor sensitivity effects to the generation of potentially harmful species.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Interaction of Polymethyl Methacrylate with Boehmite-Filmed Aluminum Cladding Under Gamma Irradiation

This paper presents an overview of ongoing work to qualify the Advanced Test Reactor (ATR) driver fuel elements that have been affected by irradiation-degraded polymethyl methacrylate (PMMA) flux wands. Irradiation testing was performed on PMMA material in contact with aluminum clad material. The cladding was prefilmed with a boehmite oxide layer, an important feature of the ATR driver fuel. The effects on the boehmite layer due to gamma irradiation of the PMMA-aluminum clad system were investigated. PMMA embrittlement, followed by softening and degradation, occurred at high radiation levels. Adhesion between the cladding and irradiated PMMA was observed. Flow testing at prototypic ATR flow rates demonstrated the effective removal of the adhered material. Measurements of the boehmite layer thickness were performed, and Raman spectroscopy was utilized to detect the presence of boehmite in the irradiated PMMA material.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Progress on Pu-238 production at Idaho National Laboratory from February 2022 to July 2023

Idaho National Laboratory (INL) has continued to qualify irradiation positions in the Advanced Test Reactor (ATR) for Pu-238 production to support NASA deep space missions. Over the past year, INL qualified Np-237 targets for ATR’s North East Flux Trap (NEFT), Inner-A and H positions. Work has begun to requalify the South Flux Trap (SFT) and to qualify the East Flux Trap (EFT) for the ATR GEN I target and is midway through the qualification process. This paper gives an overview of operational and technical activities from February 2022 to July 2023.

07 ISOTOPE AND RADIATION SOURCES↗

As-Run Thermal Analysis for the CSM-10584 Experiment

The purpose of this document is to present the as-run specimen temperatures for the CSM-10584 experiment irradiated in position B-5 of the Advanced Test Reactor (ATR) for Cycles 164A and 164B.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Completion of Irradiation of Sensors in ATRC Milestone

This set of PowerPoint slides demonstrates how milestone "M2CT-21IN0702023: Perform test of neutron flux sensors in the Advanced Test Reactor Critical Facility". It supports an entry in PICS claiming achievement of the milestone. These slides provide a good summary of the purpose and impact of the milestone for our DOE Headquarters colleagues.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Automated Internal Energy Calibration by OnTheFly for AGR-5/6/7

The software program, OnTheFly, was developed at Idaho National Laboratory (INL) to keep high-purity germanium (HPGe) detectors energy calibrated during very long experiments. Over time, spectra produced from a HPGe detector will slowly stretch or contract, causing the energy calibration to change. If the energy calibration changes too much, it will cause energy lines to be misidentified. The higher the energy line the more affected they are by this change. OnTheFly tracks and adjusts the slowly changing energy calibrations so the energy lines will not be misidentified. OnTheFly was used with the Fission Product Monitoring System (FPMS) during the AGR-5/6/7 irradiation experiment performed at INL’s Advanced Test Reactor (ATR). Five HPGe detectors were used to monitor the five capsules in AGR-5/6/7. There were also two extra HPGe detectors that were maintained as spares. Before each ATR cycle of the experiment, the HPGe detectors were energy calibrated with a thorium radioactive source. During each ATR cycle, each detector would acquire data for 8 hours and then reset and acquire data for another 8 hours. After each 8-hour run, the spectra would be saved and analyzed autonomously. The results were then read by OnTheFly and used to produce a new energy calibration for each detector. The new energy calibrations were compared to the current energy calibrations and, if certain criteria were met, the new energy calibration would replace the current energy calibration. The new energy calibration would be used for future spectra. OnTheFly was run at least every couple of days but could be run as much as after each 8-hour run. OnTheFly kept the spectra energy calibrated during the ATR cycles over the 2 years and 5 months that the AGR-5/6/7 experiment ran.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

High Temperature Steam Oxidation of Irradiated FeCrAl in the Severe Accident Test Station

FeCrAl-UO2 test capsules were fabricated at Oak Ridge National Laboratory (ORNL) and irradiated at the Advanced Test Reactor. Following irradiation, samples were sectioned from the irradiated rod and oxidation kinetics were evaluated to access the candidate cladding high-temperature oxidation performance following irradiation. The irradiation was performed at approximately 400°C to a burnup of 10 GWd/MT. The high-temperature oxidation tests were conducted in the ORNL Severe Accident Test Station at 1200 and 1300°C. Weight measurements were taken before and after oxidation testing. Cross-sections of the cladding were metallographically mounted and optical microscopy was performed. Measurements of the oxidation layer before and after high-temperature testing were collected. The results indicate the irradiated FeCrAl C35M alloy provided good thermal stability up to 1200°C.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

USHPRR MP-1 Irradiation Test: Assessment of Edge Pitting and Bond Line Corrosion in Vendor Produced Fuel Plates

This report summarizes an effort to identify the source of anomalous localized edge pitting and bond line corrosive attack of experimental mini fuel plates manufactured at the commercial fuel vendor BWXT and tested in the Advanced Test Reactor (ATR) at Idaho National Laboratory (INL) as part of the Miniplate 1 (MP-1) irradiation test. The MP-1 test was conducted by the US High Performance Research Reactor Project (USHPRR) and overseen by the Fuel Qualification Pillar (FQ). The test involved evaluation of a mix of 62 “vendor” fuel plates fabricated at BWXT and 12 “laboratory” fuel plates fabricated at Idaho National Laboratory using commercial-scale and labscale fabrication processes respectively. The MP-1 test was the first in a series of tests to generate data to support qualification of a new plate-type low-enriched uranium (LEU) U-10Mo monolithic fuel system. The major objective of the MP-1 experiment was to test, for the first time, miniplates fabricated by a commercial fuel vendor over the range of irradiation conditions relevant to conversion of NRC regulated High Performance Research Reactors (HPRRs) from high-enriched uranium to LEU. The focus of the efforts described in this report are the vendor fuel plates to inform changes in the fabrication process prior to fabrication of the next miniplate experiment MP2.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Modeling of ATR fuel in DOE Standard Canisters with Helium Backfilled Condition

Road-ready and final disposition packaging configurations for the advanced test reactor (ATR) fuel dictates storage within helium backfilled sealed DOE standard canisters. These sealed canisters are intended for extened (>50 year) dry storage). The typical packaging configuration for the 15-foot DOE canisters places 10 ATR elements within a Type 1a basket, and three baskets are loaded within each DOE canister. During in-reactor operations and cooling pond storage conditions, oxyhydroxide layers form on the surface of the aluminum clad fuel. These layers produce hydrogen gas over time due to the fuel’s radiation field. As part of the packing procedure, the ATR fuel should be dried to remove any residual physio-/chemi- sorbed water from the surface. As testing to the effectiveness of the drying procedure is still underway, this modeling will include results at fully saturated and fully dried conditions. In previous modeling efforts, the G-value for the production of hydrogen from the oxyhydroxide layers was assumed to be in argon environments as measured by Task 2 - Oxyhydroxide Layer Radiolytic Gas Generation Resolution. Previous experimental testing showed differences in the hydrogen generated based on the gaseous environment. In the associated experimental work, Task 2 - Oxyhydroxide Layer Radiolytic Gas Generation Resolution, additional tests were completed in a helium environment, and updated G-values for the radiolytic production of hydrogen from the oxyhydroxide layers were provided. These values are 28% and 58% higher than values for argon. In addition, a change to the modeling of the oxyhydroxide radiolysis has been made from previous reports. This change assumes the dependency of the dose rate on the overall reaction rate is applied to the total weight of the sample, rather than to just the weight of the oxyhydroxide layer. This decreases the dependency of the radiolytic reaction on the thickness of the oxyhydroxide layer. For a nominal scenario of stored ATR fuel, assuming the chemi-/physio- sorbed water have been fully removed, the internal canister pressure increases to 1.61 atm over a 50 year period, with a hydrogen mole percentage of 21%. As in previous modeling, any oxygen present is in negligible amounts (<1 ppt). If a small amount residual air is present, nitric acid can form up to 1300 ppm. For a scenario with high fuel decay heat, the model shows internal pressure increasing to 2.1 atm, with 39.3 mole percentage of hydrogen. In a scenario where significant chemi-/physio- sorbed water is present within the corrosion layer, the nominal scenario shows a pressure increase to 2.54 atm, with 21.1 mole percent hydrogen. The high decay heat case shows a pressure increase to 3.18 atm with 39.9 mole percent hydrogen.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Modeling Summary of ASNF in DOE Sealed Standard Canisters

A pathway for road-ready and final disposition packaging configurations for the aluminum-clad spent nuclear fuel (ANSF) fuel dictates storage within helium backfilled sealed DOE standard canisters. The typical packaging configuration for the 15-foot DOE canisters places 10 advance test reactor (ATR) elements within a Type 1a basket, and three baskets are loaded within each DOE canister. During in-reactor operations and cooling pond storage conditions, oxyhydroxide layers form on the surface of the aluminum clad fuel. These layers produce hydrogen gas over time due to the fuel’s radiation field. As part of the packing procedure, the ATR fuel should be dried to remove any residual physio-/chemi- sorbed water bound to the surface. The results of this modeling will include results at fully saturated and fully dried conditions. In addition, fuels that are currently stored at the Savannah River Site were also studied for their potential for hydrogen and pressure build up. These two additional fuels modeled were the Missouri University Research Reactor (MURR) fuel, which is packaged in the same configuration as the ATR, but with a 10-foot-tall DOE standard canister. This was selected due to its relatively high decay heat compared to other DOE-managed ASNF. The second additional fuel studied with the modeling effort was the High Flux Isotope Reactor (HFIR) fuel. This fuel is modeled as two separate DOE canisters with the inner and outer annulus split for storage. The HFIR was selected for study due to its high aluminum cladding surface area. In the associated experimental work, Task 2 - Oxyhydroxide Layer Radiolytic Gas Generation Resolution, additional tests were completed in a helium environment, and updated G-values for the radiolytic production of hydrogen from the oxyhydroxide layers were provided. These values were 2.92 ×10 -4 µmol/J at 50% relative humidity and 4.12 ×10 -4 µmol/J at 100% relative humidity. These values are lower than the value for Argon that was used in prior modeling results. In addition, prior modeling results have been completed with the G-value applied to just the mass of the corrosion layer, and this has been updated to apply the G-value for hydrogen generation to the full mass of the fuel. These two effects combine to show much smaller pressure and hydrogen build up for the sealed canister model. For a nominal scenario of stored ATR fuel, after 50 years the model results give a 1.36 atm total pressure, 7% mole percent hydrogen, for the upper decay heat, 1.51 atm total pressure, 16% mole percent hydrogen, and for upper decay heat with undried fuel 2.6 atm total pressure, 15% mole percent hydrogen. For the MURR nominal case, the model results give 1.34 atm and 6% hydrogen, for upper decay heat this gives 1.41 atm total pressure with 10.8 % hydrogen, and for upper decay heat with undried fuel, this gives 2.38 atm total pressure with 9.9% hydrogen. The nominal scenario for HFIR fuel gives 1.39 atm total pressure with 9.9% hydrogen, the upper decay heat case gives 1.43 atm with 12.1% hydrogen, and the upper decay heat with undried fuel gives 2.17 atm total pressure with 11.9% hydrogen. These results confirm the ATR scenario bounds the other intact ASNF modeled here. No case modeled yields significant oxygen, and the lower decay heat cases for all fuels modeled have hydrogen concentrations that are under the 4% flammability limit after 50 years of storage. In addition, the modeled pressures for all cases are all significantly below the 500-psi limit for the DOE standard sealed canister.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Extended Modeling of DOE Sealed Canisters with Updated Chemistry Models

Road-ready and final disposition packaging configurations for the advanced test reactor (ATR) fuel currently specifies storage within helium backfilled DOE sealed standard canisters. The aluminum cladding of the ATR fuel contains an oxyhydroxide layer of boehmite/bayerite that generates hydrogen when subjected to irradiation. Understanding the effect of this hydrogen buildup over time to important for long term storage considerations. Previous modeling efforts have built a coupled CFD-chemical model to simulate the temperature gas phase concentrations within the DOE sealed standard canisters. These models have coupled the temperature conditions to both the gas phase radiolysis chemistry and the surface chemistry associated with the oxyhydroxide layer. The previous iteration of the model utilized constant G-values for the hydrogen generation a 50-year period. This new iteration of the model utilizes new experimental data to update the hydrogen generation rate, as well as increase the simulated time to a 200-year period. Given the half-life assumed for the primary Cs-137 isotope responsible for gamma radiation in the ATR spent fuel, the 200-year period decreases the decay heat and dose rate of the spent fuel by a factor of 100, which combined with the updated chemistry substantially decreases new hydrogen generation. Continued experimental work has identified trends for aluminum surrogate samples with oxyhydroxide layers for tests done at higher dose rates. At low initial doses a fast generation rate of hydrogen occurs which starts to roll over to a lower generation as the total dose applied increase. A small-scale chemical model was built to replicate as mini-canister surrogate system at SRNL as well as for the smaller capsule tests performed at INL. A variety of chemical models to capture this effect were tested, and a back reaction of H radical absorbing onto the surface, or inhibition of the reaction by significant H 2 cover gas were both able to fit both the mini-canister and the small capsule test data. Both kinetic fits were used to generate data from the new 200-year simulation. As additional experiments continue, the kinetic fits may be adjusted to adapt to new data. However, updated data shows that hydrogen atmosphere has little effect on actual generation data, so the model was reverted to use a star-stepped G-value for low-dose and high-dose regions. For the undried fuel case, the three models differ significantly with an end concentration of 1% for back reaction, 4.2% for inhibition, and 13.1% for constant G-value for the nominal scenario. For the dried fuel case, the nominal cases showed end concentrations of 0.23% for back reaction, 1.9% for inhibition, and 4.2% for const G-value for the nominal scenario. For the constant G-value case that is less conservative than the other two, the pressure for undried fuel increases to 1.94 atm over 200 years for the nominal case and 2.11 atm for the high decay heat case. The total hydrogen concentration after 200 years is 4.92% for the low decay heat case and 27.4% for the high decay heat case for undried fuel and is 1.4% and 9.6% for low and high decay heat fuel for the dried fuel case. If small amount of residual air is present, the potential for nitric acid formation of 595, 1568, and 2816 ppm for the lower, nominal, and upper fuel decay heat can occur. At long-term timeframes no significant shift in major species present occurs, so no appreciable amount of oxygen is present in the system. The continued rate of hydrogen generation in the canister occurs at an increase of 0.04% by mole over the final 10 years. Increasing the model range out to 1000 years continues to drop the hydrogen generation rate through decreasing dose rate.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

CFD-Chemical Model of One-Third Scale Demonstration of DOE Sealed Canister with ATR Fuel

Road-ready and final disposition packaging configurations for the advanced test reactor (ATR) fuel currently specifies storage within helium backfilled DOE sealed standard canisters. The aluminum cladding of the ATR fuel contains an oxyhydroxide layer of boehmite/bayerite that generates hydrogen when subjected to irradiation. Understanding the effect of this hydrogen buildup over time to important for long term storage considerations. Previous modeling efforts have built a coupled CFD-chemical model to simulate the temperature gas phase concentrations within the DOE sealed standard canisters. A demonstration case for these DOE sealed canisters will be eventually performed with a one-third scale mockup that has been instrumented with thermocouples and gas concentration probes. This study seeks to model the planned canister for validation of the previously developed model, such that confidence in its long-term prediction can be increased. The deployment of the instrumented lid for online monitoring in intended for a period of 10+ years based on previous monitoring of commercial fuel storage; however, the model is still run for the previously used 50-year storage periods. This case is modeled with a G-value using a bi-linear function such that it decreases at higher dose rates to be consistent with experiments. Validation efforts of the model would likely revolve around the results for the 1st year, so the results of this timeframe are also highlighted. For dried fuel of the nominal decay heat (18W), the predicted hydrogen concentration is 0.19% after 1 year, 0.91% after 10 years, and 2.8% after 50 years, with a maximum pressure of 1.26 atm. Consistent with previous modeling, the decay heat of the fuel is the main factor that influences the results. For undried fuel in pure helium, the hydrogen concentration ranges from 0.23 to 1.2% after 1 year, 1.25-6.2% after 10 years and 8.8 to 18.84% after 50 years. For dried fuel in pure helium the hydrogen concentration ranges from 0.06% to 0.34% after 1 year, 0.35-2.11% after 10 years and 0.95 to 6.6% after 50 years. While long-term results in the presence of residual air are mostly the same, early reactions with O 2 can delay significant production of H 2 until it is consumed to form more water vapor, lowering the range to 0.14 to 1.0% after 1 year. The maximum absolute pressure that is reached across any scenario is 2.06 atm. In the event of residual air, the presence of nitric acid is possible in the range of 18-131 ppm after 1 year, 174-1180 ppm after 10 years, and 586-3500 ppm after 50 years. As long as the fuel is sufficiently dried, or of nominal decay heat, a 4% lower flammability limit of hydrogen will not be reached within a 10-year monitoring period.

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Milestone 1.2.11: H 2 Production from Surrogate Non-Native Corrosion Plumes on Aluminum 6061-T6 Fuel Cladding Surrogates

Thick, localized, “non-native” corrosion plumes have been identified on Advanced Test Reactor fuel elements, raising concern on their impact on the radiolytic formation of molecular hydrogen gas (H 2 ) from aluminum-clad spent nuclear fuel (ASNF) under proposed extended (> 50 years) dry storage conditions. Here, we report our findings on H 2 generation from the gamma irradiation (up to 52 MGy) of surrogate “non-native” corrosion plume coupons: ambient-temperature-corroded (~350 days in water) aluminum alloy 6061 (AA6061) coupons in helium gas environments with ~0% added relative humidity. Additionally, we provide a comparison of proposed ASNF drying techniques— vacuum drying only, vacuum drying + 100 °C for 4 hr, and vacuum drying + 220 °C for 4 hr—on the yield of H 2 from these surrogate systems. The presented data indicates that similar amounts of H 2 (~2 × 10–3 µmol J–1) are formed from gamma irradiated AA6061 coupons corroded under different temperature regimes, i.e., ambient/350 days vs. 90 C/30 days. These findings validate current, complimentary modelling predictions based on high-temperature-corrosion irradiation data only. Further, the application of a heat treatment procedure (100 and 220 °C), in conjunction with vacuum drying, accelerated the rate at which a steady-state H 2 yield was attained, in comparison to vacuum only, due to the removal of H 2 precursors in the form of adsorbed waters. Interestingly, within the confidence limits of our measurements, negligible difference in total H 2 yield was found between the two investigated heat treatment procedures.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Report on Hydrogen Content Measurements of Yttrium Hydrides

This report describes the hydrogen content measurements of yttrium samples as irradiated at Advanced Test Reactor as part of the Microreactor Program. Irradiated samples were prepared at the facilities of Analytical Research Laboratory (ARL) of Materials and Fuels Complex (MFC). Hydrogen content measurements were performed on reduced size specimens using an inert gas fusion analyzer. For a single sample, replicate samples were prepared and tested to improve statistics of results. Uncertainty analyses were conducted using two approaches to determine the hydrogen content variations in the samples. Hydrogen content of irradiated specimens were both lower and higher than the expected values, indicating stoichiometry variations. Hydrogen was detected in all samples, even for the cracked capsule’s specimens. Results also suggested a potential hydrogen redistribution is present between samples inside the capsules.

08 HYDROGEN↗