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Post-irradiation examination of UN-Mo-W fuels for space nuclear propulsion

The National Aeronautics and Space Administration's return to space nuclear propulsion stems from the need for a more efficient method of space travel. Nuclear thermal propulsion systems have been shown to be two times more efficient than chemical propulsion. NASA's Sirius program was created to fabricate and test fuels for space nuclear propulsion, specifically to determine their performance under prototypical startup conditions. The Sirius project featured 4 test capsules, Sirius-1 featured uranium nitride fuel dispersed in a matrix of tungsten and rhenium, while Sirius-2A, -2B, and -3 featured uranium nitride-molybdenum-tungsten fuel (UN-Mo-W). This study discusses the Sirius-2A and -2B irradiation experiments at the Idaho National Laboratory, specifically their performance under irradiation at the Transient Reactor Test Facility. It was found that the fuel samples overall did not exhibit significant cracking, though the Sirius-2A fuel did have one large crack on the surface of the fuel. There was minimal hydrogen absorption in the samples, though it is unknown if the absorption occurred during irradiation or during fabrication. Mechanical testing indicated that the UN fuel demonstrated ceramic behavior as expected, and the Mo/W matrix demonstrated linear elastic behavior to failure.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Progress Report on SFR Metallic Fuel Data Qualification

This report summarizes the progress of SFR metallic fuel qualification related activities, which are focused on providing quality assurance relevant information applicable to experiments irradiated during the Integral Fast Reactor (IFR) program. A background of metallic fuel performance data and the associated databases, including the EBR-II Fuels Irradiation & Physics Database (FIPD) and Out-of-Pile Transient Database (OPTD), is included. The legacy data in the databases, including as-built, post-irradiation examination (PIE), operating parameters, and out-of-pile experiment data are introduced. The SFR metallic fuel Quality Assurance Program Plan (QAPP) and its implementation to qualify these legacy data is described in detail. Important PIE data QA documents and the specifications of four types of PIE measurements (contact profilometry, laser profilometry, neutron radiography and gamma scan) are provided. Examples of the implementation of the QAPP to qualify each of those types of PIE data are provided.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Progress Report on SFR Metallic Fuel Data Qualification

This report summarizes the progress of SFR metallic fuel qualification related activities, which are focused on providing quality assurance relevant information applicable to experiments irradiated during the Integral Fast Reactor (IFR) program. An overview of the metallic fuel performance data and the associated databases, including the EBR-II Fuels Irradiation & Physics Database (FIPD), Out-of-Pile Transient Database (OPTD), and TREAT Experimental Relational Database (TREXR) is included. The legacy data in the databases, including as-built, post-irradiation examination (PIE), operating parameters, and out-of-pile experiment post-test data are introduced. The SFR metallic fuel Quality Assurance Program Plan (QAPP) and its implementation to qualify these legacy data is described in detail. Important PIE data QA documents and the specifications of seven types of PIE measurements (contact profilometry, laser profilometry, neutron radiography, gamma scan, fission gas release fission gas chemistry, and metallography) are provided. Examples of the implementation of the QAPP to qualify each of those types of PIE data are provided.

Mo, Kun [Argonne National Laboratory (ANL), Argonn↗

JMOCUP Physics Depletion Calculations for the As-Run AGR-5/6/7 TRISO Particle Experiment in ATR Northeast Flux Trap

This ECAR documents the as-run Jim Sterbentz’s MCNP ORIGEN Coupled Utility Program (JMOCUP) physics depletion calculation and the calculated results for the AGR-5/6/7 irradiation experiment in the Advanced Test Reactor (ATR). AGR 5/6/7 was irradiated for nine power cycles in the northeast flux trap. The depletion calculations were performed to provide input data for a variety of other engineering analyses supporting the AGR-5/6/7 experiment along with post-irradiation characterization of the tri-structural isotropic (TRISO) particle fuel compacts. Detailed full-core MCNP models and Oak Ridge Isotope Generation (ORIGEN2) radionuclide generation models were specifically developed as part of the JMOCUP Monte Carlo depletion calculations. The MCNP ORIGEN2 computer codes were coupled using the well-established JMOCUP utility modules to couple the two codes and run the depletion calculations. The physics calculations were performed in support of the Advanced Gas Reactor (AGR) program.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Assessing the Impact of Large Removable Beryllium Reflector Experiments on HFIR Performance and Safety Metrics

This study investigated the effect of various removable beryllium (RB) experiment configurations on High Flux Isotope Reactor (HFIR) metrics to address increasing interest in these facilities for materials and fuels irradiation research. The RB reflector contains eight large and four small irradiation experiment facilities that offer excellent neutron flux conditions to perform fission and fusion reactor materials and fuels irradiation research. This work aims to outline acceptable RB configurations based on safety, performance, and programmatic metrics. This study assessed experiment effects on reactivity, cycle length, fission rate density distributions, and neutron flux distributions using the Shift, HFIRCON, and SCALE ORIGEN codes. Initial evaluations focused on generic experiment materials including aluminum plugs, stainless steel plugs, molybdenum plugs, and aluminum plugs with gadolinium shields. Subsequent analyses of MiniFuel experiments were performed to evaluate a heterogenous experiment, consisting of a more complex geometry and bearing several materials, and to test the correlations developed with the generic materials on a real experiment. Furthermore, the effects of neutron poison concentrations in the standard beryllium plugs were evaluated. When assuming a reference RB configuration with eight large fresh beryllium plugs, perturbed configurations with three aluminum plugs, one stainless steel plug, one molybdenum plug, one gadolinium-shielded aluminum plug, and one MiniFuel experiment resulted in a cycle length reduction of less than 1.3 days, the current threshold before requiring additional approvals. Configurations with five aluminum plugs, one stainless steel plug, one molybdenum plug, one gadolinium-shielded aluminum plug, and two MiniFuel experiments meet the 1.3 day limit if irradiated beryllium plugs are considered. Fuel element fission rate density distributions remained within safety limits, with maximum local increases under 9%. Neutron flux calculations revealed large thermal flux depressions inside and around the perturbed RB facilities, while epithermal and fast neutron fluxes increased because of reduced neutron moderation by the perturbed materials. These findings provide valuable guidance for optimizing RB configurations to balance safety and performance at HFIR.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Role of microstructure on CO corrosion of SiC layer in UO₂-TRISO fuel

The Advanced Gas Reactor Fuel Qualification and Development (AGR) program has focused on qualification of UCO kernel tristructural-isotropic (TRISO) particle fuel relative to UO₂ kernel TRISO particle fuel. However, a UO₂ kernel variant was included in the second AGR irradiation experiment (AGR-2) for comparison and to connect to historic fuel irradiation data. The development of a multiscale, post-irradiation examination (PIE) analysis approach through the AGR Program has allowed for a comprehensive understanding of individual particle failure. This approach has been applied to gain an understanding of SiC layer failure in UO₂ kernel TRISO fuel from AGR-2 after safety testing at 1600–1700 °C. Particle failure by intergranular CO corrosion, facilitated by a compromised inner pyrolytic carbon layer, has been confirmed through the combined application of modern x-ray computed tomography and electron microscopy techniques. In addition, a relationship between grain boundary character and CO corrosion has been identified. This finding provides an opportunity to develop mitigating strategies to improve the resilience of the SiC layer to CO corrosion in UO₂ TRISO fuel.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Fundamental Graphite Irradiation Behavior Research at ORNL for FY23

This letter report is in submission of completion of the Level 3 milestone number within the larger Advanced Reactor Technologies Gas Cooled Reactor program at Oak Ridge National Laboratory (ORNL). The focus of this year’s efforts is the aggregation of background information about the irradiation experiments for property change in H-451 graphite, getting the irradiation-induced property change of IG-110 and ETU-10 written up in journal articles for publication, and involvement with ASTM D02.F0 Manufactured Carbon and Graphite Products and the ASME Working Group on Nonmetallic Design and Materials (SG HTR)(BPV III). This report will document the status of these activities.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Develop Accurate Techniques for Passive SiC Temperature Monitoring of Miniature Samples for Cross-Cutting Applications

Passive thermometry is critically important because most fuels and materials irradiation experiments are not instrumented, and it is necessary to understand the irradiation temperature to properly interpret any post-irradiation examination data, including evolving properties and/or microstructures. The standard passive thermometry approach uses continuous dilatometry to evaluate changes in the instantaneous coefficient of thermal expansion during post-irradiation thermal annealing. This approach has limitations in terms of sample size (minimum length requirements) and the maximum irradiation temperature that can be accurately determined, which is limited by the reduced swelling (and therefore recovery) following higher temperature irradiation and limitations on the furnaces used with push-rod dilatometers. This work evaluates two new proposed techniques for post-irradiation evaluation of passive SiC temperature monitors: differential scanning calorimetry (DSC) and Raman spectroscopy. DSC is an extremely sensitive technique that can be used for any specimen geometry and is capable of higher temperature operation. Raman spectroscopy is similar in that it is a surface technique capable of examining extremely small samples (submillimeter), can be used with a heated stage up to 1,500°C (planned for future work), and is capable of mapping local irradiation temperatures throughout a sample. Existing SiC samples that were previously irradiated over a wide range of temperatures were cut into multiple pieces to allow for annealing studies using multiple different techniques: dilatometry, DSC, and Raman spectroscopy. This approach mitigates the concern that samples analyzed using one technique may have a slightly different irradiation history than those analyzed using a different technique. Recovery was clearly observed during annealing using both DSC and dilatometry. In some cases, a direct comparison could not be made due to some of the DSC runs accidentally including material from multiple specimens and issues with using an alternative DSC sample holder for the highest temperature annealing studies. Nevertheless, one trend was clear: the DSC runs resulted in higher irradiation temperatures compared to those of the dilatometry runs. Part of this could be attributed to the higher temperature ramp rates used during the DSC runs, which are often preferred to reduce noise in the measurements. By comparison, dilatometry has previously been shown to produce better data at lower ramp rates. Future work should further investigate the ideal ramp rate for both techniques to produce consistent results. Additional work should evaluate the best holder material to use for DSC runs exceeding 1,000°C to provide reliable data while preventing interactions between SiC and the holder.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Develop Accurate Techniques for Passive SiC Temperature Monitoring of Miniature Samples for Cross-Cutting Applications

Passive thermometry is critically important because most fuels and materials irradiation experiments are not instrumented, and it is necessary to understand the irradiation temperature to properly interpret any post-irradiation examination data, including evolving properties and/or microstructures. The standard passive thermometry approach uses continuous dilatometry to evaluate changes in the instantaneous coefficient of thermal expansion during post-irradiation thermal annealing. This approach has limitations in terms of sample size (minimum length requirements) and the maximum irradiation temperature that can be accurately determined, which is limited by the reduced swelling (and therefore recovery) following higher temperature irradiation and limitations on the furnaces used with push-rod dilatometers. This work evaluates two new proposed techniques for post-irradiation evaluation of passive SiC temperature monitors: differential scanning calorimetry (DSC) and Raman spectroscopy. DSC is an extremely sensitive technique that can be used for any specimen geometry and is capable of higher temperature operation. Raman spectroscopy is similar in that it is a surface technique capable of examining extremely small samples (submillimeter), can be used with a heated stage up to 1,500°C (planned for future work), and is capable of mapping local irradiation temperatures throughout a sample. Existing SiC samples that were previously irradiated over a wide range of temperatures were cut into multiple pieces to allow for annealing studies using multiple different techniques: dilatometry, DSC, and Raman spectroscopy. This approach mitigates the concern that samples analyzed using one technique may have a slightly different irradiation history than those analyzed using a different technique. Recovery was clearly observed during annealing using both DSC and dilatometry. In some cases, a direct comparison could not be made due to some of the DSC runs accidentally including material from multiple specimens and issues with using an alternative DSC sample holder for the highest temperature annealing studies. Nevertheless, one trend was clear: the DSC runs resulted in higher irradiation temperatures compared to those of the dilatometry runs. Part of this could be attributed to the higher temperature ramp rates used during the DSC runs, which are often preferred to reduce noise in the measurements. By comparison, dilatometry has previously been shown to produce better data at lower ramp rates. Future work should further investigate the ideal ramp rate for both techniques to produce consistent results. Additional work should evaluate the best holder material to use for DSC runs exceeding 1,000°C to provide reliable data while preventing interactions between SiC and the holder.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Contribution of Lobe Power to Experiment Heating in the Advanced Test Reactor

In order to ease the computational burden associated with designing irradiation experiments in the Advanced Test Reactor (ATR), scaling factors are often used to estimate design parameters at different lobe powers. Here, this paper examines the validity of long-standing assumptions about the contribution of lobe power to total experiment heating in the ATR. For each of the ATR’s 77 different experiment positions, the fractional contribution of each of the ATR’s five lobes to the total heating in that position is calculated and compared to traditional assumptions. The updated fractional contributions are then used to scale heating rates in a sample problem, and the results are compared to traditional scaling methods as well as explicit MC21 heating calculations. It is concluded that for experiment locations in close proximity to the ATR driver fuel (i.e. flux traps and the A, H, and B positions), heating rates scaled with the updated fractional contributions generally agree better with explicit MC21 calculations than do heating rates scaled using the traditionally assumed contributions. For the I positions, which are located on the very periphery of the ATR core, both scaling methods led to poor results when compared against explicit calculations due to the effect that movement of the outer shim control cylinders has on the experiment heating in those positions.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

The Effect of Radiation Damage on the Charge Collection Efficiency of Silicon Avalanche Photodiodes

Understanding radiation effects on avalanche photodiodes (APDs) is important because they are used in several applications involving harsh radiation environments. APDs are used as photosensors in applications where speed and detection efficiency are critical. Proton irradiation experiments on a commercial off-the-shelf APD demonstrated that the irradiation flux and applied reverse bias have a strong influence on the severity of radiation effects. This is measured using the ion beam induced charge (IBIC) technique in which charge collection efficiency (CCE) describes the signal response from a device. CCE can degrade substantially due to radiation damage, but recent measurements show that certain combinations of irradiation flux and reverse bias can lead to increases in CCE up to 186% ± 24% for irradiations with 2 MeV protons at a fluence of 6.4 × 10 11 cm –2 . This defect-enhanced charge multiplication (DECM) only appeared when the reverse bias during irradiation ranged from 170 to 1830 V out of a maximum operating bias of 2000 V and the proton flux ranged from 9.8 × 10 7 to 3.4 × 10 9 cm –2 s –1 . Furthermore values outside of either range led to losses in CCE. It is expected that DECM should be encountered in other devices, especially those with sufficiently high electric fields to cause impact ionization.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Accident Tolerant Fuel Test 2B (ATF-2B) Irradiation Test Report

A fully prototypic testing platform for testing new accident tolerant fuel (ATF) designs for light water reactors has been established in the center flux trap of Idaho National Laboratory’s advanced test reactor (ATR). The irradiation experiment named ATF-2 has completed 7 cycles of prototypic steady state irradiation irradiating 41 test pins to burnups as high as 30 MWd/kgU. Irradiation conditions have been maintained via the loop 2a pressurized water coolant loop and have been monitored through in-situ instrumentation during each cycle. Power and fast neutron flux histories of each of the 41 test pins has been calculated using a combined MCNP, and ORIGIN methodology to provide accurate and reliable power histories on a per pin basis.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

AGR-5/6/7 Irradiation Disassembly and Metrology First Look

The Advanced Gas Reactor (AGR) Fuel Development and Qualification Program was established to perform research and development on tristructural isotropic (TRISO)-coated particle fuel to support deployment of high-temperature gas-cooled reactors (HTGRs), which are graphite-moderated nuclear reactors cooled with helium. This work continues as part of the Advanced Reactor Technologies (ART) TRISO Fuel Program. The overarching program goal is to provide a baseline fuel qualification data set to support licensing, deployment, and operation of HTGRs in the United States. To achieve these goals, the program includes fuel fabrication, irradiations of TRISO fuels and high-temperature materials (e.g., graphite), safety testing and post-irradiation examination (PIE), fuel performance modeling, and fission product transport and source term determination. The ART AGR program has conducted four distinct fuel irradiation experiments in the Advanced Test Reactor (ATR) at Idaho National Laboratory (INL). The first of these irradiation tests, designated AGR-1, began in ATR in December of 2006 and ended in November 2009. This experiment was primarily to act as a shakedown test of the multi-capsule test train design and to provide early data on fuel performance that would be used in fuel fabrication process development. AGR-1 fuel kernels were produced on an engineering scale, but the TRISO coatings and cylindrical fuel compacts were fabricated on a laboratory scale. The AGR-1 PIE was completed and the final report was published in 2015. The second irradiation test, AGR-2, started in ATR in June 2010 and ended in October 2013. The AGR-2 irradiation test was designed to provide fuel performance data for coated particles fabricated on an engineering-scale pilot line using a coater with an internal chamber diameter of 150 mm (6 in.). The final PIE report was published in 2021. AGR-3/4, a single irradiation that combined what were originally conceived as the third and fourth tests, was to support the refinement of fission product transport models and to assess the effects of sweep gas impurities on fuel performance and fission product transport. PIE of the AGR-3/4 experiment is still in progress as of this writing. The subject of this report is AGR-5/6/7, the final qualification test of AGR TRISO fuel made entirely at the engineering scale.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

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↗

Ta–Zr carbides: Synthesis advances via carbothermal reduction and defect evolution observed through transmission electron microscopy ion irradiation

The thermodynamic stability of six distinct compositions within the Zr—Ta—C ternary system is investigated in this study, marking the first report of their synthesis through carbothermic reduction in vacuum. A prolonged annealing process at 2200°C enabled high densification and phase equilibrium. Detailed phase identification and microstructural characterization through microscopy and X-ray diffraction techniques revealed clear compositional trends and stable phase formations. Two compositions ((Ta 0.2 Zr 0.8 )C 0.6 and (Ta 0.5 Zr 0.5 )C 1 ) were selected for ion irradiation experiments using 200 keV Kr + at 600°C—representing the first-ever irradiation study on the Zr—Ta—C system. The findings indicated defect accumulation and nanoscale cavity formation without any evidence of amorphization, highlighting the system's structural stability under irradiation. Together, the synthesis and irradiation results provide a basis for further investigation of the system and suggest its relevance for applications under extreme environments.

36 MATERIALS SCIENCE↗

Recent progress on understanding the temperature-dependent irradiation resistance ranking among NiFe, NiCoCr, and NiCoFeCr alloys: A review

Systematic temperature-effects investigations on damage evolution in ion-irradiated Ni-based concentrated solid-solution alloys (CSAs) are pivotal to provide reliance on their use in nuclear applications. Here, in search of the origin behind the temperature-dependent irradiation resistance ranking among equiatomic NiFe, NiCoCr and NiCoFeCr alloys, we have compared, previously experimental and theoretical published data involving ion irradiation experiments performed on these alloys with new ion channeling results from ion-irradiated NiCoFeCr at 500 K. Moreover, the current results are compared with independent theoretical calculations and relevant TEM results from literature, which allow us to suggest that the lower migration energy of vacancies in NiCoCr, as compared with those in NiFe and NiCoFeCr, is the reason behind why NiCoCr is no longer outperforming NiFe under ion irradiation above 300 K.

99 GENERAL AND MISCELLANEOUS↗

Irradiation Testing of Nuclear Flux Sensors - Presentation for 2021 ASI Annual Webinar

This power point presentation is a summary of the work produced in FY2021 under the Irradiation Testing of Neutron Flux Sensors project funded by DOE's Advanced Sensor Initiative, and the outlook for FY22. The objective of this portion of the ASI program is to "Test and demonstrate in-pile instrumentation in conditions similar to those expected to be seen in service, i.e., the conditions they would see in either in irradiation experiments supporting advanced reactors, or ultimately, in advanced reactors themselves". The presentation describes how neutron flux sensors were tested in four INL reactors plus Idaho State University's research reactor during FY2021, and the results obtained from these tests.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Irradiation-induced swelling of pure chromium with 5 MeV Fe ions in the temperature range 450–650 °C

A surface coating using pure chromium has been proposed to increase the accident tolerance of Zircaloy cladding in pressurized water reactors. However, there is not much irradiation experience with Cr alloys and especially pure Cr. In the present study, pure chromium was irradiated with 5 MeV Fe ions to 50 peak dpa (displacements per atom) at temperatures of 450, 500, 550, 600 and 650 °C. Then irradiation at the peak swelling temperature of 550 °C was conducted to 50, 100, 150 peak dpa. Swelling at 50 dpa was observed over the entire temperature range studied, 450–650 °C, but appeared to be decreasing strongly at the temperature boundaries of the experiment. After an initial transient of rapid swelling, chromium was observed to swell at a rate of ~0.03–0.04%/dpa (up to 120 local dpa), which is much lower than pure Fe at 0.2%/dpa. This low swelling rate was found to be relatively insensitive to dpa rate, which varied by a factor of ~2 over the depth of data collection. Here, swelling was observed to begin quickly with an incubation period less than 10 dpa. Self-organization in the form of void ordering was observed to be developing at 50 dpa, becoming better defined with increasing dose. The void alignment direction is determined to be the $\langle$111$\rangle$ axial direction.

36 MATERIALS SCIENCE↗