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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↗

Acceptance Test Data for the AGR-5/6/7 Irradiation Test Fuel Composite Defective IPyC Fraction and Pyrocarbon Anisotropy

Coated particle composite J52R-16-98005 was produced by Babcock and Wilcox Technologies (BWXT) as fuel for the Advanced Gas Reactor Fuel Development and Qualification (AGR) Program’s AGR-5/6/7 irradiation test in the Idaho National Laboratory (INL) Advanced Test Reactor (ATR). This composite was comprised of four coated particle fuel batches J52O-16-93165B (26%), 93168B (26%), 93169B (24%), and 93170B (24%), chosen based on the Quality Control (QC) data acquired for each individual candidate AGR-5/6/7 batch. Each batch was coated in a 150-mm-diameter production-scale fluidized-bed chemical vapor deposition (CVD) furnace. Tristructural isotropic (TRISO) coatings were deposited on 425-μm-nominal-diameter spherical kernels from BWXT Lot J52R-16-69317 containing a mixture of 15.5%-enriched uranium carbide and uranium oxide (UCO). The TRISO coatings consisted of four consecutive CVD layers: a ~50% dense carbon buffer layer with 100-μm-nominal thickness, a dense inner pyrolytic carbon (IPyC) layer with 40-μm-nominal thickness, a silicon carbide (SiC) layer with 35-μm-nominal thickness, and a dense outer pyrolytic carbon (OPyC) layer with 40-μm-nominal thickness. The TRISO-coated particle batches were sieved to upgrade the particles by removing over-sized and under-sized material, and the upgraded batches were designated by appending the letter A to the end of the batch number (e.g., 93165A). Secondary upgrading by sieving was performed on the A-designated batches to remove particles with missing or very-thin buffer layers that were identified during previous analysis of the individual batches for defective IPyC, as reported in the acceptance test data report for the AGR-5/6/7 production batches [Hunn et al. 2017]. The additionally-upgraded batches were designated by appending the letter B to the end of the batch number (e.g., 93165B).

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Confirmatory LBL Analysis of AGR-5/6/7 Compacts and Over-Coated Particles BWXT Batches 11034, 14154C, 14156C, AND 14156D

Fuel for the Advanced Gas Reactor Fuel Development and Qualification (AGR) Program’s AGR-5/6/7 irradiation test in the Idaho National Laboratory (INL) Advanced Test Reactor (ATR) was produced by BWX Technologies (BWXT) Nuclear Operations Group in Lynchburg, Virginia. Tristructural isotropic (TRISO) coatings were deposited using a 150-mm-diameter production-scale fluidized-bed chemical vapor deposition (CVD) furnace on 425-μm-nominal-diameter spherical kernels from Lot J52R-16-69317 containing a mixture of 15.5% 235U low-enriched uranium carbide and uranium oxide (UCO). The TRISO coatings consisted of four consecutive CVD layers: a ~50% dense carbon buffer layer with 100-μmnominal thickness, a dense inner pyrolytic carbon (IPyC) layer with 40-μm-nominal thickness, a silicon carbide (SiC) layer with 35-μm-nominal thickness, and a dense outer pyrolytic carbon (OPyC) layer with 40-μm-nominal thickness. TRISO-coated particle Lot J52R-16-98005 was over-coated with a graphite/resin blend and these over-coated particles were pressed in half-inch-diameter, one-inch-long cylindrical compacts. Two packing fractions (PF) were produced, 40%PF and 25%PF, where the TRISO particle volume made up approximately 40% and 25% of the total compact volume, respectively. The AGR-5/6/7 Fuel Specification, SPC-1352 [Marshall 2016], provides the requirements necessary for acceptance of the fuel manufactured for the AGR-5/6/7 irradiation test. Quality control (QC) acceptance testing for all AGR-5/6/7 composited lots and single batches was performed by BWXT, with the exception of pyrolytic carbon (PyC) anisotropy and defective IPyC fraction in the TRISO candidate batches and final composite, which were measured at the Oak Ridge National Laboratory (ORNL) and reported in ORNL/TM-2017/036 [Hunn et al. 2017] and ORNL/TM-2017/037 [Helmreich et al. 2017a].

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

AGR-1 Thermocouple Data Analysis

This report documents an effort to analyze measured and simulated data obtained in the Advanced Gas Reactor (AGR) fuel irradiation test program conducted in the INL's Advanced Test Reactor (ATR) to support the Next Generation Nuclear Plant (NGNP) R&D program. The work follows up on a previous study (Pham and Einerson, 2010), in which statistical analysis methods were applied for AGR-1 thermocouple data qualification. The present work exercises the idea that, while recognizing uncertainties inherent in physics and thermal simulations of the AGR-1 test, results of the numerical simulations can be used in combination with the statistical analysis methods to further improve qualification of measured data. Additionally, the combined analysis of measured and simulation data can generate insights about simulation model uncertainty that can be useful for model improvement. This report also describes an experimental control procedure to maintain fuel target temperature in the future AGR tests using regression relationships that include simulation results. The report is organized into four chapters. Chapter 1 introduces the AGR Fuel Development and Qualification program, AGR-1 test configuration and test procedure, overview of AGR-1 measured data, and overview of physics and thermal simulation, including modeling assumptions and uncertainties. A brief summary of statistical analysis methods developed in (Pham and Einerson 2010) for AGR-1 measured data qualification within NGNP Data Management and Analysis System (NDMAS) is also included for completeness. Chapters 2-3 describe and discuss cases, in which the combined use of experimental and simulation data is realized. A set of issues associated with measurement and modeling uncertainties resulted from the combined analysis are identified. This includes demonstration that such a combined analysis led to important insights for reducing uncertainty in presentation of AGR-1 measured data (Chapter 2) and interpretation of simulation results (Chapter 3). The statistics-based simulation-aided experimental control procedure described for the future AGR tests is developed and demonstrated in Chapter 4. The procedure for controlling the target fuel temperature (capsule peak or average) is based on regression functions of thermocouple readings and other relevant parameters and accounting for possible changes in both physical and thermal conditions and in instrument performance.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Evaluations of University of Wisconsin Silicon Carbide Temperature Monitors 300 LO and 400 LO B

Silicon carbide (SiC) temperature monitors 05R4-02-A KG1403 (300 LO) and 05R4-01-A KG1415 (400 LO B) were evaluated at the High Temperature Test Lab (HTTL) to determine their peak irradiation temperatures. HTTL measurements indicate that the peak irradiation temperature for the 300 LO monitor was 295 {+-} 20 °C and the peak irradiation temperature for the 400 LO B monitor was 294 {+-} 25 °C. Two silicon carbide (SiC) temperature monitors irradiated in the Advanced Test Reactor (ATR) were evaluated at the High Temperature Test Lab (HTTL) to determine their peak temperature during irradiation. These monitors were irradiated as part of the University of Wisconsin Pilot Project with a target dose of 3 dpa. Temperature monitors were fabricated from high density (3.203 g/cm 3 ) SiC manufactured by Rohm Haas with a nominal size of 12.5 mm x 1.0 mm x 0.75 mm (see Attachment A). Table 1 provides identification for each monitor with an expected peak irradiation temperature range based on preliminary thermal analysis (see Attachment B). Post irradiation calculations are planned to reduce uncertainties in these calculated temperatures. Since the early 1960s, SiC has been used as a post-irradiation temperature monitor. As noted in Reference 2, several researchers have observed that neutron irradiation induced lattice expansion of SiC annealed out when the post-irradiation annealing temperature exceeds the peak irradiation temperature. As noted in Reference 3, INL uses resistivity measurements to infer peak irradiation temperature from SiC monitors. Figure 1 depicts the equipment at the HTTL used to evaluate the SiC monitors. The SiC monitors are heated in the annealing furnace using isochronal temperature steps that, depending on customer needs, can range from 50 to 800 °C. This furnace is located under a ventilation hood within the stainless steel enclosure. The ventilation system is activated during heating so that any released vapors are vented through this system. Annealing temperatures are recorded using a National Institute of Standards and Technology (NIST) traceable thermocouple inserted into an alumina tube in the furnace. After each isochronal annealing, the specimens are placed in a specialized fixture located in the constant temperature chamber (maintained at 30 °C) for a minimum of 30 minutes. After the 30 minute wait time, each specimen's resistance is measured using the specialized fixture and a calibrated DC power analyzer. This report discusses the evaluation of the SiC monitors and presents the results. Testing was conducted in accordance with Reference 3. Sections 2 and 3 present the data collected for each monitor and provide interpretation of the data. Section 4 presents the evaluated temperature results.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

AGR-3/4 Irradiation Test Train Disassembly and Component Metrology First Look Report

The AGR-3/4 experiment was designed to study fission product transport within graphitic matrix material and nuclear-grade graphite. To this end, this experiment consisted of 12 capsules, each fueled with 4 compacts containing UCO TRISO particles as driver fuel and 20 UCO designed-to-fail (DTF) fuel particles in each compact. The DTF fuel was fabricated with a thin pyrocarbon layer which was intended to fail during irradiation and provide a source of fission products. These fission products could then migrate through the compact and into the surrounding concentric rings of graphitic matrix material and/or nuclear graphite. Through post-irradiation examination (PIE) of the rings (including physical sampling and gamma scanning) fission product concentration profiles within the rings can be determined. These data can be used to elucidate fission product transport parameters (e.g. diffusion coefficients within the test materials) which will be used to inform and refine models of fission product transport. After irradiation in the Advanced Test Reactor (ATR) had been completed in April 2014, the AGR-3/4 experiment was shipped to the Hot Fuel Examination Facility (HFEF) at the Materials and Fuels Complex (MFC) for inspection, disassembly, and metrology. The AGR-3/4 test train was received at MFC in two separate shipments between February and April 2015. Visual examinations of the test train exterior did not indicate dimensional distortion, and only two small discolored areas were observed at the bottom of Capsules 8 and 9. No corresponding discoloration was found on the inside of these capsules, however. Prior to disassembly, the two test train sections were subject to analysis via the Precision Gamma Scanner (PGS), which did not indicate that any gross fuel relocation had occurred. A series of specialized tools (including clamps, cutters, and drills) had been designed and fabricated in order to carry out test train disassembly and recovery of capsule components (graphite rings and fuel compacts). This equipment performed well for separating each capsule in the test train and extracting the capsule components. Only a few problems were encountered. In one case, the outermost ring (the sink ring) was cracked during removal of the capsule through tubes. Although the sink ring will be analyzed in order to obtain a mass balance of fission products in the experiment, these cracks do not pose a major concern because the sink ring will not be analyzed in detail to obtain the spatial distribution of fission products. In Capsules 4 and 5, the compacts could not be removed from the inner rings. Strategies for removing the compacts are being evaluated. Sampling the inner rings with the compacts in-place is also an option. Dimensional measurements were made on the compacts, inner rings, outer rings, and sink rings. The diameters of all compacts decreased by 0.5 to 2.0 %. Generally, the extent of diametric shrinkage increased linearly with increasing neutron fluence. Most compact lengths also decreased. Compact lengths decreased with increasing fluence, reaching maximum shrinkage of about 0.9 % at a fast fluence of 4.0x1025 n/m2 E > 0.18 MeV. Above this fluence, the extent of length shrinkage appeared to decrease with fluence, and two compacts from Capsule 7 were found to have slightly increased in length (< 0.1 %) after a fluence of 5.2x1025 n/m2.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

AGR-3/4 Irradiation Test Train Disassembly and Component Metrology First Look Report

The AGR-3/4 experiment was designed to study fission product transport within graphitic matrix material and nuclear-grade graphite. To this end, this experiment consisted of 12 capsules, each fueled with 4 compacts containing UCO TRISO particles as driver fuel and 20 UCO designed-to-fail (DTF) fuel particles in each compact. The DTF fuel was fabricated with a thin pyrocarbon layer which was intended to fail during irradiation and provide a source of fission products. These fission products could then migrate through the compact and into the surrounding concentric rings of graphitic matrix material and/or nuclear graphite. Through post-irradiation examination (PIE) of the rings (including physical sampling and gamma scanning) fission product concentration profiles within the rings can be determined. These data can be used to elucidate fission product transport parameters (e.g. diffusion coefficients within the test materials) which will be used to inform and refine models of fission product transport. After irradiation in the Advanced Test Reactor (ATR) had been completed in April 2014, the AGR-3/4 experiment was shipped to the Hot Fuel Examination Facility (HFEF) at the Materials and Fuels Complex (MFC) for inspection, disassembly, and metrology. The AGR-3/4 test train was received at MFC in two separate shipments between February and April 2015. Visual examinations of the test train exterior did not indicate dimensional distortion, and only two small discolored areas were observed at the bottom of Capsules 8 and 9. No corresponding discoloration was found on the inside of these capsules, however. Prior to disassembly, the two test train sections were subject to analysis via the Precision Gamma Scanner (PGS), which did not indicate that any gross fuel relocation had occurred. A series of specialized tools (including clamps, cutters, and drills) had been designed and fabricated in order to carry out test train disassembly and recovery of capsule components (graphite rings and fuel compacts). This equipment performed well for separating each capsule in the test train and extracting the capsule components. Only a few problems were encountered. In one case, the outermost ring (the sink ring) was cracked during removal of the capsule through tubes. Although the sink ring will be analyzed in order to obtain a mass balance of fission products in the experiment, these cracks do not pose a major concern because the sink ring will not be analyzed in detail to obtain the spatial distribution of fission products. In Capsules 4 and 5, the compacts could not be removed from the inner rings. Strategies for removing the compacts are being evaluated. Sampling the inner rings with the compacts in-place is also an option. Dimensional measurements were made on the compacts, inner rings, outer rings, and sink rings. The diameters of all compacts decreased by 0.5 to 2.0 %. Generally, the extent of diametric shrinkage increased linearly with increasing neutron fluence. Most compact lengths also decreased. Compact lengths decreased with increasing fluence, reaching maximum shrinkage of about 0.9 % at a fast fluence of 4.0x10 25 n/m 2 E > 0.18 MeV. Above this fluence, the extent of length shrinkage appeared to decrease with fluence, and two compacts from Capsule 7 were found to have slightly increased in length (< 0.1 %) after a fluence of 5.2x10 25 n/m 2 .

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Scaling Analysis of Vortex Shedding Frequency between In line Plates

The Global Threat Reduction initiative (GTRI) was established by the National Nuclear Security Administration (NNSA) in 2004. One of the highlights of the program is to convert research and test reactors at home and abroad from Highly Enriched Uranium (HEU) to Low Enriched Uranium (LEU) fuels. By switching directly from HEU to LEU, an LEU reactor produces fewer neutrons than an HEU reactor and in some cases; a direct switch from HEU to LEU results in the reactor being unable to achieve criticality. Under certain circumstances, criticality is achieved and the original neutron fluxes are restored with LEU fuel by adding more fuel elements to the core. Not all reactors, exemplified by the Advanced Test Reactor (ATR) at the Idaho National Lab (INL), have the luxury of simply adding more fuel to the core. In such cases, entirely new designs must be created and tested. The ATR utilizes plate type fuel. During the design and testing of the ATR fuel, vortex shedding was identified as potential source for experiment and fuel failure. For fuel conversion, elements must be tested in pile prior to the qualification of the new fuel design. For some test elements, the primary test plate is followed by a secondary handling plate. It is known that objects downstream influence the vortex shedding. While vortex shedding is an important and well-studied phenomenon, not only in the context of nuclear engineering, but in fields as diverse as aeronautical engineering and biology, there is a significant gap in the understanding of vortex shedding in regards to two bluff bodies in line direct line with one another. The study provides a scaling analysis of the frequency of vortex shedding for plates in line. The scaling analysis is then compared to numerical simulation of two in line plates. The study provided a scaling analysis and suggested parameter for determining the expected trends in the Strouhal number for a plate with some object downstream. The analysis made the consideration of differing length scales as the cause for a reduction in vortex shedding frequency as well as looked at the potential impact of boundary layer growth on vortex shedding for a flat plate. The comparison between the expected scaling and numerical data was less than ideal, but there are several potential causes. One of the biggest issues with the comparison is the uncertainty associated with the defect velocity. The frequency was well established in several cases, but the velocity was not always well established resulting in a larger uncertainty. In the cases where the velocity was near zero (i.e. b/d = 0.5), the uncertainty dominated since the corrected Strouhal number is divided by the defect velocity. The Reynolds numbers were not incredibly large, ranging from 350-1600. The low Reynolds numbers potentially undermine the principle assumption made in the scaling analysis, i.e. Reynolds number is negligibly small. Additionally, the exact definition of the 'reduced velocity' was never explicitly defined, merely inferred from the assumption that the x length scale and y length scale were in fact different. Another potential problem is the defect velocities in the lower Reynolds number cases were not much smaller than the free stream velocity. Further work needs to be done at higher Reynolds numbers and with more data points to ensure the assumptions made are valid as well as confirm the accuracy of the scaled relationship. (authors)

42 ENGINEERING↗

Production of LEU fully ceramic microencapsulated fuel for irradiation testing

The Advanced Fuels Campaign of the US DOE Fuel Cycle Research/Development program is currently engaged in production of FCM fuel for irradiation testing in the Advanced Test Reactor (ATR) at Idaho National Laboratory (INL). FCM fuel production is a serial process with 3 major steps namely kernel, TRISO, and compact production. The first step in the kernel process is production of air-dried UO{sub 3} gel spheres with suspended carbon particles. These spheres, roughly 2 mm in size, are then calcined to produce a mixture of UO{sub 2} and carbon. This calcination step may be performed in either argon, hydrogen, or mixtures of these gases. Once the calcination step is complete, temperature is increased (>1400 Celsius degrees) to convert this mixture to UO{sub 2} + UC{sub x}. Once dense oxide-carbide kernels are available, the inert environment is switched to a nitrogen containing one to facilitate carbothermic reduction of kernels and production of UN. Essentially, the oxygen and carbon in the oxide-carbide kernels react with one another to produce CO and are replaced with nitrogen inside the lattice. The TRISO step in fuel production is incorporation of a porous carbon buffer layer, a dense inner pyrolytic carbon layer (IPyC), a SiC layer, and finally and outer pyrolytic carbon layer (OPyC) onto the UN kernels. The coating layer deposition step is carried out inside a graphite furnace using a fluidized bed chemical vapor deposition (CVD) process. In essence, a mixture of reactant and inert gasses flow from the bottom through a bed of particles that are in turn fluidized by the gas stream. The particles undergo CVD and once a different coating layer is to be incorporated, the furnace temperature is adjusted and the reactant gases are changed. The final step in the series of fuel production activities is the consolidation of UN TRISO particles inside the SiC matrix to produce cylindrical pellets. It entails 3 critical areas: SiC powder mixing, over-coating of particles, and high-temperature densification. Optimal execution of the powder mixing step is vital to achieve a fully dense SiC matrix at the end of the process. The SiC matrix is consolidated using a special form of liquid phase sintering (LPS) involving nano-powder feedstock that is designated as the NITE process. The SiC nano-powder slurry is sprayed directly onto the particle surface using a piezoelectric nozzle. Once the over-coated particles are available, final consolidation step at high temperatures (1875 Celsius degrees) is carried out.

36 MATERIALS SCIENCE↗

Report on partially complete post-irradiation-examination of the INL samples

Ferritic-martensitic steels (NF616 and T91), and austenitic stainless steel 800H and its Grain Boundary Engineering (GBE)-treated version 800H-TMP (ThermoMechanical Processing) were irradiated in the Advanced Test Reactor (ATR) at Idaho National Laboratory (INL) and their microstructures and mechanical properties were characterized. Ferritic-martensitic steels were irradiated up to 8.16 dpa in the irradiation temperatures ranging from 241 °C to 447.5 °C. Selected 800H and 800H-TMP samples were also irradiated up to 9.12 dpa at 359°C to 431°C. Vickers hardness measurement, fractography, and microstructural characterization were performed on the selected samples in the LAMDA lab. Radiation-induced hardening of NF616 and T91 was observed in the hardness measurements which show ~37% to ~65% increases, depending on irradiation dose and irradiation temperature. Within the irradiation conditions studied in this work, samples with a higher dose had a higher hardness. All the tested alloy 800H and 800H-TMP in this work showed irradiation-hardening by ~96±7% to ~152±10%. Alloy 800HTMP tended to have slightly smaller irradiation-hardening than alloy 800H. The fractography of NF616 samples D2 (2.96 dpa at 291.5°C), D4 (5.91 dpa at 359°C), and D6 (8.16 dpa at 431°C) indicated loss of ductility with negligible necking for the sample D2, yet obvious ductile failure for samples D4 and D6. Fractography of alloy 800H samples N4 (7.27 dpa at 359°C), N5 (3.9 dpa at 451.5°C), and N6 (9.01 dpa at 431°C), and alloy 800H-TMP samples P4 (7.36 dpa at 359°C), P5 (3.95 dpa at 451.5°C), and P6 (9.12 dpa at 431°C) indicated that all samples failed in a ductile mode, with obvious necking. Dimples were observed where large Ti-containing particles were observed for the samples. TEM characterization was performed on alloy 800H (N4, N5, N6) and 800H-TMP (P4, P5 and P6). Accumulation of M23C6 precipitates at grain boundaries was observed in all samples, and the presence of Ti(C,N) precipitates at grain boundaries and in the matrix was observed in alloy 800H-TMP. M23C6 precipitates were found to have the cube-on-cube orientation relationship with the matrix. In addition, nanoscale Si-rich clusters were observed in the matrix of all samples. Atom probe tomography was conducted on the same samples, and their results are being analyzed to be integrated with the TEM results for a confident description of the clustering behavior. Due to the low irradiation temperature (up to 451.5°C), dislocation loops formed in all samples, with the density and the average size of dislocation loops in the order of 1022 – 1023 m-3 and 11.7 – 15.9 nm, respectively. The loop densities in alloy 800H were higher than that in alloy 800H-TMP under the same irradiation conditions. Further systematic data analyses, together with some complementary experiments, will be pursued for these samples to foster peer-reviewed journal article publications.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Nanoscale clustering and fission product segregation in irradiated annular U-10Zr fuel

Zirconium (Zr) is added to uranium (U) to improve the performance of metallic fuel for fast reactor applications. This study employs transmission electron microscopy (TEM) and atom probe tomography (APT) to investigate nanoscale clustering of U and Zr, as well as segregation of fission products (FPs), in annular U-10Zr (in weight) metallic fuel irradiated at the Advanced Test Reactor (ATR). The results reveal variations in the shape, size, and chemical composition of clusters at different radial locations within the irradiated fuel cross-section. Zr-rich clusters exhibit higher concentration of FPs compared to U-rich clusters, potentially due to the co-precipitation of Zr and FPs in the fuel matrix during cooling at the end-of-life. In conclusion, this work complements the study of fuel constituents and fission product distribution across multiple length scales in irradiated U-10Zr metallic fuel.

Atom probe tomography↗

Microstructure and mechanical behavior of neutron irradiated ultrafine grained ferritic steel

Neutron irradiation effects on ultra-fine grain (UFG) low carbon steel prepared by equal channel angular pressing (ECAP) has been examined. Counterpart samples with conventional grain (CG) sizes have been irradiated alongside with the UFG ones for comparison. Samples were irradiated in the Advanced Test Reactor (ATR) at Idaho National Laboratory (INL) to 1.24 dpa. Atom probe tomography revealed manganese, silicon-enriched clusters in both ECAP and CG steel after neutron irradiation. X-ray quantitative analysis showed that dislocation density in CG increased after irradiation. However, no significant change was observed in UFG steel revealing better radiation tolerance.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

FABRICATION OF URANIUM OXYCARBIDE KERNELS AND COMPACTS FOR HTR FUEL

As part of the program to demonstrate tristructural isotropic (TRISO)-coated fuel for the Next Generation Nuclear Plant (NGNP), Advanced Gas Reactor (AGR) fuel is being irradiation tested in the Advanced Test Reactor (ATR) at Idaho National Laboratory (INL). This testing has led to improved kernel fabrication techniques, the formation of TRISO fuel particles, and upgrades to the overcoating, compaction, and heat treatment processes. Combined, these improvements provide a fuel manufacturing process that meets the stringent requirements associated with testing in the AGR experimentation program. Researchers at Idaho National Laboratory (INL) are working in conjunction with a team from Babcock and Wilcox (B&W) and Oak Ridge National Laboratory (ORNL) to (a) improve the quality of uranium oxycarbide (UCO) fuel kernels, (b) deposit TRISO layers to produce a fuel that meets or exceeds the standard developed by German researches in the 1980s, and (c) develop a process to overcoat TRISO particles with the same matrix material, but applies it with water using equipment previously and successfully employed in the pharmaceutical industry. A primary goal of this work is to simplify the process, making it more robust and repeatable while relying less on operator technique than prior overcoating efforts. A secondary goal is to improve first-pass yields to greater than 95% through the use of established technology and equipment. In the first test, called “AGR-1,” graphite compacts containing approximately 300,000 coated particles were irradiated from December 2006 to November 2009. The AGR-1 fuel was designed to closely replicate many of the properties of German TRISO-coated particles, thought to be important for good fuel performance. No release of gaseous fission product, indicative of particle coating failure, was detected in the nearly 3-year irradiation to a peak burn up of 19.6% at a time-average temperature of 1038–1121°C. Before fabricating AGR-2 fuel, each fabrication process was improved and changed. Changes to the kernel fabrication process included replacing the carbon black powder feed with a surface-modified carbon slurry and shortening the sintering schedule. AGR-2 TRISO particles were produced in a 6-inch diameter coater using a charge size about 21-times that of the 2-inch diameter coater used to coat AGR-1 particles. The compacting process was changed to increase matrix density and throughput by increasing the temperature and pressure of pressing and using a different type of press. AGR-2 fuel began irradiation in the ATR in late spring 2010.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

An analysis of nuclear fuel burnup in the AGR-1 TRISO fuel experiment using gamma spectrometry, mass spectrometry, and computational simulation techniques

AGR 1 was the first in a series of experiments designed to test US TRISO fuel under high temperature gas-cooled reactor irradiation conditions. This experiment was irradiated in the Advanced Test Reactor (ATR) at Idaho National Laboratory (INL) and is currently undergoing post irradiation examination (PIE) at INL and Oak Ridge National Laboratory. One component of the AGR 1 PIE is the experimental evaluation of the burnup of the fuel by two separate techniques. Gamma spectrometry was used to non destructively evaluate the burnup of all 72 of the TRISO fuel compacts that comprised the AGR 1 experiment. Two methods for evaluating burnup by gamma spectrometry were developed, one based on the Cs 137 activity and the other based on the ratio of Cs 134 and Cs 137 activities. Burnup values determined from both methods compared well with the values predicted from simulations. The highest measured burnup was 20.1% FIMA for the direct method and 20.0% FIMA for the ratio method (compared to 19.56% FIMA from simulations). An advantage of the ratio method is that the burnup of the cylindrical fuel compacts can determined in small (2.5 mm) axial increments and an axial burnup profile can be produced. Destructive chemical analysis by inductively coupled mass spectrometry (ICP MS) was then performed on selected compacts that were representative of the expected range of fuel burnups in the experiment to compare with the burnup values determined by gamma spectrometry. The compacts analyzed by mass spectrometry had a burnup range of 19.3% FIMA to 10.7% FIMA. The mass spectrometry evaluation of burnup for the four compacts agreed well with the gamma spectrometry burnup evaluations and the expected burnup from simulation. For all four compacts analyzed by mass spectrometry, the maximum range in the three experimentally determined values and the predicted value was 6% or less. Furthermore, the results confirm the accuracy of the nondestructive burnup evaluation from gamma spectrometry for TRISO fuel compacts across a burnup range of approximately 10 to 20% FIMA and also validate the approach used in the physics simulation of the AGR 1 experiment.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Critical processes and parameters in the development of accident tolerant fuels drop-in capsule irradiation tests

The goal of the Accident Tolerant Fuel (ATF) program is to develop the next generation of Light Water Reactor (LWR) fuels with improved performance, reliability, and safety characteristics during normal operations and accident conditions and with reduced waste generation. An irradiation test series has been defined to assess the performance of proposed ATF concepts under normal LWR operating conditions. The Phase I ATF irradiation test series is planned to be performed as a series of drop-in capsule tests to be irradiated in the Advanced Test Reactor (ATR) operated by the Idaho National Laboratory (INL). Design, analysis, and fabrication processes for ATR drop-in capsule experiment preparation are presented in this paper to demonstrate the importance of special design considerations, parameter sensitivity analysis, and precise fabrication and inspection techniques for figure innovative materials used in ATF experiment assemblies. A Taylor Series Method sensitivity analysis approach was used to identify the most critical variables in cladding and rodlet stress, temperature, and pressure calculations for design analyses. The results showed that internal rodlet pressure calculations are most sensitive to the fission gas release rate uncertainty while temperature calculations are most sensitive to cladding I.D. and O.D. dimensional uncertainty. The analysis showed that stress calculations are most sensitive to rodlet internal pressure uncertainties, however the results also indicated that the inside radius, outside radius, and internal pressure were all magnified as they propagate through the stress equation. This study demonstrates the importance for ATF concept development teams to provide the fabricators as much information as possible about the material properties and behavior observed in prototype testing, mock-up fabrication and assembly, and chemical and mechanical testing of the materials that may have been performed in the concept development phase. Special handling, machining, welding, and inspection of materials, if known, should also be communicated to the experiment fabrication and inspection team.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

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↗

Advanced Autonomous Welding for Refabrication and Follow-On Testing of Previously Irradiated Nuclear Fuel

The performance of follow-on experiments using irradiated nuclear fuel at any point in its lifecycle is a critical step in understanding phenomena and behavior. Transient experiments with high-burnup fuel can deepen the understanding of fuel fragmentation, relocations, and dispersal under loss-of-coolant accidents. An advanced autonomous welding process to refabricate commercial fuel rods inside a hot cell was created and tested to enable flexible experiment approaches on fuels irradiated in commercial and test reactors. Irradiated light water reactor fuel test pins from experiments performed at the Advanced Test Reactor (ATR) at Idaho National Laboratory were used to demonstrate the refabrication process. The welding process was found to be sensitive to welding parameters but flexible such that multiple passes could be performed on the same location until a hermetic weld was obtained. The refabrication of rodlets and successful welds was also found to be sensitive to the preparation of the irradiated cladding and endcaps. Thorough defueling of the fuel at the weld location and proper sizing of the endcaps and backing material mitigated these issues. The use of strategically located heat sinks in contact with the cladding and endcap materials also increased welding and refabrication success. For this work, the test pins were sectioned to remove the original endcaps and fuel was removed from both ends of each rodlet. The reassembly of the rodlets was then completed in four steps, which included the press fitting of new endcaps, the circumferential welding of rodlet endcaps to the cladding, rodlet pressurization in a pressure chamber, and seal welding the rodlet under pressure. The integrity of the refabricated rodlets was then verified via helium leak checking inside a vacuum chamber. The advanced welding system is capable of refabricating rodlets up to 380 mm in length, and repressurizing them up to 15 500 kPa. The refabricated lengths of the rodlets used in this work ranged from 149 to 165 mm and the refabricated fuel stack heights ranged from 70.4 to 79.8 mm. Here, the rodlets were pressurized with argon to an average pressure of 3617 kPa, and the average leak rate after refabrication was 6.7 • 10 -8 cm 3 • s -1 .

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗