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Quality Assurance Program Plan for SFR Metallic Fuel Data Qualification

This document contains an evaluation of the applicability of the current Quality Assurance Standards from the American Society of Mechanical Engineers Standard NQA-1 (NQA-1) criteria and identifies and describes the quality assurance process(es) by which attributes of historical, analytical, and other data associated with sodium-cooled fast reactor [SFR] metallic fuel will be evaluated. This process is being instituted to facilitate validation of data to the extent that such data may be used to support future licensing efforts associated with advanced reactor designs. The initial data to be evaluated under this program were generated during the US Integral Fast Reactor program between 1984-1994, where the data include, but are not limited to, research and development data and associated documents, test plans and associated protocols, operations and test data, technical reports, and information associated with past United States Nuclear Regulatory Commission reviews of SFR designs. It is recognized that managing the data generated by large research and development projects presents a significant challenge for retaining data integrity and availability. American Society of Mechanical Engineers Standard NQA-1 (NQA-1) 2008/2009a provides appropriate requirements for this plan.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Quality Assurance Program Plan for SFR Metallic Fuel Data Qualification

This document contains an evaluation of the applicability of the current Quality Assurance Standards from the American Society of Mechanical Engineers Standard NQA-1 (NQA-1) criteria and identifies and describes the quality assurance process(es) by which attributes of historical, analytical, and other data associated with sodium-cooled fast reactor [SFR] metallic fuel will be evaluated. This process is being instituted to facilitate validation of data to the extent that such data may be used to support future licensing efforts associated with advanced reactor designs. The initial data to be evaluated under this program were generated during the US Integral Fast Reactor program between 1984-1994, where the data include, but are not limited to, research and development data and associated documents, test plans and associated protocols, operations and test data, technical reports, and information associated with past United States Nuclear Regulatory Commission reviews of SFR designs. It is recognized that managing the data generated by large research and development projects presents a significant challenge for retaining data integrity and availability. American Society of Mechanical Engineers Standard NQA-1 (NQA-1) 2008/2009a provides appropriate requirements for this plan.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Determining the effects of U/Pu ratio on subsolidus phase transitions in U-Pu-Zr metallic fuel alloys

Here, ternary alloys consisting primarily of uranium, plutonium, and zirconium (U-Pu-Zr) are among the leading candidate fuel systems considered for fast spectrum nuclear reactors. Despite historical operation data from the testing of U-Pu-Zr rods in the Experimental Breeder Reactor-II, considerable uncertainty about the evolution of phases and microstructure across the ternary composition space exists. Due to sluggish kinetics and other difficulties in handling metal actinide specimens, quantitative measurements of phase-transitions in U-Pu-Zr alloys remain sparse in scientific literature, with most investigators reporting either phase-transition temperatures or phase identification data, but not both from the same specimens. The purpose of this paper is to critically compare experimental and calculated phase transition data and correlate with the microstructure and phase characterization data of as-cast and annealed U-Pu-Zr alloys. Phase transition peaks were measured using differential scanning calorimetry in the subsolidus regions (723-948 K) of three ternary U-Pu-Zr alloys with the same zirconium concentration but various U/Pu ratios. Overlapping peaks were deconvoluted using a Frazier-Suzuki peak fitting algorithm, and the critical peak temperatures and enthalpies were calculated. In general, increasing concentrations of Pu were associated with enhanced thermal stability of the body-centered cubic γ phase upon both heating and cooling. Experimental phase transition temperatures in this study tended to agree well with the predictions of the established ternary phase diagrams and other reported phase transition temperatures in literature. Additionally, the TAF-ID thermodynamic database was used to calculate a U-Pu-40 at.% Zr pseudobinary diagram as well as ternary diagrams from 773 to 973 K. The equilibrium phase transition temperatures tended to be considerably lower than measured peak temperatures upon both heating and cooling. Recommendations for improving the quality of data in future U-Pu-Zr characterization studies are also discussed.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

An investigation of the phase behaviors for quaternary U-Nb/Mo-Ti-Zr metallic fuel alloys

We report quaternary fuel alloys containing U, Nb/Mo, Ti, and Zr are proposed as fuel candidates for sodium-cooled fast reactors (SFRs). In this work, two Nb-bearing alloys, i.e., U-NT5Z (U-2.5Nb-2.5Ti-5.0Zr in wt%) and U-NT7Z (U-1.5Nb-1.5Ti-7.0Zr in wt%), and two Mo-bearing alloys, i.e., U-MT5Z (U-2.5Mo-2.5Ti-5.0Zr in wt%) and U-MT7Z (U-1.5Mo-1.5Ti-7.0Zr in wt%) were characterized and compared. The characterization techniques were differential scanning calorimetry (DSC), X-ray powder diffraction (XRD), and scanning electron microscopy/energy dispersive X-ray spectroscopy (SEM/EDS). DSC was performed to obtain the transition behaviors, and XRD and SEM/EDS were applied for phase identification. The results were combined to obtain the solid-state phase transitions between 500 °C and 850 °C for the alloys. It is found that the Nb-bearing alloys comprise similar phase transition behaviors as the Mo-bearing alloys. The phase transitions in U-NT5Z are a →γ at 608 °C and U 2 Ti → γ at 627 °C, which are ~40 °C higher than that of U-MT5Z. The phase transition in U-NT7Z is a → γ at 645 °C, and is 23 °C higher than that of U-MT7Z.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Solid-state phase transitions of two quaternary metallic fuel alloys (U-2.5Mo-2.5Ti-5.0Zr and U-1.5Mo-1.5Ti-7.0Zr in wt. %)

This study focuses on the solid-state phase transitions of two quaternary fuel alloys for fast reactors: U-1.5Mo-1.5Ti-7.0Zr (U-MT7Z) and U-2.5Mo-2.5Ti-5.0Zr (U-MT5Z). Here, the phase transitions were determined by differential scanning calorimetry (DSC), X-ray powder diffraction (XRD), and scanning electron microscopy/energy dispersive X-ray spectroscopy (SEM/EDS). To identify the high temperature phases, the alloys were annealed at 873K, 948K, 1023K, and 1123K (all under 72 hours). Combining those characterizations, the phase transitions are determined. In U-MT7Z, there is one phase transition observed, and it is ascribed to α + U 2 Ti → γ transition. In U-MT5Z, two transitions are found. The first transition is α → γ, while the second is U 2 Ti → γ. The γ phase onset temperature of U-MT5Z is lower than that of U-MT7Z due to the higher Mo content.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Scoping Studies to ascertain the change in the phase transition temperature of metallic fuels

Microstructure evolution due to irradiation in a nuclear reactor can have a dramatic effect on material properties. A better understanding of this evolution is necessary for developing improved nuclear fuels and materials. In the current scoping study we evaluate the influence of irradiation induced defects on the recrystallization temperature of a single component fuel surrogate.

36 MATERIALS SCIENCE↗

Electrometallurgical Treatment of Used Sodium-Bonded Metal Fuels

This is a teaching presentation for the University of New Mexico, Radioactive Waste Management class. This is a senior/graduate level class. The presentation does not contains any OUO information. All information provided has been previously presented publicly.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Epsilon Metal: A Waste Form for Noble Metals from Used Nuclear Fuel

Epsilon metal (e-metal) is the metallic phase that forms as inclusions at the grain boundaries in the UO2 fuel during reactor operation. This metal is composed of Pd, Mo, Rh, Ru, and Tc. These metallic inclusions are insoluble in strong acid and remnants of these metallic inclusions have been found in the UO2 matrix that remains from the natural reactors in Gabon that were active 1.8 billion years ago, therefore e-metal should be an excellent waste form for the immobilization of the long-lived isotopes 107Pd (6.5 ? 106 a) and 99Tc (2.13 ? 105 a), with 99Tc being the isotope of interest for repository performance. Therefore, the chemical durability of this potential waste form is assessed in this study. Typically, corrosion rates for metallic materials are measured electrochemically because they are quick, inexpensive, and can reveal the mechanism by which a metal corrodes, at least initially. However, in a repository the waste form would be subjected to slowly flowing water without an applied electrical potential over long time periods. Therefore, the corrosion rates of e-metal specimens were measured with both electrochemical tests and the single-pass flow-through test (SPFT). Potentiodynamic and potentiostatic polarization results suggest that a thin passive film exists on the alloy surface, which seems to be responsible for its high corrosion resistance. Additionally, X-Ray photoelectron spectroscopic results suggest that Pd oxides are significantly enriched in the passive film Results from the SPFT show that the dissolution rates were weakly dependent on pH. Only Mo and Re were found in solution and were used for the calculation of the dissolution rates. In general, the electrochemically determined corrosion rates agree reasonably well with the initial dissolution rate measured with the SPFT test, but they are about one or two orders of magnitude higher than the steady state rates. The causes for this discrepancy are discussed.

epsilon-metal, nuclear waste form, corrosion, sing↗

Development and preliminary validation of a mechanistic multiscale model for fuel-cladding chemical interaction in metallic nuclear fuels

Despite decades of fuel rod material and design improvements, fuel-cladding chemical interaction (FCCI) remains the single-most lifetime-limiting behavior for modern metallic fuel rods. Constraining fuel lifetime increases operating costs, limiting the economic viability of commercializing metallic nuclear fuel technology. A mechanistic multiscale model utilizing the finite element method-based MARMOT and BISON codes was developed to more confidently predict cladding-side FCCI and its impact on fuel performance. The new BISON model incorporates mesoscale models for the effects of fuel microstructure evolution on the transport of wastage-inducing lanthanides through the fuel and for the kinetics of cladding wastage layer growth. The mesoscale models, in turn, build on lanthanide transport property data obtained from the atomistic scale. Preliminary validation studies using wastage thickness and cladding profilometry data from four fuel rods irradiated in Experimental Breeder Reactor II experiment X447 and one fuel rod from Fast Flux Test Facility experiment IFR1 show that the new model predicts cladding wastage and its effects on cladding deformation as well as existing empirical FCCI correlations. The new model is expected to aid in the design of new metallic fuel concepts, including fuel additives, cladding liners, and sodium-free annular fuel geometries. In conclusion, future work will focus on broader validation and refinement of the model’s treatment of different fuel alloys and cladding materials.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Direct utilization of gaseous fuels in metal supported solid oxide fuel cells

Direct utilization and internal reforming of gaseous fuels is investigated on symmetric-architecture metal supported solid oxide fuel cells (MS-SOFCs) with thin ceramic electrolyte and scaffold backbone layers, and low cost ferritic stainless steel supports on both sides. Infiltrated Pr-oxide and Ni/samarium-doped ceria catalysts are added to the cathode and anode electrodes, respectively. Initial performance and durability is evaluated for MS-SOFCs operating with natural gas, propane, ammonia, and dimethyl ether at 700 °C. Cells for natural gas and propane utilize a novel high entropy alloy (HEA) catalyst for internal reforming with performance and degradation rates similar to H 2 (0.5W cm -2 and ~12%/100 h). In conclusion, initial testing with sulfur shows reversible degradation for levels found in natural gas and irreversible degradation for higher levels found in commercial propane. Overall, MS-SOFCs show successful fuel flexibility.

08 HYDROGEN↗

Correlating Nanoscale Secondary Ion Mass Spectrometry and Atom Probe Tomography Analysis of Uranium Enrichment in Metallic Nuclear Fuel

Distribution and enrichment of 235U within nuclear fuels are essential to material performance and reactor safety. With the development of metallic U fuels, understanding 235U homogeneity has become increasingly important, however, it is difficult to map with high spatial, and mass resolution to analyze both matrix and secondary phase precipitates. Here, we analyze 235U enrichment in matrix and carbide phases in LEU-Mo via two chemical imaging modalities: nanoscale secondary ion mass spectrometry (nanoSIMS) and atom probe tomography (APT). NanoSIMS and APT provided consistent results, with no statistically significant difference between measured and nominal enrichment (19.75 % 235U).

U-10Mo, atom probe tomography, nanoscale secondary↗