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Uranium nitride fuel fabrication for SP-100 reactors

Fuel pins of uranium mononitride clad in Nb-1 percent Zr were fabricated for irradiation tests in EBR-II. Laboratory scale process parameters to synthesize UN powders and fabricate UN pellets were developed. Uranium mononitride was prepared by converting UO2 to UN. Fuel pellets were prepared by communition of UN briquettes, uniaxial pressing, and high temperature sintering. Techniques for machining, cleaning, and welding Nb-1 percent Zr cladding components were developed. End caps were electron beam welded to the tubing. Helium back-fill holes were sealed with a laser weld.

Mason, Richard E.↗

Initial results from safety testing of US AGR-2 irradiation test fuel

Two cylindrical compacts containing tristructural isotropic (TRISO)-coated particles with kernels that contained a mixture of uranium carbide and uranium oxide (UCO) and two compacts with UO 2 -kernel TRISO particles have undergone 1600°C safety testing. These compacts were irradiated in the US Advanced Gas Reactor Fuel Development and Qualification Program's second irradiation test (AGR-2). The time-dependent releases of several radioisotopes ( 110m Ag, 134 Cs, 137 Cs, 154 Eu, 155 Eu, 90 Sr, and 85 Kr) were monitored while heating the fuel specimens to 1600°C in flowing helium for 300 h. The UCO compacts behaved similarly to previously reported 1600°C-safety-tested UCO compacts from the AGR-1 irradiation. No failed TRISO or failed SiC were detected (based on krypton and cesium release), and cesium release through intact SiC was very low. Release behavior of silver, europium, and strontium appeared to be dominated by inventory originally released through intact coating layers during irradiation but retained in the compact matrix until it was released during safety testing. Both UO 2 compacts exhibited cesium release from multiple particles whose SiC failed during the safety test. Europium and strontium release from these two UO 2 compacts appeared to be dominated by release from the particles with failed SiC. Silver release was characteristically like the release from the UCO compacts in that an initial release of the majority of silver trapped in the matrix occurred during ramping to 1600°C. However, additional silver release was observed later in the safety testing due to the UO 2 TRISO with failed SiC. Failure of the SiC layer in the UO 2 fuel appears to have been dominated by CO corrosion, as opposed to the palladium degradation observed in AGR-1 UCO fuel.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

AGR-2 Irradiation Test Final As-Run Report, Rev 3

This document presents the as run analysis of the AGR 2 irradiation experiment. AGR 2 is the second of the planned irradiations for the Advanced Gas Reactor (AGR) Fuel Development and Qualification Program. Funding for this program is provided by the U.S. Department of Energy as part of the Very High Temperature Reactor (VHTR) Technology Development Office (TDO) program. The objectives of the AGR 2 experiment are to: 1. Irradiate UCO (uranium oxycarbide) and UO2 (uranium dioxide) fuel produced in a large coater. Fuel attributes are based on results obtained from the AGR 1 test and other project activities. 2. Provide irradiated fuel samples for post irradiation experiment (PIE) and safety testing. 3. Support the development of an understanding of the relationship between fuel fabrication processes, fuel product properties, and irradiation performance.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

AGR-2 Irradiation Test Final As-Run Report (Revision 4)

This document presents the as run analysis of the AGR 2 irradiation experiment. AGR 2 is the second of the planned irradiations for the Advanced Gas Reactor (AGR) Fuel Development and Qualification Program. Funding for this program is provided by the U.S. Department of Energy as part of the Very High Temperature Reactor (VHTR) Technology Development Office (TDO) program. The objectives of the AGR 2 experiment are to: 1. Irradiate UCO (uranium oxycarbide) and UO2 (uranium dioxide) fuel produced in a large coater. Fuel attributes are based on results obtained from the AGR 1 test and other project activities. 2. Provide irradiated fuel samples for post irradiation experiment (PIE) and safety testing. 3. Support the development of an understanding of the relationship between fuel fabrication processes, fuel product properties, and irradiation performance.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

SCANAIR-BISON BENCHMARK ON CIP0-1 RIA TEST

In the frame of their research programs on fuel safety, the French “Institut de Radioprotection et de Sûreté Nucléaire” (IRSN) and the Idaho National Laboratory (INL) have developed respectively SCANAIR and BISON codes to describe the thermo-mechanical behavior of irradiated fuel rods during Reactivity Initiated Accidents (RIA) in LWR. A RIA, characterized by a very rapid increase of reactivity and power in some rods of the reactor, can be schematically represented in two main phases. First, the energy deposition leads to a rapid rise of the fuel temperature which induces thermal swelling of the fuel pellets. During this phase, the Pellet Clad Mechanical Interaction (PCMI) leads to clad deformation and potentially to failure depending on fuel enthalpy increase and on the level of clad embrittlement. After the PCMI phase, the increase of clad temperature can lead to the boiling crisis of the water surrounding the rod. During the film boiling phase, the clad to coolant heat transfer becomes very low and the clad can reach high temperature (>700°C). Depending on the internal gas pressure, the ductile clad can undergo large deformation and possible failure. The RIA codes have to predict properly these two phases of the transient in order to be used, in particular, to assess current fuel safety criteria but also to be able to predict the behavior of upcoming fuel (such as accident tolerant fuel). In this paper, codes computation comparison against experimental data obtained on CIP0-1 test is done for the first phase of the transient, the PCMI phase, in order to point out the strengths and weaknesses of the codes. The CIP0-1 experiment was performed with UO2 high burnup fuel in the CABRI sodium loop facility, at 280°C and low pressure (~3 bars) without boiling crisis and no failure of the fuel rod. The initial state of the rod calculated by irradiation codes are compared with measurements before the transient. Then global rod thermal behavior during the CIP0-1 test is assessed with the sodium coolant temperature measurements. The rod mechanical behavior is analyzed with the fuel and clad elongation and the clad residual hoop strain. Finally comparison of the fission gas behavior between codes is performed and compared to the measurements of the fission gas released in the experiment.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Phase-field simulations of fission gas bubbles in high burnup UO2 during steady-state and LOCA transient conditions

To improve the economics of commercial nuclear energy generation, U.S. utilities are currently seeking licensing approval to operate UO2 fuel to higher burnups. One significant safety issue that must be addressed to obtain approval is the potential for fine fragmentation/pulverization of the fuel during a loss-of-coolant accident (LOCA). It has been hypothesized this is caused by the rapid increase of pressure in fission gas bubbles in the high burnup region of the fuel. To better understand this phenomenon, a novel phase-field model of the fission gas bubble microstructure in UO2 has been developed and implemented in Idaho National Laboratory's Marmot application for phase-field simulation of nuclear materials. Simulations of bubble growth in the high burnup region during steady-state conditions showed that initially overpressurized bubbles decreased in pressure during growth, but still remained above equilibrium pressure. During a LOCA transient, simulations of bubbles in the high burnup region showed that bubble size did not change significantly, and the pressure increase due to the transient was calculated and passed to a phase-field model of fracture.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

AGR-2 Irradiation Test Final As-Run Report, Rev 2

This document presents the as-run analysis of the AGR-2 irradiation experiment. AGR-2 is the second of the planned irradiations for the Advanced Gas Reactor (AGR) Fuel Development and Qualification Program. Funding for this program is provided by the U.S. Department of Energy as part of the Very High Temperature Reactor (VHTR) Technical Development Office (TDO) program. The objectives of the AGR-2 experiment are to: (a) Irradiate UCO (uranium oxycarbide) and UO 2 (uranium dioxide) fuel produced in a large coater. Fuel attributes are based on results obtained from the AGR-1 test and other project activities. (b) Provide irradiated fuel samples for post-irradiation experiment (PIE) and safety testing. (c) Support the development of an understanding of the relationship between fuel fabrication processes, fuel product properties, and irradiation performance. The primary objective of the test was to irradiate both UCO and UO 2 TRISO (tri-structural isotropic) fuel produced from prototypic scale equipment to obtain normal operation and accident condition fuel performance data. The UCO compacts were subjected to a range of burnups and temperatures typical of anticipated prismatic reactor service conditions in three capsules. The test train also includes compacts containing UO 2 particles produced independently by the United States, South Africa, and France in three separate capsules. The range of burnups and temperatures in these capsules were typical of anticipated pebble bed reactor service conditions. The results discussed in this report pertain only to U.S. produced fuel. In order to achieve the test objectives, the AGR-2 experiment was irradiated in the B-12 position of the Advanced Test Reactor (ATR) at Idaho National Laboratory (INL) for a total irradiation duration of 559.2 effective full power days (EFPD). Irradiation began on June 22, 2010, and ended on October 16, 2013, spanning 12 ATR power cycles and approximately three and a half calendar years. The test contained six independently controlled and monitored capsules. Each U.S. capsule contained 12 compacts of either UCO or UO2 AGR coated fuel. No fuel particles failed during the AGR-2 irradiation. Final burnup values on a per compact basis ranged from 7.26 to 13.15% FIMA (fissions per initial heavy-metal atom) for UCO fuel, and 9.01 to 10.69% FIMA for UO 2 fuel, while fast fluence values ranged from 1.94 to 3.47 x 10 25 n/m 2 (E >0.18 MeV) for UCO fuel, and from 3.05 to 3.53 x 10 25 n/m 2 (E >0.18 MeV) for UO 2 fuel. Time-average volume-average (TAVA) temperatures on a capsule basis at the end of irradiation ranged from 987°C in Capsule 6 to 1296°C in Capsule 2 for UCO, and from 996 to 1062°C in UO 2 -fueled Capsule 3. By the end of the irradiation, all of the installed thermocouples (TCs) had failed. Fission product release-to-birth (R/B) ratios were quite low. In the UCO capsules, R/B values during the first three cycles were below 10 -6 with the exception of the hotter Capsule 2, in which the R/Bs reached 2 x 10 -6 . In the UO 2 capsule (Capsule 3), the R/B values during the first three cycles were below 10 -7 . R/B values for all following cycles are not reliable due to gas flow and cross talk issues.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

BISON Capability, Validation and Demonstration for Reactivity-Initiated Accidents

Reactivity Initiated Accidents (RIA) are design basis accidents that could have adverse impacts on the core coolability. In the unlikely event that sufficient reactivity is inserted into the reactor core by the ejected/dropped control rod, prompt energy deposition into the fuel can occur, which when sufficiently high can lead to fuel rod failure or, at large energy deposition levels, expulsion of UO2 fragments or molten UO2 material from the fuel rod. This results in a release of fission product and fuel into the coolant and has the potential to compromise core coolability and threatening the pressure boundary of the primary coolant system. The design basis RIA is one of the industry challenging problems that the CASL aimed to address; the CASL RIA Challenge Problem Charter [1] states, ?The Pressurized Water Reactor (PWR) Rod Ejection Accident (REA) and Boiling Water Reactor (BWR) Control Rod Drop Accident (CRDA) are postulated accidents with consequences that are important to nuclear safety (fuel rod integrity and core coolability). Currently each reload core design must be analyzed to meet regulatory acceptance criteria. The goal of CASLs ModSim capability for RIA is to model the event at a higher fidelity, with validation to existing tests, to better model the transient neutronics and the progression of the fuel and cladding thermal-mechanical behavior. These improved analytical capabilities can be used to better inform reload core design, limits on fuel assembly discharge burnup, restrictions on placement of fuel in the reactor, control rod insertion limits, operating margin, and performance sensitivities.? In support of that charter, BISON, the fuel performance code has been used to demonstrate the simulation of thermal-mechanical behavior of LWR fuels during a reactivity-initiated accident. The combination of mechanical, thermal, and thermal-hydraulic phenomena all present during an RIA makes a multi-physics code such as BISON a valuable tool for modeling these scenarios. This paper will highlight many of the activities associated with BISON relevant to reactivity-initiated accident capability development and validation efforts. These efforts have been performed under both CASL and the Nuclear Energy Advanced Modeling and Simulation (NEAMS) programs.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Analytical workflow dependence of experimental observables for uranium chemistries

In this work, we investigated how the sequencing of laboratory analytical methods used for chemical and morphological characterization influences analytical findings for particulate materials relevant to the nuclear fuel cycle, including UO2, U3O8, studtite (UO2O2·4H2O), and β-UO3, in the context of nuclear forensic analysis. Particles of each chemistry obtained from consistent production batches were exposed to Raman spectroscopy and scanning electron microscopy in varying orders to elucidate how the order in which the techniques are applied influences morphological and chemical observations as a function of particle size. The results indicate that particles from all four chemistries exposed to high-resolution electron imaging before Raman spectral analysis demonstrate optical vibrational spectral changes that reduce accurate interpretation of the underlying chemistry via Raman spectral analysis. We hypothesize that these changes are due to the thermal load of the electron beam imparted to the sample being unable to be dissipated by materials with poor thermal conduction properties. Results from this study will aid in determining best practices for forensic analysis procedures to reduce uncertainty in chemical determination of unknown particulate samples.

Manns, Rebecca [University of Nevada, Las Vegas]↗

UZrCN Synthesis via Arc Melting - A Novel Synthesis Study

The next generation of nuclear reactors for both power production and space nuclear propulsion require fuel that is more durable, thermally stable, and more thermally conductive to support rapid heat transfer. High temperature gas reactors (HTGR), advanced gas reactors (AGR), and space-based nuclear thermal propulsion (NTP) are advanced reactor concepts that require a fuel type that can withstand high temperatures (1000-2900K) and flow of corrosive gas coolants such as helium, hydrogen, and carbon dioxide. One fuel with the potential to meet these demanding requirements is uranium-zirconium-carbonitride (UZrCN). UZrCN has many favorable fuel qualities compared to other eligible fuel forms such as uranium dioxide (UO2) and uranium mononitride (UN) that could support the aforementioned reactor concepts. UZrCN has an exceptionally high operating temperature and thermal conductivity which are highly desirable to improve reactor economics and safety. It far exceeds the properties of UO2 which is the most common fuel form in the United States. UZrCN also surpasses UN in terms of thermal conductivity and operating temperature by eliminating the dissociation problem UN has at 1700K. UZrCN could improve gas reactor performance and enable NTP technologies; however, it is an under-researched fuel that lacks rigorous scientific study. In recent efforts by the Idaho National Laboratory, a variety of novel methods to produce this fuel composition have been explored. One such method is via arc melting of uranium, zirconium, and carbon under a nitrogen atmosphere. Alloy fabrication using arc melting has been utilized for close to 150 years now and is well-understood as a method for rapid alloy prototyping. This process will be used to perform in-situ nitriding to form UZrCN.

36 MATERIALS SCIENCE↗

UZrCN Formation via Arc Melting – A Novel Synthesis Study

The next generation of nuclear reactors for both power production and space nuclear propulsion require fuel that is more durable, thermally stable, and more thermally conductive to support rapid heat transfer. High temperature gas reactors (HTGR), advanced gas reactors (AGR), and space-based nuclear thermal propulsion (NTP) are advanced reactor concepts that require a fuel type that can withstand high temperatures (1000-2900K) and flow of corrosive gas coolants such as helium, hydrogen, and carbon dioxide. One fuel with the potential to meet these demanding requirements is uranium-zirconium-carbonitride (UZrCN). UZrCN has many favorable fuel qualities compared to other eligible fuel forms such as uranium dioxide (UO2) and uranium mononitride (UN) that could support the aforementioned reactor concepts. UZrCN has an exceptionally high operating temperature and thermal conductivity which are highly desirable to improve reactor economics and safety. It far exceeds the properties of UO2 which is the most common fuel form in the United States. UZrCN also surpasses UN in terms of thermal conductivity and operating temperature by eliminating the dissociation problem UN has at 1700K. UZrCN could improve gas reactor performance and enable NTP technologies; however, it is an under-researched fuel that lacks rigorous scientific study. In recent efforts by the Idaho National Laboratory, a variety of novel methods to produce this fuel composition have been explored. One such method is via arc melting of uranium, zirconium, and carbon under a nitrogen atmosphere. Alloy fabrication using arc melting has been utilized for close to 150 years now and is well-understood as a method for rapid alloy prototyping. This process will be used to perform in-situ nitriding to form UZrCN.

36 MATERIALS SCIENCE↗

Assembly Bowing Reactivity Calculation Methodology Applied to Lead Fast Reactor

Ducted assemblies bow during operation due to power and temperature gradients which can be influenced by operating flow rates. For fast spectrum cores using ducted assemblies, the bowing behavior follows that of the duct and because there are gaps between the ducts, the bowing can result in compaction or expansion of the active core. This local displacement can have a positive or negative impact and knowing the net effect during transients is important for system reactivity control. Keeping the net bowing reactivity worth low is possible with attentive placement of load pads above the active core and selecting load pad gap thicknesses that result in a desired behavior at standard operating conditions. This paper considers a Lead Fast Reactor (LFR) concept fueled by HALEU UO2 developed by Westinghouse Electric Company (WEC) and applies a workflow of Argonne-developed codes to estimate the core bowing reactivity worth. Using orifice flow rates grouped by assembly type, the net reactivity impact due to core assembly bowing for the LFR was found to be small and in line with other liquid metal fast reactors: +29/+32/+35 pcm, or about +$0.049/+$0.055/+$0.059, for BOEC/MOEC/EOEC, respectively.

bowing reactivity↗

Identifying microstructures susceptible to pulverization in commercially irradiated high burnup UO2 under LOCA conditions

High burnup fuel fragmentation (HBFF) has been a concern in the nuclear industry for many years. When UO2 reaches and exceeds pellet average burnups around 55 GWd/tU, microstructural changes in the fuel pellet begin to occur that render the pellet susceptible to fine fragmentation under loss-of-coolant accident (LOCA) conditions. During a LOCA event, the cladding balloons and bursts, potentially releasing part of these fine fuel fragments into the reactor pressure vessel. This process is known as fuel fragmentation, relocation, and dispersal (FFRD). Presently, the US nuclear industry is developing a safety basis for FFRD with the goal of increasing burnups and pressurized water reactor cycle lengths. Increased cycle lengths would push the burnup limits of the fuel rods past the known threshold for HBFF susceptibility. In this work, the microstructural impact on HBFF was investigated by comparing the microstructures of as-irradiated rod segments to their post-LOCA tested counterparts. This investigation found that varied operational histories result in different microstructural evolutions across the pellet radius, which impacts the fragmentation behavior and radial location of the fragmentation. It is noted that regions with a high bubble density and a high density of grain boundaries fragment under LOCA-relevant conditions. In addition to the fragmentation that has been previously reported at the periphery of the fuel, fragmentation was also noted in the dark zone toward the fuel center. Analysis of the power histories of the fuel samples suggests that the dark zone forms in the central regions of the pellet between temperatures of approximately 740 and 960 °C.

McKinney, Casey [ORNL] (ORCID:0000000335383614)↗

Phase-field simulations to inform nuclear fuel performance modeling

Software tools to simulate nuclear fuel performance at the engineering scale, such as Idaho National Laboratory (INL)’s BISON code, are increasingly relied upon in regulatory and economic decision-making. However, accurate results from these tools depends on the availability of materials parameters that are used as input. In recent years, atomistic and mesoscale simulation methods have emerged as a cost-effective, expedient means to obtain such input parameters. Phase-field simulations using INL’s Marmot application have been used to obtain microstructure-level parameters and to improve material models for fuel performance modeling using BISON. In this talk, recent examples of this process are given, including applications in UO2, U3Si2, and UZr fuel.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Advanced Pellet Cladding Interaction Modeling Using the US DOE CASL Fuel Performance Code: Peregrine

The US DOE’s Consortium for Advanced Simulation of LWRs (CASL) program has undertaken an effort to enhance and develop modeling and simulation tools for a virtual reactor application, including high fidelity neutronics, fluid flow/thermal hydraulics, and fuel and material behavior. The fuel performance analysis efforts aim to provide 3-dimensional capabilities for single and multiple rods to assess safety margins and the impact of plant operation and fuel rod design on the fuel thermomechanical- chemical behavior, including Pellet-Cladding Interaction (PCI) failures and CRUD-Induced Localized Corrosion (CILC) failures in PWRs. [1-3] The CASL fuel performance code, Peregrine, is an engineering scale code that is built upon the MOOSE/ELK/FOX computational FEM framework, which is also common to the fuel modeling framework, BISON [4,5]. Peregrine uses both 2-D and 3-D geometric fuel rod representations and contains a materials properties and fuel behavior model library for the UO2 and Zircaloy system common to PWR fuel derived from both open literature sources and the FALCON code [6]. The primary purpose of Peregrine is to accurately calculate the thermal, mechanical, and chemical processes active throughout a single fuel rod during operation in a reactor, for both steady state and off-normal conditions.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Advanced Pellet-Cladding Interaction Modeling using the US DOE CASL Fuel Performance Code: Peregrine

The US DOE’s Consortium for Advanced Simulation of LWRs (CASL) program has undertaken an effort to enhance and develop modeling and simulation tools for a virtual reactor application, including high fidelity neutronics, fluid flow/thermal hydraulics, and fuel and material behavior. The fuel performance analysis efforts aim to provide 3-dimensional capabilities for single and multiple rods to assess safety margins and the impact of plant operation and fuel rod design on the fuel thermo-mechanical-chemical behavior, including Pellet-Cladding Interaction (PCI) failures and CRUD-Induced Localized Corrosion (CILC) failures in PWRs. [1-3] The CASL fuel performance code, Peregrine, is an engineering scale code that is built upon the MOOSE/ELK/FOX computational FEM framework, which is also common to the fuel modeling framework, BISON [4,5]. Peregrine uses both 2-D and 3-D geometric fuel rod representations and contains a materials properties and fuel behavior model library for the UO2 and Zircaloy system common to PWR fuel derived from both open literature sources and the FALCON code [6]. The primary purpose of Peregrine is to accurately calculate the thermal, mechanical, and chemical processes active throughout a single fuel rod during operation in a reactor, for both steady state and off-normal conditions.

CASL, Consortium for Advanced Simulation of LWRs, ↗

Separate Effects Testing in TREAT for ATF Fuels

This work performed examinations on high burnup UO2 from commercial power plant with the intention of better understanding fission gas and fragmentation behavior. Fuel fragmentation, relocation, and dispersal (FFRD) is a major factor in fuel lifetime limits imposed on UO2 by regulators, both domestic and foreign, and is a major area of interest by industry groups (e.g., Electric Power Research Institute, [EPRI]). The characterization of the fuel focused on the differences in porosity between the high burnup (rim) zone, the dark (intermediate) zone, and center zones of the fuel as well as the fission gas content of each region. Work involved thermal treatments to analyze fission gas and high resolution microscopy techniques to investigate pore structure.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Mn-doped oxide nuclear fuel

A nuclear fuel includes uranium(IV) oxide (UO2) and manganese (Mn) as a dopant. The Mn dopant may be present in the fuel in an amount up to the solubility limit for Mn under a given set of conditions, for example, about 0.01 wt % to about 1 wt %. The nuclear fuel is substantially free of aluminum (Al). The nuclear fuel exhibits enhanced grain size development during sintering temperatures as low at 1400 K due to an increase in uranium sub-lattice vacancies induced by dissolution of the Mn dopant at interstitial defect sites. The Mn-doped nuclear fuel exhibits improved grain sizes at lower temperatures compared to Cr-, Al-, and undoped UO2, and therefore desirably exhibits lower fission gas release and higher plasticity, reducing the chances of fuel rod failure.

Cooper, Michael William Donald↗