SEARCH · Engineering Papers
Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.
Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.
UO2Ge crystallizes in the tetragonal I4_1/a space group. The structure is three-dimensional and consists of eight germanium molecules and one UO2 framework. In the UO2 framework, U is bonded in a 6-coordinate geometry to six equivalent O atoms. There are a spread of U–O bond distances ranging from 2.14–2.44 Å. O is bonded in a distorted trigonal non-coplanar geometry to three equivalent U atoms.
Abstract Kroupaite (IMA 2017-031), ideally KPb0.5[(UO2)8O4(OH)10]·10H2O, is a new uranyl-oxide hydroxylhydrate mineral found underground in the Svornost mine, Jáchymov, Czechia. Electron-probe micro-analysis (WDS) provided the empirical formula (K1.28Na0.07)Σ1.35(Pb0.23Cu0.14Ca0.05Bi0.03Co0.02Al0.01)Σ0.48 [(UO2)7.90(SO4)0.04O4.04(OH)10.00]·10H2O, on the basis of 40 O atoms apfu. Sheets in the crystal structure of kroupaite adopt the fourmarierite anion topology, and therefore kroupaite belongs to the schoepite-family of minerals with related structures differing in the interlayer composition and arrangement, and charge of the sheets. Uptake of dangerous radionuclides (90Sr or 135Cs) into the structure of kroupaite and other uranyl-oxide hydroxy-hydrate is evaluated based on crystal-chemical considerations and Voronoi-Dirichlet polyhedra measures. These calculations show the importance of these phases for the safe disposal of nuclear waste.
Cost module on LWR fuel fabrication to accompany the Advanced Fuel Cycle Cost Basis Report. In this update, we are adding detailed life cycle cost data and a calculated, levelized fabrication cost derived from a non-proprietary bottom-up estimate prepared in 1978 by Oak Ridge National Laboratory (ORNL) (Judkins and Olsen 1978a). In 2018, the 1978 ORNL estimate was escalated by SA&I authors to 2017 USD using factors that represent inflation, escalation above inflation typical of nuclear projects, and the effects of more stringent safety and environmental regulations. In this FY-21 document, the $/kgU results in 2017 USD from the unpublished 2018 interim study (Williams and Ganda 2018) can be escalated to 2020 USD using a factor of 1.052. The literature-based unit cost (or price) data from previous (2004–2017) AFC-CBRs are escalated to 2020 USD using factors from Chapter 8 of the main FY-21 AFC-CBR document. This data, in addition to the results of the updated bottom-up estimate, are used to define the “what-it-takes” (WIT) range for the unit fabrication costs for conventional ceramic UOX light-water reactor (LWR) fuel. This FY-23 document also includes calculated unit costs for accident-tolerant LWR fuels (ATFs) of three different types. Some of these fuels constitute a ceramic pelletized form with fuel meat uranium compounds other than UO2 (a.k.a.,. UOX), thus the change in the title of this module in which the word “UO2” is changed to “Uranium-based Ceramic.”
The relevance of multidimensional and porous crystalline materials to nuclear waste remediation and storage applications has motivated exploratory research focused on materials discovery of compounds, such as actinide mixed-oxoanion phases, which exhibit rich structural chemistry. The novel phase K1.8Na1.2[(UO2)BSi4O12] has been synthesized using hydrothermal methods, representing the first example of a uranyl borosilicate. The three-dimensional structure crystallizes in the orthorhombic space group Cmce with lattice parameters a = 15.5471(19) Å, b = 14.3403(17) Å, c = 11.7315(15) Å, and V = 2615.5(6) Å3, and is composed of UO6 octahedra linked by [BSi4O12]5− chains to form a [(UO2)BSi4O12]3− framework. The synthesis method, structure, results of Raman, IR, and X-ray absorption spectroscopy, and thermal stability are discussed.
The recent interest in advanced fuel forms that offer increased thermal conductivity and uranium density, as well as modifications (e.g., use of dopants or additives) to traditional UO2 fuel, necessitates a vehicle for performing high-throughput irradiation testing of these fuels before they can be safely deployed. This interest, combined with the recent decommissioning of the Halden Reactor, places a strong burden on the remaining test reactors to provide the scientific data needed to advance these fuels toward commercialization. Oak Ridge National Laboratory is actively working to alleviate some of this burden by commissioning a new “MiniFuel” test facility that will provide a vehicle for performing accelerated separate-effects irradiation testing of sub-sized nuclear fuel specimens. The small size of the fuel allows for a flexible irradiation vehicle capable of exploring a wide range of fuel performance variables within a reasonable time and cost. This paper describes the experiment facility, and the initial irradiation experiments being performed including uranium nitride (UN) kernels, coated tristructural-isotropic (TRISO) UN particles, doped and un-doped (reference) UO2 disks, U3Si2 disks, and fully ceramic microencapsulated (FCM) pellets with UN kernels and a SiC matrix. A focus is placed on the performance of miniature FCM pellets, which are being considered as the ultimate accident tolerant fuel for light water reactors. The experiments described in this paper will provide basic scientific data (e.g., swelling, fission gas release) regarding irradiation performance under well-characterized conditions.
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.
A method of forming a water resistant boundary on a fissile material for use in a water cooled nuclear reactor is described. The method comprises coating the fissile material, such as a pellet of U3Si2 and/or the grain boundaries, to a desired thickness with a suitable coating material, such as atomic layer deposition or a thermal spray process. The coating material may be any non-reactive material with a solubility at least as low as that of UO2. Exemplary coating materials include ZrSiO4, FeCrAl, Cr, Zr, Al—Cr, CrAl, ZrO2, CeO2, TiO2, SiO2, UO2, ZrB2, Na2O—B2O3—SiO2—Al2O3 glass, Al2O3, Cr2O3, carbon, and SiC, and combinations thereof. The water resistant layer may be overlayed with a burnable absorber layer, such as ZrB2 or B2O3—SiO2 glass.
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.
This work is being performed as part of the DOE NE Spent Fuel and Waste Science and Technology Campaign, Argillite and Crystalline Rock R&D work packages: SF-19AN01030101 and SF-19AN01030201. This document meets the milestone M4SF-19AN010301013 for Argillite R&D and the milestone M4SF-19AN010302013 for Crystalline R&D. The fuel matrix degradation (FMD) model calculates the degradation rate of spent UO2 fuel based on fundamental electrochemical theory and thermodynamics. The model provides the quantitative basis for radionuclide source term predictions in the generic disposal system analysis (GDSA) performance assessment (PA) model. The FMD model has been implemented in a manner that facilitates its integration with the GDSA-PA code and a preliminary, integrated FMD-GDSA model has been successfully tested (Jerden et al., 2017). The specific focus of on-going work is to accurately and quantitatively represent the generation of H2 in a breached waste package and its effect on the spent fuel degradation rate so that this key process can be accurately represented in PA models. It has been shown experimentally that millimolar concentrations of dissolved H2 in contact with spent fuel will inhibit oxidative dissolution and decrease the fuel degradation rates by as much as three orders of magnitude (e.g., Röllin et al., 2001, Ollila, 2008). This will lead to a significant decrease in the radionuclide source term values used in repository PA models. Sensitivity studies using the FMD model have shown that the dissolved H2 concentration is the dominant environmental variable affecting the UO2 spent fuel dissolution rate as long as a source of H2 persists in the breached waste package (Jerden et al., 2015). Therefore, on-going experimental and modeling efforts focus on H2 production, accumulation and interfacial reactions within a breached waste package. The anoxic corrosion of metallic engineering materials within a breached waste package will be the main source of H2 in crystalline and argillite rock repository systems. The most important H2-producing alloys present within a waste package include stainless steel, carbon steel, and aluminum alloys and the Zircaloy fuel cladding. A steel corrosion module was added to the FMD model to account for these H2 sources and couple the H2 generation rate with fuel degradation processes (Jerden et al., 2017). As discussed below, there is a need for experimental data from electrochemical corrosion tests to quantify the H2 generation rates due to the corrosion of these waste package alloys as a function of key environmental variables (Eh, pH, groundwater chemistry). This report presents results from series of electrochemical corrosion tests with materials present in waste packages that provide information needed to parameterize and validate the FMD model. The alloys tested include 316L stainless steel (316SS), AISI 4320 carbon steel (C-steel) and Zircaloy-4 fuel cladding (unirradiated). Potentiodynamic polarization and potentiostatic polarization tests were performed in buffer solutions at pH 4, 7 and 10 with NaCl concentrations of 0, 4 and 100 millimolar (mM). The potentiostatic tests were performed at voltages varying from 0.5 volts down to -0.66 volts, vs the standard hydrogen electrode (SHE), and all tests were performed at laboratory ambient temperatures (~22 °C). The corrosion rates measured during the electrochemical tests were used as direct input to a new FMD/in-package chemistry model that is being developed to provide accurate long-term spent fuel degradation rates as chemical conditions (Eh, pH, speciation) evolve within a breached waste package. This new model was developed by coupling the FMD model with the reactive transport code X1t, which is a module within the Geochemist’s Workbench (GWB) reaction path modeling code (Jerden et al., 2019). The reactive transport model consists of a 1D domain discretized with 21 reaction diffusion cells and includes a single waste packag
A prototype gamma-ray scanning system was designed to perform post-irradiation measurements of nuclear fuel at Idaho National Laboratory (INL). The system is composed of a coaxial high-purity germanium (HPGe) detector, a collimator, and mechanical positioning stages that translate the fuel sample across the front of the collimator. This paper documents the design process, modeling and the laboratory characterization performed to validate the system. The modeling of the system was done using the Monte Carlo N-Particle code with vendor-supplied design specifications, dimensional measurements, and x-ray radiographs of the HPGe detector. The characterization included measurements of calibrated radiation sources in different geometries, and calculations for absolute efficiency and dead time. Benchmark measurements were performed by scanning an irradiated fuel rodlet containing ten pellets of 4.9% enriched UO2 in zirconium alloy. These results were compared to simulated spectra to further help characterize the detector model. One goal of the system is to determine the number of fissions per gram of UO2 in the fuel; comparison of the results from this prototype system's assay of the irradiated fuel rodlet are in agreement with previously estimated results.
The Transient Reactor Test Facility (TREAT) at Idaho National Laboratory (INL) has been successfully restarted. A principal goal of restarting the reactor was to perform transient testing of Accident Tolerant Fuels (ATF), supporting their safe adoption by the commercial Light Water Reactor (LWR) fleet. This paper will describe the efforts underway at INL to conduct testing of ATF under Reactivity Initiated Accident (RIA) conditions in an inert helium atmosphere. Tests in an inert helium atmosphere capsule provide valuable information about initial deposition and distribution of energy in the nuclear fuel. Tests in an inert helium atmosphere are especially suited for ATF concepts where the thermophysical properties of the new fuel material differ from UO2 such as the U3Si2 fuel concept and other non-oxide materials. These tests are also useful for exploring the thermal mechanical interaction of pellets with cladding where the cladding mechanical properties do not change much with temperature such as Silicon Carbide Cladding. Tests with nominal dimensions will be used to determine how fresh fuel failure and core coolability limits of ATF pellet and cladding materials compare with that of standard LWR fuel made up of UO2 pellets and Zircaloy cladding. Tests with a reduced pellet cladding gap will be used as a preliminary indicator of any pellet cladding mechanical interaction (PCMI) vulnerabilities of the new fuel concepts. The materials, methods, and schedule for the ATF RIA tests will be discussed in the paper.
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.
A gamma-ray scanning system was designed to perform post-irradiation measurements of nuclear fuel at Idaho National Laboratory (INL). The system is composed of a coaxial high-purity germanium (HPGe) detector, a collimator, and mechanical positioning stages that translate the fuel sample across the front of the collimator. A Monte Carlo N-Particle code simulation of the system and the fuel were created with vendor-supplied design specifications, dimensional measurements, and x-ray radiographs of the HPGe detector as well as all available fuel specifications. Benchmark measurements were performed by scanning an irradiated fuel rodlet containing eight pellets of 0.74% enriched UO2 in zirconium alloy. This fuel rodlet was part of the Static Environment Rodlet Transient Test Apparatus (SERTTA) testing campaign in the Transient Reactor Test Facility (TREAT). These results were compared to simulated spectra to help characterize the detector model and establish fidelity. A goal of the system is to determine the number of fissions per gram of UO2 in the fuel. This paper documents the modeling of the system and the calculation of the number of fissions per gram along the axial length of the SERTTA-C rodlet.
A prototype gamma-ray scanning system was designed to perform post-irradiation measurements of nuclear fuel at Idaho National Laboratory (INL). The system is composed of a coaxial high-purity germanium (HPGe) detector, a collimator, and mechanical positioning stages that translate the fuel sample across the front of the collimator. This paper documents the design process, modeling and the laboratory characterization performed to validate the system. The modeling of the system was done using the Monte Carlo N-Particle code with vendor-supplied design specifications, dimensional measurements, and x-ray radiographs of the HPGe detector. The characterization included measurements of calibrated radiation sources in different geometries, and calculations for absolute efficiency and dead time. Benchmark measurements were performed by scanning an irradiated fuel rodlet containing ten pellets of 4.9% enriched UO2 in zirconium alloy. These results were compared to simulated spectra to further help characterize the detector model. One goal of the system is to determine the number of fissions per gram of UO2 in the fuel; comparison of the results from this prototype system's assay of the irradiated fuel rodlet are in agreement with previously estimated results.
Investigation of Uranyl Perchlorate Anion Complexes in the Gas Phase via Infrared Multiphoton Dissociation and Collision Induced Dissociation Brittany D. M. Hodges, Christopher A. Zarzana, JungSoo Kim, Jonathan Martens, and W. C. M. Berden Introduction (120 words max) Effects of electronic structure on chemical bonding and reactivity play critical roles shaping the chemical bonding and reactivity behaviors of heavy elements. Understanding the role of f electrons in bond formation between the actinide-series elements like uranium with other ligands is critical for solving technical challenges associated with these heavy elements, important to nuclear fuel cycles, efficient separations of rare earth metals, and understanding the chemistry of stored nuclear fuels and related environmental management sites. In this study, we further examine the interactions between uranyl and the perchlorate ion in order to understand the structures of these ions through the use of IRMPD. Here we report the IRMPD spectra of [UO2(ClO4)3]-, [UO3(ClO4)2]-, and a proposed transition state. Methods (120 word max) IRMPD spectra and CID spectra were acquired using a Bruker amaZon QIT/MS instrument at the Free-Electron Lasers for Infrared eXperiments (FELIX) laboratory at Radboud University. The FELIX QIT/MS is modified to allow for the high-intensity tunable IR beam from FELIX to be directed into the ion packet, resulting in multiphoton dissociation that is measured only when the IR frequency is in resonance with an adequately high absorption vibrational mode of the mass-selected complex. DFT geometry optimizations and frequency calculations using the Gaussian suite of programs were performed using B3LYP, TPSSh, and PBE0 level of theory with 6-31+G(d) basis for the O, C, H, and N atoms and the SDD basis set for U. The SDD basis set employs the Stuttgart/Dresden effective core potential. Preliminary Data or Plenary Speakers Abstract (300 words max) Metal ion clusters of uranyl perchlorate were formed via direct electrospray ionization. For each metal ligand complex of interest, the parent ion was isolated and collision induced dissociation fragmentation and Infrared Multiphoton Dissociation (IRMPD) fragmentation spectra were acquired. Results presented here are the first look at the IRMPD spectra of [UO3(ClO4)2]-, [UO2(ClO4)3]-. Structures were examined using Gaussian at different levels of theory B3LYP level of theory, TPPSh and PBE0 levels, to reflect the behaviors of uranium metal ligand complexes most accurately. In these structures, we identified an overlap between each of these uranyl stretches resulting in their largely being obscured by a perchlorate mode. The CID product spectra agree with similar structures reported by Groenewold for uranyl nitrate in 2006 (10.1021/ja058106n).
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.
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.
A gamma-ray scanning system was designed to perform post-irradiation measurements of nuclear fuel at Idaho National Laboratory (INL). The system is composed of a coaxial high-purity germanium (HPGe) detector, a collimator, and mechanical positioning stages that translate the fuel sample across the front of the collimator. A Monte Carlo N-Particle code simulation of the system and the fuel were created with vendor-supplied design specifications, dimensional measurements, and x-ray radiographs of the HPGe detector as well as all available fuel specifications. Benchmark measurements were performed by scanning an irradiated fuel rodlet containing eight pellets of 0.74% enriched UO2 in zirconium alloy. This fuel rodlet was part of the Environment Rodlet Transient Test Apparatus (SERTTA) testing campaign in the Transient Reactor Test Facility (TREAT). These results were compared to simulated spectra to help characterize the detector model and establish fidelity. One goal of the system is to determine the number of fissions per gram of UO2 in the fuel. This article documents the modeling, benchmarking measurements, and the calculated number of fissions per gram in the SERTTA-A rodlet which was previously irradiated at TREAT.