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DOE OSTI2020

Requirements Description of the REBUS Software for the Versatile Test Reactor

This report presents the modeling and simulation capabilities of Argonne National Laboratory’s fuel cycle analysis code, the REactor BUrnup System (REBUS), that will be relied on for the VTR project. These capabilities will then be used to establish the set of REBUS verification tasks necessary to verify REBUS for usage on the VTR project. A similar path was followed for the DIF3D software where its’ requirements and verification tasks were established. REBUS has been maintained by Argonne since the early 1960s to support its reactor design mission. That software transitioned from the original REBUS to REBUS-2 in the mid 1970s and to REBUS-3 in the mid 1980s. Since then REBUS has gone through many revisions to the current REBUS-11. Note that this version numbering is consistent with the progression of DIF3D, the base flux solver that REBUS is built upon. The name REBUS refers to a pictorial based puzzle as the original developers were inspired by having to track thousands of unique fuel assemblies as they are inserted into the reactor, depleted, shuffled, discharged, and reprocessed.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2015

Viscosity Meaurement Technique for Metal Fuels

Metallic fuels have exceptional transient behavior, excellent thermal conductivity, and a more straightforward reprocessing path, which does not separate out pure plutonium from the process stream. Fabrication of fuel containing minor actinides and rare earth (RE) elements for irradiation tests, for instance, U-20Pu-3Am-2Np-1.0RE-15Zr samples at the Idaho National Laboratory, is generally done by melt casting in an inert atmosphere. For the design of a casting system and further scale up development, computational modeling of the casting process is needed to provide information on melt flow and solidification for process optimization. Therefore, there is a need for melt viscosity data, the most important melt property that controls the melt flow. The goal of the project was to develop a measurement technique that uses fully sealed melt sample with no Americium vapor loss to determine the viscosity of metallic melts and at temperatures relevant to the casting process. The specific objectives of the project were to: develop mathematical models to establish the principle of the measurement method, design and build a viscosity measurement prototype system based on the established principle, and calibrate the system and quantify the uncertainty range. The result of the project indicates that the oscillation cup technique is applicable for melt viscosity measurement. Detailed mathematical models of innovative sample ampoule designs were developed to not only determine melt viscosity, but also melt density under certain designs. Measurement uncertainties were analyzed and quantified. The result of this project can be used as the initial step toward the eventual goal of establishing a viscosity measurement system for radioactive melts.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2016

Present and future potential of krypton-85 for the detection of clandestine reprocessing plants for treaty verification

Burnup calculations are applied to determine the amount of krypton-85 that is produced during the irradiation of nuclear fuel. Since krypton-85 is most likely released into the atmosphere during reprocessing to separate plutonium, atmospheric transport modeling is used to calculate the worldwide distribution of krypton-85 concentrations stemming from emissions from declared reprocessing plants. Our results are the basis for scenarios in which emissions from clandestine reprocessing facilities have to be detected against various background levels. We conclude that today’s background imposes heavily on the ability to detect small and medium plutonium separation rates; only high separation rates of 1 SQ per week and higher have a chance to be detected with feasible outlay. A fixed network of monitoring stations seems too costly; instead the high number of samples that are required rather calls for mobile sampling procedures, where air samples are collected at random locations over the world and are analyzed in regional laboratories for their krypton-85 concentration. Furthermore, it is argued that krypton-85 emissions from declared reprocessing activities have to be significantly lowered to enable a worldwide verification of the absence of even smaller clandestine reprocessing. For each scenario the number of samples that have to be taken for probable detection is calculated.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2016

A Pebble-Bed Breed-and-Burn Reactor

The primary objective of this project is to use three-dimensional fuel shuffling in order to reduce the minimum peak radiation damage of ~550 dpa present Breed-and-Burn (B&B) fast nuclear reactor cores designs (they feature 2-D fuel shuffling) call for to as close as possible to the presently accepted value of 200 dpa thereby enabling earlier commercialization of B&B reactors which could make substantial contribution to energy sustainability and economic stability without need for fuel recycling. Another objective is increasing the average discharge burnup for the same peak discharge burnup thereby (1) increasing the fuel utilization of 2-D shuffled B&B reactors and (2) reducing the reprocessing capacity required to support a given capacity of FRs that are to recycle fuel.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

DOE OSTI2025

Actinide oxide dissolution in tributyl phosphate

An alternative to dissolving used nuclear fuel (UNF) in an acidic solution during reprocessing is direct dissolution in an organic solution, which would eliminate an aqueous dissolution step, decrease the amount of nitrate needed, and reduce the facility size. The flowsheet for this potentially less expensive alternative is first to voloxidize the UNF to remove fission product gases and form an oxide. After voloxidation, the UNF is then dissolved in an organic solution containing an extractant mixed with an aliphatic diluent and pre-equilibrated with nitric acid. The organic solution then goes through a solvent extraction process to recover the uranium and/or other desired radionuclides. This work qualitatively studied the dissolution of actinide oxides (UO2, NpO2, and PuO2) in tributyl phosphate using UV-Vis-NIR absorbance spectroscopy to ascertain dissolution behavior. Initial studies included material that is otherwise difficult to dissolve in only nitric acid, specifically CeO2, that is sometimes used as a dissolution surrogate for PuO2. This work confirmed that CeO2, NpO2, and PuO2 are difficult to dissolve in 30 vol% TBP-dodecane pre-equilibrated with 10 M HNO3 and will readily dissolve when co-precipitated with U (i.e., the mixed oxides U-Ce, U-Np, and U-Pu), surrogates for voloxidized nuclear fuel.

Gogolski, Jarrod [Savannah River National Laborato↗

DOE OSTI2019

La Hague STE2 Sludge Retrieval and Conditioning Strategy - 19229

About 9000 m{sup 2} of Long-Lived Intermediate Level Waste LL-ILW STE2 sludges have been generated by the reprocessing operations of UNGG and later UOx fuel in La Hague (UP2-400) and subsequent liquid effluent treatment. They were placed into a set of adjoining tanks, called the STE2 silos. Today, the STE2 Sludges have to be retrieved and conditioned for final disposal in the deep geological repository under development in France (Cigeo). To this end, since the early 2000's, different retrieval and conditioning scenarios have been evaluated. This paper tracks the history of the technical and non-technical key factors having led to the choice of the baseline scenario developed until the end of 2016, describes the technical achievements and makes a state-of the art of the current scenario consisting in retrieving and temporarily storing STE2 sludges and, meanwhile, studying, researching and testing final conditioning processes and technologies in the aim of achieving a technical and economic optimum. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2015

A two-dimensional, finite-difference model of the oxidation of a uranium carbide fuel pellet

The oxidation of spent uranium carbide fuel, a candidate fuel for Generation IV nuclear reactors, is an important process in its potential reprocessing cycle. However, the oxidation of uranium carbide in air is highly exothermic. A model has therefore been developed to predict the temperature rise, as well as other useful information such as reaction completion times, under different reaction conditions in order to help in deriving safe oxidation conditions. Finite difference-methods are used to model the heat and mass transfer processes occurring during the reaction in two dimensions and are coupled to kinetics found in the literature.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2024

Concepts for Actinide Recovery from TRISO Used Nuclear Fuel

The work described in this report has developed a preliminary conceptual flowsheet based on limited published literature for the head-end of a TRISO oxycarbide UNF reprocessing plant. The essential function of the head-end is to prepare the UNF for subsequent separation of actinides. The main steps of the conceptual TRISO UNF head-end reprocessing flowsheet are: 1. Fragmentation of the graphite moderator to expose the fuel particles. 2. Separation of fuel particles from fragmented graphite moderator by sieving and fluidization. 3. Fragmentation of the fuel particles to expose the fuel kernel. 4. Dissolution of the fuel kernel in nitric acid. Noteworthy at this step is the formation of organic acids (mainly oxalic and mellitic acids) from the carbon associated with the fuel and TRISO coatings. These acids can interfere with actinide separations and solvent extraction hydraulic performance and carbon dioxide gas generation. 5. Clarification of the dissolved fuel solution to separate the coating fragments. 6. Dissolver off-gas treatment with specific emphasis on managing generation of carbon dioxide gas containing carbon-14. The quantity of carbon dioxide is projected to be 100 to 1000 times greater than that arising from dissolving LWR UNF. Pre or post treatment of the exposed fuel kernels could be undertaken to mitigate the formation of organic acids but there still exists a significant off-gas treatment challenge. The literature on reprocessing uranium nitride UNF was reviewed but a flowsheet was not specifically developed since its scope and uncertainties are expected to be encompassed by the oxycarbide flowsheet. Overall, the predominant feature of processing TRISO UNF is carbon management to reduce waste volume and mitigate the formation of carbon dioxide and organic acids. This report recommends broad areas of research that will help to further define the head-end flowsheet.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2017

Effect of Moisture on the Adsorption of Iodine and Krypton in Multicomponent Streams on the 10 WT% C/ETS-10 Sorbent

Over 13% of the world's energy demand is supplied by nuclear power plants in 31 countries. This demand is growing; by 2030 the IAEA predicts a 100% increase in the demand for nuclear energy. The increase in nuclear energy production imposes a growing strain on the uranium fuel supply. At current consumption rates the world's supply of uranium is projected to last ∼200 years. With the growing energy consumption, uranium supplies will dwindle even more quickly. However, ∼95% of uranium is left in used nuclear fuel (UNF) and may be utilized through reprocessing. A main concern with reprocessing is the release of off-gas. The major constituents of off-gas include {sup 85}Kr, {sup 129}I, {sup 14}C, {sup 3}H, and various Xe isotopes. {sup 85}Kr and {sup 129}I present the largest threat due to their harmful environmental effects and abundance. Several methods have been studied for the removal of these contaminants, including cryogenic distillation, fluorocarbon absorption, wet scrubbing, and adsorption have been employed. Adsorption on porous solid sorbents has the advantages of being simple, effective, and economic. Thus many studies have been performed investigating several sorbents such as silver impregnated mordenite, silver Engelhard titanosilicate 10, chalcogen-based aerogels, and metal organic frameworks. Despite these advances, many of these studies have been conducted under ideal conditions: cryogenic temperature, helium as a carrier gas, and single component adsorption. The need for investigating adsorption under conditions more representative of practical use is needed. Thus our work has been devoted to the study of adsorption of {sup 85}Kr and {sup 129}I from a simulated off-gas on an Engelhard titanosilicate 10 (ETS-10) supported carbon nanopolyhedron sorbent (C/ETS-10) in a multicomponent system at ambient temperatures. Previously we have reported sorption capacities of C/ETS-10 for single component krypton, and iodine. The effects multi-contaminant iodine and krypton and their respective inlet concentrations on the sorption capacity of 10 wt% C/ETS-10 have also been studied. Investigations into the effect of the presence of moisture in the multicomponent gas mixture on the sorption on 10 wt% C/ETS-10 are described in this paper.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Griffin-m

Griffin-m is a MOOSE-based reactor multiphysics application that streamlines the analysis of a variety of nuclear multiphysics simulations, including steady-state and transient radiation transport, core performance, fuel depletion, criticality and decay heat calculations, reprocessing and post-irradiation examination. This streamlining is accomplished via enhanced flexibility of the tools, uniform syntax in the MOOSE framework, dynamic linking of all relevant physics and a single point of execution. The design for flexible multi-physics, multi-radiation, multi-scheme tasks demands and ultimately makes Griffin-m a highly extendable code system. A software quality assurance (SQA) procedure is enforced during Griffin-m development. The Griffin-m version will be the main production version and it includes the MCC3 code, which was originally developed at Argonne National Laboratory to prepare cross sections for fast reactors.

Ortensi, Javier [Idaho National Laboratory (INL), ↗

DOE OSTI2021

Griffin: A Moose-based Reactor Multiphysics Application For Radiation Transport And Depletion Simulations

Griffin is a MOOSE-based reactor multiphysics application that streamlines the analysis of a variety of nuclear multiphysics applications, including steady-state and transient radiation transport, core performance, fuel depletion, criticality and decay heat calculations, reprocessing and post-irradiation examination. This streamlining is accomplished via enhanced flexibility of the tools, uniform syntax in the MOOSE framework, dynamic linking of all relevant physics and a single point of execution. The design for flexible multi-physics, multi-radiation, multi-scheme tasks demands and ultimately makes Griffin a highly extendable code system. A software quality assurance (SQA) procedure is enforced during Griffin development.

DeHart, MarkD.↗

NASA NTRS2008

Mars Rocket Propulsion System

A report discusses the methane and carbon monoxide/LOX (McLOx) rocket for ascent from Mars as well as other critical space propulsion tasks. The system offers a specific impulse over 370 s roughly 50 s higher than existing space-storable bio-propellants. Current Mars in-situ propellant production (ISPP) technologies produce impure methane and carbon monoxide in various combinations. While separation and purification of methane fuel is possible, it adds complexity to the propellant production process and discards an otherwise useful fuel product. The McLOx makes such complex and wasteful processes unnecessary by burning the methane/CO mixtures produced by the Mars ISPP systems without the need for further refinement. Despite the decrease in rocket-specific impulse caused by the CO admixture, the improvement offered by concomitant increased propellant density can provide a net improvement in stage performance. One advantage is the increase of the total amount of propellant produced, but with a decrease in mass and complexity of the required ISPP plant. Methane/CO fuel mixtures also may be produced by reprocessing the organic wastes of a Moon base or a space station, making McLOx engines key for a human Lunar initiative or the International Space Station (ISS) program. Because McLOx propellant components store at a common temperature, very lightweight and compact common bulkhead tanks can be employed, improving overall stage performance further.

Zubrin, Robert↗

DOE OSTI2015

Cold crucible deployment in La Hague facility: the feedback from the first four years of operation - 15119

In April 2010, a Cold Crucible Induction Melter (CCIM) started hot operation for the first time ever in an existing very high active facility (R7) at La Hague. This was the culmination of more than two decades of R and D involving progressive process and technological development. The industrial deployment included extensive cleaning of the hot cell, removal of the previous melter, exchange of several mechanical and process components in the cell, and implementation of the various additional utilities and components necessary for operation of the new CCIM. The design and implementation phases for this deployment were described in a previous paper at WM. The CCIM has now been operated for more than four years, essentially processing active effluents from D and D operations and high-level liquid waste from reprocessed U-Mo-Sn-Al spent fuel. During this period, many data have been collected to confirm the process parameters that were defined during the qualification of this innovating process. Even if some difficulties occurred, the experience of the operating teams with the support of engineering and R and D allow managing them. This paper presents the start-up methodology and history of the cold crucible deployment in La Hague facility with the feedback from the first years of operation. The production records with the different liquid solutions treated in the process are itemized. The lessons learned during the first four years of operation of the CCIM are presented with the difficulties encountered and the solutions implemented, emphasizing the benefits of a close integration between RD, engineering, and operation teams. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2018

Vitrification Process for Idaho HLW Calcine - 18433

The majority of the liquid wastes produced from reprocessing of several types of spent nuclear fuel at the Department of energy's (DOE) Idaho site have been volume reduced by calcination. The resulting ∼155,600 ft{sup 3} of calcined waste is stored in 43 shielded stainless steel bins, which have a 500-year design life. The calcined material is both a high-level waste and a RCRA hazardous waste, which complicates treatment and disposal options. In addition to a potential direct disposal option, treatment options that have been considered include steam reforming, hot isostatic pressing (HIP), and vitrification. This paper describes testing and evaluation of a vitrification option for the calcine. Vitrification to produce a borosilicate glass has the advantage that it is the only treatment that provides a waste form that meets the current HLW repository waste acceptance criteria. It is therefore the lowest risk option in terms of regulatory and legislative concerns. The present work addressed several key questions: (i) Calcine waste loadings in glass, which determine the number of HLW canisters produced and the required glass production rate (throughput) for the system design; (ii) Melt rate per unit glass pool surface area of the melter, which determines the sizing of the vitrification system; and (iii) The ability to meet waste form acceptance requirements (PCT and TCLP) while achieving reasonable waste loadings. These are issues of fundamental importance to the sizing estimates for the unit operations and overall flow-sheet and they, therefore, directly impact the cost and schedule estimates. Fully compliant, high-waste-loading glasses were developed for two of the four Idaho calcine wastes. The results demonstrate that waste loadings of 35 wt% waste oxides are achievable for the two alumina calcines and about 30 wt% is achievable for the two zirconia calcines. Testing of these formulations in a joule-heated ceramic melter showed glass production rates of over 5000 kg/(m2/d) for the Alumina calcine and over 8500 kg/(m{sup 2}/d) for the Zirconium-Na Blend calcine. These extremely high production rates translate directly into smaller system size and shorter mission duration and, therefore, reduced costs. Based on these results, a preliminary design for the full-scale vitrification system was developed. The system consists of waste receipt, vitrification, off-gas treatment, and canister sealing and decontamination equipment. The calcine is blended with the appropriate glass forming chemicals (or glass frit) and fed to the melter as a solid stream. The melter has a glass pool surface area of about 2.5 m{sup 2} and is equipped with a bubbling system to increase processing rates. Glass production rates of about 6 metric tons per day are projected. The vitrification system would be installed into the existing Idaho Waste Treatment Unit Facility (IWTU) so that no new facilities are required to house the treatment system, thus greatly reducing overall cost, duration, and risk. The system would be designed to treat all of the calcine waste within a period of 12 years at an operating efficiency of 80%, producing a total of about 8500 canisters each weighing two metric tons. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2025

Exploring the influence of transition metals on f-element bonding

The United States aims to triple its nuclear energy production by 2050, which will result in increased uranium usage and spent nuclear fuel generation. This highlights the need for a comprehensive understanding of actinide coordination chemistry, which is crucial for the extraction, processing, purification, and fabrication of uranium-based fuels. Moreover, it is vital for the reprocessing or safe disposal of nuclear waste and effective remediation efforts. Achieving this successfully requires an in-depth understanding of f-electron behavior, as “the role of 5f electrons in bond formation remains a fundamental topic in actinide chemistry”. Introducing a second metal into the system can increase structural dimensionality and diversify structural architecture. Heterometallic systems can also alter material properties, such as magnetic and spectroscopic characteristics, luminescence, and actinide mobility. Additionally, secondary transition metals, even when present only in the second coordination sphere and not directly coordinated, can influence the electron density at the actinyl metal center. In this study, uranium heterometallic single crystals were synthesized by incorporating transition metals such as iron(III), iron(II), nickel(II), manganese(II), copper(I), and cobalt(II). The crystals were formed using 2,6-pyridine dicarboxylic acid and other structurally similar ligands with varying functional groups. The synthesized crystals were analyzed using an extensive array of analytical and computational characterization techniques, including single crystal X-ray diffraction, Raman and infrared spectroscopy, and density functional theory calculations.

37 - INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL C↗

DOE OSTI2019

DEHBA (di-2-ethylhexylbutyramide) gamma radiolysis under spent nuclear fuel solvent extraction process conditions

Di-2-ethylhexylbutyramide (DEHBA) has been presented as part of a hydro-reprocessing solvent extraction system for the co-extraction of uranium and plutonium from spent nuclear fuel. Yet, there remains a lack of quantitative understanding of the impact of chemical environment on the radiation chemistry of DEHBA, especially under conditions expected in real-world solvent extraction processes. Therefore, we have undertaken a systematic investigation into the radiolytic degradation of DEHBA in n-dodecane under fully aerated and biphasic conditions. DEHBA integrity and degradation product formation were measured for both extraction (in contact with 4.0 M HNO 3(aq) ) and stripping (in contact with 0.1 M HNO 3(aq) ) formulations. At the lower acidity the rate of DEHBA/n-dodecane degradation was slow (G = -0.26 ± 0.02 µM J -1 ) whereas at the higher acidity this degradation was about 35% faster (G = -0.35 ± 0.02 µM J-1). Both values were much less than analogous measurements under deaerated conditions. Under continuously aerated conditions, FTIR and ESI-MS measurements identified the two major degradation products, bis-2-ethylhexylamine (b2EHA) and N-(2-ethylhexyl)butyramide (MEHBA), as well as the presence of additional oxidized product species. Solvent system performance was also investigated using uranium extraction and strip distribution ratio measurements. These reports showed that there was only minimal change in uranium extraction and stripping performance with absorbed gamma dose.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

DOE OSTI2019

Researching the Effects of Long-Term Dry Storage on Commercial Spent Nuclear Fuel

When the fuel in a nuclear reactor no longer contributes efficiently to power production, it is discharged and stored onsite in a water-filled spent fuel pool. When nuclear power plants in the United States were originally designed, it was expected that onsite storage would be temporary. The used nuclear fuel, also known as spent nuclear fuel (SNF), was to be removed from the storage pools after only a few years of cooling and sent for reprocessing. However, commercial reprocessing was not implemented in the United States, and utility spent fuel pools began running out of room. In order to continue power production, nuclear utilities began expanding onsite fuel storage capacities, first by increasing the density of fuel in the fuel pool racks, and then by developing and implementing dry storage casks. The dry storage casks are stored onsite by each utility at a licensed and secured independent spent fuel storage installation (ISFSI). Dry storage casks are robust systems typically consisting of a sealed metal cylinder surrounded by a combination of steel and concrete to provide radiation shielding. The first dry storage casks were loaded with SNF in 1986. Currently there are over 3,000 loaded dry storage casks, and approximately 200 new casks are being placed into service annually at operating nuclear power plants nationwide. Multiple nuclear power plant sites in the United States have shut down and completed decommissioning activities except for the removal of fuel in dry storage. Eventually, the 75,000+ tons of discharged SNF at more than 70 secured locations will need to be safely and securely transported to a new location(s) for eventual disposition. The continued safety and security of this material must be assured.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2019

Status PIE Report on Legacy EBR-II and FFTF Metallic Fuel Experiments

A long term research focus of the US Department of Energy (DOE) Advanced Fuels Campaign (AFC) is to investigate technologies that can allow for increased actinide utilization in nuclear fuel for fast neutron spectrum reactors. In order to reach these goals, many experimental campaigns have been tested in an approximated fast reactor neutron spectra at the Idaho National Laboratory Advanced Test Reactor (ATR) in order to study the performance of metallic, nitride, ceramic and advance fuel forms. In addition and complementary to ATR testing, systematic characterization of experiments irradiated in true fast reactors are performed in order to assess ATR in qualifying fast reactor fuel. For this purpose, complementary postirradiation examinations (PIE) are performed on several metallic fuel pins previously irradiated in the EBR II. Advanced PIE techniques developed since the initial PIE of EBR II samples in the 1980’s have been applied in new examinations of irradiated samples during past EBR-II operations. The EBR-II metallic fuel pins analyzed in this report are X501 G591, an early minor actinide-bearing metallic fuel alloy; X430-T653, a U-19Pu-10Zr metallic fuel alloy with a larger diameter compared to EBR-II driver fuel, and more prototypic of future commercial fast reactors; X521-G594, a unique experiment to test the feasibility to burn weapon grade Pu without reprocessing; X496 CL47&CL39 from a long-life metallic fuel experiment with the goal to reach very high burnup; and X486-J555 a U-10Zr Mk-IIIA qualification fuel test that will serve as first of a kind “modelling driven PIE.” These legacy pins were evaluated against the historical fuel performance of previously irradiated fuel from literature. Fuel performance was investigated through a suite of PIE techniques including neutron radiography, gamma spectrometry, dimensional inspection, fission gas release measurements, chemical burnup analysis, optical microscopy, and advance microscopy. So far, the PIE campaign revealed fuel performance and characteristics that are generally in line with literature or EBR-II experience. Some exceptions are present, and they are directly discussed in this report.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗