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At least 703 records · Page 39

THE EFFECT OF TEMPERATURE AND UNIAXIAL PRESSURE ON THE DENSIFICATION BEHAVIOR OF SILICA AEROGEL GRANULES

Materials are being developed in U.S. for the removal and immobilization of iodine from gaseous products of nuclear fuel reprocessing in support of the Fuel Cycle Technology Separations and Waste Forms Campaign. The silver-functionalized silica aerogel proved to be an excellent candidate for this treatment because of its high selectivity and sorption capacity for radioiodine and its possible conversion to a durable silica-based waste form. The present study investigated with nitrogen sorption and helium pycnometry the effect of pressureless isothermal sintering at temperatures of 900-1400°C for 2.5-90 min or isothermal hot-pressing at 1200°C for 2.5 min on densification of raw and silver-functionalized silica aerogel granules. Rapid sintering was observed at 1050 and 1200°C. Only 15 min of pressureless sintering at 1200°C resulted in almost complete densification. The macropores disappeared, surface area decreased from 1114 m2/g to 25 m2/g, pore volume from 7.41 cm3/g to 0.09 cm3/g, and adsorption pore size from 18.7 to 7 nm. The skeletal density of sintered granules was similar to the bulk density of amorphous silica (2.2 g/cm3). The hot-pressing accelerated the sintering process, decreasing significantly the pore size and volume.

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Saltstone 4QCY14 TCLP Toxicity and UTS Results

A Saltstone Disposal Facility (SDF) waste form was prepared in the Savannah River National Laboratory (SRNL) from a Tank 50H sample and Z-Area premix material for the fourth quarter of calendar year 2014 (4QCY14). After a 47 day cure, a sample of the SDF waste form was collected, and shipped to a certified laboratory for Toxic Characteristic and Universal Treatment Standards (UTS) analysis. The metals analysis is performed using the Toxic Characteristic Leaching Procedure (TCLP) . The 4QCY14 saltstone sample results show that the saltstone is Resource Conservation Recovery Act (RCRA) nonhazardous, but is greater than the universal treatment standard for land disposal. The Saltstone Production Facility (SPF) and SDF were in a maintenance outage during the 4QCY14. Thus no processing or disposal of saltstone, as characterized by this 4QCY14 sample, occurred.

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Saltstone 4QCY14 TCLP Toxicity and UTS Results

A Saltstone Disposal Facility (SDF) waste form was prepared in the Savannah River National Laboratory (SRNL) from a Tank 50H sample and Z-Area premix material for the fourth quarter of calendar year 2014 (4QCY14). After a 47 day cure, a sample of the SDF waste form was collected, and shipped to a certified laboratory for Toxic Characteristic and Universal Treatment Standards (UTS) analysis. The metals analysis is performed using the Toxic Characteristic Leaching Procedure (TCLP) 1 . The 4QCY14 saltstone sample results show that the saltstone is Resource Conservation Recovery Act (RCRA) nonhazardous, but is greater than the universal treatment standard for land disposal. The Saltstone Production Facility (SPF) and SDF were in a maintenance outage during the 4QCY14. Thus no processing or disposal of saltstone, as characterized by this 4QCY14 sample, occurred.

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Preliminary Evaluation of Removing Spent Nuclear Fuel from Shutdown Nuclear Power Plant Sites - 2018 - 19101

This is a technical paper that does not take into account the contractual limitations under the Standard Contract for Disposal of Spent Nuclear Fuel and/or High-Level Radioactive Waste (Standard Contract) (10 CFR Part 961). Under the provisions of the Standard Contract, DOE does not consider spent nuclear fuel in multi-assembly canisters to be an acceptable waste form, absent a mutually agreed to contract amendment. To the extent discussions or recommendations in this paper conflict with the provisions of the Standard Contract, the Standard Contract provisions prevail. The U.S. Department of Energy Office of Integrated Waste Management (DOE-IWM) continues to conduct evaluations of removing spent nuclear fuel (SNF) from shutdown nuclear power plant sites. The 14 shutdown sites included in the evaluation to date have nuclear power reactors that have been permanently shut down and the sites have been decommissioned or are undergoing decommissioning. The 14 shutdown sites are Maine Yankee, Yankee Rowe, Connecticut Yankee, Humboldt Bay, Big Rock Point, Rancho Seco, Trojan, La Crosse, Zion, Crystal River, Kewaunee, San Onofre, Vermont Yankee, and Fort Calhoun. The Oyster Creek Nuclear Generating Station ceased operations in September 2018 and will be included in future evaluations. The evaluations of the shutdown sites contain four components: - A characterization of the SNF and greater-than-Class C low-level radioactive waste (GTCC waste) inventory; - A description of the on-site infrastructure at the shutdown sites; - An evaluation of the near-site transportation infrastructure and experience at the shutdown sites - An evaluation of the actions necessary to prepare for and remove SNF and GTCC waste. The primary sources for the inventory of SNF were the DOE GC-859 and RW-859 spent nuclear fuel inventory databases. This inventory has been augmented with data obtained from the shutdown sites for SNF discharges that occurred after June 2013. The primary sources for information on the conditions of site and near-site transportation infrastructure and experience included field observations and information collected during visits to the 14 shutdown sites, information provided by managers and staff at the shutdown sites, and Google Earth imagery. Extensive photographs taken during the shutdown site visits have proven to be particularly useful in documenting the current conditions at and near the shutdown sites. Tribal and state representatives, State and Regional Group representatives, and Federal Railroad Administration representatives have participated in 11 of the shutdown site visits. In addition to visiting the shutdown site, site visits often include activities such as meeting with local railroads to discuss the near-site railroad infrastructure and meeting with community engagement panels. Oyster Creek permanently ceased power operations on September 17, 2018 and fuel was removed from the reactor vessel on September 25, 2018. Planning for the Oyster Creek site visit has begun and is conducted in three stages. In the first stage, data and documents that are applicable to Oyster Creek are collected. In the second stage, questions are developed based on the data and documents collected during the first stage. These questions are submitted to the Oyster Creek site approximately one month before the site visit. The third stage involves establishing specific schedules and participants. Participants will likely include tribal and state representatives, the Council of State Governments - Eastern Regional Conference, and the Federal Railroad Administration. State participation will likely include a representative of the State Rail Safety Participation Program, the New Jersey Department of Transportation, and the New Jersey Bureau of Nuclear Engineering. The site visit is tentatively expected to occur in April or May of 2019. (authors)

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Immobilization of 99-Technetium (VII) by Fe(II)-Goethite and Limited Reoxidation

During the nuclear waste vitrification process volatilized {sup 99}Tc will be trapped by melter off-gas scrubbers and then washed out into caustic solutions, and plans are currently being contemplated for the disposal of such secondary waste. Solutions containing pertechnetate [{sup 99}Tc(VII)O{sub 4}{sup -}] were mixed with precipitating goethite and dissolved Fe(II) to determine if an iron (oxy)hydroxide-based waste form can reduce Tc(VII) and isolate Tc(IV) from oxygen. The results of these experiments demonstrate that Fe(II) with goethite efficiently catalyzes the reduction of technetium in deionized water and complex solutions that mimic the chemical composition of caustic waste scrubber media. Identification of the phases, goethite + magnetite, was performed using XRD, SEM and TEM methods. Analyses of the Tc-bearing solid products by XAFS indicate that all of the Tc(VII) was reduced to Tc(IV) and that the latter is incorporated into goethite or magnetite as octahedral Tc(IV). Batch dissolution experiments, conducted under ambient oxidizing conditions for more than 180 days, demonstrated a very limited release of Tc to solution (2-7 {micro}g Tc/g solid). Incorporation of Tc(IV) into the goethite lattice thus provides significant advantages for limiting reoxidation and curtailing release of Tc disposed in nuclear waste repositories.

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Geochemical Model of E h and pH Transitions in Pore Fluids during Saltstone and SDU Concrete Aging: Saltstone Disposal Facility PA Revision

The chemical and physical properties of the cementitious materials (dry cement, blast furnace slag, and fly ash) used to construct the Saltstone Disposal Units (SDUs) and saltstone waste form play a key role in the design and long-term performance of the Saltstone Disposal Facility. Chemical degradation of the reducing saltstone and concrete over time will impact radionuclide release and transport due to the changing chemical composition of groundwater (GW) percolating through the porous saltstone waste form. An equilibrium reaction path model was developed using The Geochemist’s Workbench® (GWB) software to estimate the timescales (expressed as number of pore volumes) for chemical degradation of the reducing cementitious materials as indicated by changes in redox potential (E h ) and pH.

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Phase 2 testing results of immobilization of WTP effluent management facility vaporator bottoms simulant

The Hanford Waste Treatment and Immobilization Plant (WTP) Low Activity Waste (LAW) vitrification facility will generate an aqueous condensate recycle stream (LAW Melter Off-Gas Condensate) from the primary off-gas system. This work examined three waste form formulations based on previous testing with related simulants: 8 wt% ordinary portland cement (OPC), 47 wt% blast furnace slag (BFS), 45 wt% fly ash (FA) known as Cast Stone formulation; 20 wt% Aquaset® II-GH and 80 wt% BFS; 20 wt% OPC and 80 wt% BFS. These tests successfully produced one waste form that set within five days (Cast Stone formulation); however the other two formulations, Aquaset® II-GH/BFS and OPC/BFS, took approximately eight and fourteen days to set, respectively.

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Integrated Disposal Facility FY2011 Glass Testing Summary Report [Erratum]

Pacific Northwest National Laboratory was contracted by Washington River Protection Solutions, LLC to provide the technical basis for estimating radionuclide release from the engineered portion of the disposal facility (e.g., source term). Vitrifying the low-activity waste at Hanford is expected to generate over 1.6 x 10 5 m 3 of glass (Certa and Wells 2010). The volume of immobilized low-activity waste (ILAW) at Hanford is the largest in the DOE complex and is one of the largest inventories (approximately 8.9 x 10 14 Bq total activity) of long-lived radionuclides, principally 99 Tc (t 1/2 = 2.1 x 10 5 ), planned for disposal in a low-level waste (LLW) facility. Before the ILAW can be disposed, DOE must conduct a performance assessment (PA) for the Integrated Disposal Facility (IDF) that describes the long-term impacts of the disposal facility on public health and environmental resources. As part of the ILAW glass testing program PNNL is implementing a strategy, consisting of experimentation and modeling, in order to provide the technical basis for estimating radionuclide release from the glass waste form in support of future IDF PAs. The purpose of this report is to summarize the progress made in fiscal year (FY) 2011 toward implementing the strategy with the goal of developing an understanding of the long-term corrosion behavior of low-activity waste glasses.

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Investigations on Repository Near-Field Thermal Modeling - Repository Science/Thermal Load Management & Design Concepts (M41UF033302) (Rev.1)

The modeling tools generated in MathCAD, Excel, and MatLab were used to calculate the temperature evolution for combinations of waste form and geologic medium, assuming a particular emplacement layout for each concept (Sutton et al. 2011). Two types of spent nuclear fuel assemblies (SNFA) were considered, namely UOX from an open fuel cycle and MOX from a modified-­‐open fuel cycle. Four types of high level waste (HLW) canisters were considered, namely “co-­‐extraction” glass from a modified-­‐open fuel cycle and “new extraction” glass, electrochemical ceramic (EC-­‐C) and electrochemical metal (EC-­‐M) from a closed fuel cycle. While the “coextraction” process is similar in function to the industrial Co-­‐Extraction™ (COEX) process deployed by AREVA, the two processes assume different processing methods and steps and so the product and waste streams cannot be directly compared. Similar is true for the “new extraction” process documented in this report and the NUEX industrial process proposed by Energy Solutions, which also cannot be directly compared.

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Tritiated waste management opportunities based on the reduction of tritium activity and outgassing - 15607

Tritiated waste is called as such because tritium is the main radionuclide contained in this waste which is generally produced by nuclear research, fusion facilities and small producers, e.g. hospitals, research centers and industries. The management of this type of waste can be improved by using techniques that reduce the tritium activity and outgassing levels. Several options are possible depending on the waste form and the amount of tritium: temporary storage for tritium decay up to 50 years, thermal treatment such as incineration and melting, and high-integrity containers for conditioning, either considered alone or in combination with one of the other options. This paper compares a number of waste management parameters with respect to tritiated waste: the environmental impact of tritium releases, secondary waste management, volume reduction of the waste for final disposal, and the waste activity after treatment, not to mention the related safety issues, the performance of the techniques used in each option, and economic aspects. The results of this comparative work are given in this paper, with the advantages and drawbacks of each option discussed in detail. (authors)

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Coupled hydro-thermal flow and radionuclide transport driven by spatial variation of heat-generating radioactive wastes in shale formations

Deep geologic disposal of multiple nuclear waste packages with various heat sources can induce nonuniform hydro-thermal behaviors in the near-field of the repository, consequently influencing the long-term radionuclide transport in the far-field once waste form breach initiates. Here, this study looks into three cases with variation in the spatial order of six groups of heat sources (10th, 50th, 75th, 90th, 95th, and 99th percentiles of heat outputs generated from 1,981 as-loaded dual-purpose canisters in the field site) in a shale-hosted repository with respect to the uni-directional groundwater flow (from west to east): (1) cooler waste packages from west to east, (2) hotter waste packages from west to east, and (3) hottest waste packages in the middle of the repository. Our field-scale PFLOTRAN simulation represents heat-driven multiphysics coupled mechanisms, including multiphase flow, heat transfer, and chemical/radioactive transport, and also, calculates the onset of waste form breach based on temperature-dependent canister vitality. The results from this sensitivity study will quantify the short- (less than 1 × 10 3 years) and long-term (up to 1 × 10 6 years) impacts of sporadic heat pulses from waste package on the spatio-temporal perturbation in hydro-thermal flow quantities and the rate of radionuclide transport in both near- and far-field of the repository system.

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Post-closure Nuclear Criticality Safety Evaluations for Disposition of Criticality Control Overpacks at the Waste Isolation Pilot Plant

The Waste Isolation Pilot Plant (WIPP) is a geological repository in southern New Mexico that provides for disposal of transuranic (TRU) wastes from atomic energy defense activities. The Sandia National Laboratories (Sandia) Report, Consideration of Nuclear Criticality When Disposing of Transuranic Waste at the Waste Isolation Pilot Plant, addresses nuclear criticality safety based on the projected inventory characteristics for the initial compliance certification application of WIPP in 1996. As the inventory, waste forms, and disposal package designs change, revised or new analyses are necessary to demonstrate acceptability for these configurations within the WIPP safety basis and compliance with 10,000-year post-closure standards of the US Environmental Protection Agency (EPA). Saylor and Scaglione evaluated criticality control overpacks (CCOs) in 2017 based on conservative assumptions for post-closure repository structural conditions with resulting effects on containers and container spacing, The Saylor and Scaglione evaluation of CCOs addressed a single waste configuration that represents the Surplus Plutonium Disposition Program’s dilute and dispose waste form and composition. This initial CCO study demonstrated that 50 grams of boron carbide (B 4 C) per CCO is sufficient to ensure post-closure criticality safety based on a well-mixed waste composition, and Oak Ridge National Laboratory (ORNL) subsequently determined that this amount of B 4 C does not require constraints on moisture or plastic present as moderator. The Saylor and Scaglione analysis conservatively assumes repository room closure that eliminates all space between fissile gram equivalent (FGE) 239 Pu masses. The close-packed array was selected based on limited availability of repository salt creep modeling results at that time. In 2019, Brickner provided additional evaluations for pipe overpack containers (POCs), building on the conservative basis provided by Saylor and Scaglione. Brickner’s 2019 analysis made use of new geomechanical data for post-closure spacing that rely on advances in repository modeling as documented in the work by Reedlunn and Bean. This current CCO evaluation for generic waste materials expands on earlier work performed at ORNL and includes evaluation of CCOs across a much broader range of possible waste compositions and geometries. This evaluation is intended to provide input for the required feature, event and process (FEP) screening to determine if post-closure criticality must be included as an event in the 10,000-year regulatory evaluation. As such, the approach to modeling post-closure criticality presented in this report has been coordinated with the Sandia team responsible for FEP screening. The resulting analysis supports disposition of fissile materials in the CCO containing up to 380 FGE 239 Pu and expands conditions acceptable for disposal of fissile material in CCOs. This evaluation builds on the methodology of Saylor and Scaglione and Brickner, using the most recently available geomechanical data for CCO spacing under salt creep compaction scenarios provided by Reedlunn and Bean. The broad range of fissile material configurations analyzed in this report are intended to account for configurations that may occur during the post-closure disposal time period, and it also includes waste configurations that are not physically possible to support analysis of conditions that influence neutron fluence.

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Corrosion of Metal Inclusions In Bulk Vitrification Waste Packages. Erratum

This report refers to or contains K g values for glasses LAWA44, LAWB45 and LAWC22 affected by calculations errors as identified by Papathanassiu et al. (2011). The corrected K g values are reported in an erratum included in the revised version of the original report. The revised report can be referenced as follows: Pierce E. M. et al. (2004) Waste Form Release Data Package for the 2005 Integrated Disposal Facility Performance Assessment. PNNL-14805 Rev. 0 Erratum. Pacific Northwest National Laboratory, Richland, WA, USA.

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Integrated Disposal Facility FY2011 Glass Testing Summary Report. Erratum

This report refers to or contains K g values for glasses LAWA44, LAWB45 and LAWC22 affected by calculations errors as identified by Papathanassiu et al. (2011). The corrected K g values are reported in an erratum included in the revised version of the original report. The revised report can be referenced as follows: Pierce E. M. et al. (2004) Waste Form Release Data Package for the 2005 Integrated Disposal Facility Performance Assessment. PNNL-14805 Rev. 0 Erratum. Pacific Northwest National Laboratory, Richland, WA, USA.

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Solubility constants of hydroxyl sodalite at elevated temperatures evaluated from hydrothermal experiments: Applications to nuclear waste isolation

In this study, solubility constants of hydroxyl sodalite (ideal formula, Na 8 [Al 6 Si 6 O 24 ][OH] 2 ·3H 2 O) from 25°C to 100°C are obtained by applying a high temperature Al—Si Pitzer model to evaluate solubility data on hydroxyl sodalite in high ionic strength solutions at elevated temperatures. A validation test comparing model-independent experimental data to model predictions demonstrates that the solubility values produced by the model are in excellent agreement with the experimental data. In addition, the equilibrium constants obtained in this study have a wide range of applications, including synthesis of hydroxyl sodalite, de-silication in the Bayer process for extraction of alumina, and the performance of proposed sodalite waste forms in geological repositories in various lithologies including salt formations. The thermodynamic calculations based on the equilibrium constants obtained in this work indicate that the solubility products in terms of m ΣAl ×m ΣSi for hydroxyl sodalite are very low (e.g., ~10 -13 [mol·kg -1 ] 2 at 100°C) in brines characteristic of salt formations, implying that sodalite waste forms would perform very well in repositories located in salt formations. Finally, the information regarding the solubility behavior of hydroxyl sodalite obtained in this study provides guidance to investigate the performance of other pure end-members of sodalite such as chloride- and iodide-sodalite, which may be of interest for geological repositories in various media.

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Advanced Retrieval and Disposition Techniques for Remote Handled Mixed Low-Level Waste - 20319

Legacy waste generated by the sodium-cooled fast reactor, EBR-II, program at the Idaho National Laboratory (INL) (owned by the U.S. Department of Energy and managed and operated by Battelle Energy Alliance, LLC) is challenging to treat and disposition using conventional methods. As a result, Veolia Nuclear Solutions is under contract with the Idaho National Laboratory to demonstrate an integrated retrieval and disposition solution for Remote-Handled Mixed Low-Level Waste currently stored in underground liners at INL. Delivery of the integrated solution builds on the expertise and successes of Veolia Nuclear Solutions under its Problematic Waste Treatment Initiative with INL. This initiative focuses solely on the treatment of problematic (reactive metal containing) waste streams using the Veolia Nuclear Solutions GeoMelt{sup R} In-Container Vitrification (ICV{sup TM}) technology. Under the contract, Veolia Nuclear Solutions will provide a fully commissioned prototype remote retrieval system to semi-remotely retrieve and size-reduce problematic waste liners into a safe and consolidated package for transport. The consolidated package will be shipped to Richland, Washington for demonstration treatment using the robust GeoMelt Richland system at Perma-Fix Northwest. The treated waste will ultimately be disposed of as a vitrified Low-Level Waste glass monolith. Veolia Nuclear Solutions has delivered countless remotely operated systems globally to solve some of the industry's most challenging problems. To ensure risk is mitigated in the best possible manner, a methodical phased approach is being utilized to validate the integrated solution. This contract focuses on the delivery and deployment of the prototype retrieval system onsite and the treatment of a single liner. Following successful demonstration treatment using GeoMelt ICV, the project is planning to make prototype enhancements before retrieving and treating another liner. Establishing a new integrated approach for retrieval and disposition of waste offers many benefits to INL and the U.S. Department of Energy. It is anticipated that the integrated solution will provide significant cost and schedule savings by increasing the number of liners dispositioned per year. In addition, the complexity of the overall waste disposition process will be reduced. Remotely retrieving and size-reducing waste in the field will provide additional safety to operational personnel and allow critical resources, such as hot cells, to focus on the primary missions at hand. Vitrification (using the GeoMelt ICV technology) allows for the direct processing of metal clad waste thereby significantly reducing pretreatment steps while providing a robust waste form for long-term disposal. The results from this ongoing contract are presented in this paper. (authors)

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Report for Treating Hanford LAW and WTP SW Simulants: Pilot Plant Mineralizing Flowsheet

The US Department of Energy is responsible for managing the disposal of radioactive liquid waste in underground storage tanks at the Hanford site in Washington State. The Hanford waste treatment and immobilization plant (WPT) will separate the waste into a small volume of high level waste (HLW), containing most of the radioactive constituents, and a larger volume of low activity waste (LAW), containing most of the non-radioactive chemical and hazardous constituents. The HLW and LAW will be converted into immobilized waste forms for disposal. Currently there is inadequate LAW vitrification capacity planned at the WTP to complete the mission within the required timeframe. Therefore additional LAW capacity is required. One candidate supplemental treatment technology is the fluidized bed steam reformer process (FBSR). This report describes the demonstration testing of the FBSR process using a mineralizing flowsheet for treating simulated Hanford LAW and secondary waste from the WTP (WTP SW). The FBSR testing project produced leach-resistant solid products and environmentally compliant gaseous effluents. The solid products incorporated normally soluble ions into an alkali alumino-silicate (NaS) mineral matrix. Gaseous emissions were found to be within regulatory limits. Cesium and rhenium were captured in the mineralized products with system removal efficiencies of 99.999% and 99.998 respectively. The durability and leach performance of the FBSR granular solid were superior to the low activity reference material (LMR) glass standards. Normalized product consistency test (PCT) release rates for constituents of concern were approximately 2 orders of magnitude less than that of sodium in the Hanford glass [standard].

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Synthesis and Characterization of Silicon Carbide Ceramic Composites with CeO 2 Powder

This study pioneers the fabrication and characterization of silicon carbide (SiC) containing cerium dioxide (CeO 2 ). CeO 2 powder was tested as a surrogate for actinide oxide waste forms such as uranium dioxide (UO 2 ) and plutonium dioxide (PuO 2 ). Several syntheses were evaluated with varying amounts of preceramic polymer (SMP-10 resin) and CeO 2 containing either SiC fiber, carbon fiber, or no fibers. Scanning electron microscopy (SEM) was used to characterize morphology and compositional differences, and energy-dispersive x-ray spectroscopy (EDS) was used to provide semiquantitative elemental analysis. In addition, each sample was characterized by density, powder x-ray diffraction (pXRD), and Raman spectroscopy. Samples containing nearly more than four times CeO 2 powder than SMP-10 resin by mass had the best properties. This research establishes a unique synthesis for SiC containing high concentrations of CeO 2 powder to illustrate how it may be managed as a potential waste form.

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