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At least 91 records · Page 5

Respirable Release Fraction Measurement Chamber (RRFMC) - 18321

The Respirable Release Fraction Measurement Chamber (RRFMC) is designed to hoist a container to a predetermined height, drop it, and then utilize aerosol particle counters to measure the mass of powder that is released from failed containers. The RRFMC hoist mechanism is located inside an airtight (6.1 m high) steel enclosure that isolates the released test aerosol from the surrounding lab room environment. Accurate measurement of the released test powder is necessary for estimating the total released mass of material. Cerium oxide will be used as a surrogate for plutonium oxide. The range of the aerodynamic diameter of cerium oxide test powder was characterized both by cascade impaction and aerodynamic sizing. The scope of this paper includes the physical parameters required for accurately measuring the total mass of released powder, the fabrication of the tower, various strategies to optimize concentration sampling, and developing methods to accurately measure the respirable fraction, airborne release fraction, and the damage ratio. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Development of Automated Material Handling System with Alternate Gripper Designs for the Purpose of Increased Performance & Worker Safety

Savannah River National Laboratory’s (SRNL) Surplus Plutonium Disposition (SPD) Program leads the development and transition of automated unit operations for the processing of Plutonium oxide. A mixing can is opened, filled with material, mixed, set inside of a die can, and finally punched into compressed material. Replication of the process is constructed in A-area, where the mixing can weighs 1.6 kg (3.5 lbs.) and the compressed material weighs 4 kg (8.8 lbs.). Due to the constant process of Plutonium disposition, the fatigue on workers and worker dose accumulates quickly over time. SPD aims to automate this process by using a robotic arm to replace the hands-on worker. Automation will: Reduce worker radiation dose; Increase process throughout; Reduce costs for the disposition of Plutonium oxide.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

ARIES Blend Lot Book Data Analysis

The Advanced Recovery Integrated Extraction System (ARIES) Program being executed at Los Alamos TA-55 produces unpolished plutonium oxide powder from pit disassembly in batches of material referred to as a blend lot. Each blend lot is sampled and analyzed by Los Alamos group C-AAC (Chemistry Division, Actinide Analytical Chemistry Group) for radioactive and nonradioactive constituents contained in the material. A blend lot, which nominally consists of 12 kg(Pu), is then packaged into three DOE-STD-3013 containers that are analyzed by nondestructive analysis (NDA) to determine the fraction and total amount of plutonium mass relative to impure plutonium oxide. The analytical and NDA data are presented in a Blend Lot Book (BLB). The data are used to confirm that a blend lot grouping of three cans meets the requirements for off-site shipment specified in the formal interface control document (ICD). The analytical and NDA data from 49 blend lots were reviewed to provide summary-level information on the constituents present in the blend lots. The results provide an overall perspective in historical amounts for constituent averages over all blend lots and similar information in the variation between constituent levels. Note that to properly compare the can contents, it would be most appropriate to decay all of cans’ constituents to a particular date. Previously, this analysis only examined statistical data as determined at the time of blend lot chemical analysis. The chemical analysis dates span the period from June 2011 to May 2015 (4 years), which is 28% of one Pu-241 half-life. Therefore, the approximate nature of the aggregate information must be properly understood in this light. However, to address this issue, a new table is included in this revision that decays the 48 blend lots to a single date.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Characteristics of Uranium-Plutonium Mixed Oxide Nondestructive Assay Standards

A set of six well-characterized, homogeneous, mixed HEU-WGPu oxide standards has been manufactured for and are proposed for qualification as NDA working reference standards with SAFE-NMCA. These standards, if approved, will provide the basis for qualifying the FRAM isotopic systems for use in accountability measurements of 235U in the presence of Pu for unknown mixed U-Pu items by nondestructive assay. The U to Pu elemental mass ratios of the six analytical standards are nominally in the proportions 0.1, 0.25, 1.0, 2.5, 10, and 20; these values were chosen to span the U/Pu mass ratios of inventory items that ultimately will be measured by nondestructive assay and which currently reside in long term storage. The measured characteristics, including plutonium and uranium elemental masses and isotopic distribution, of each standard and relevant source documentation are reported here.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Particle size of several plutonium-238 oxide fuel samples from oxalate precipitation processes

Particle size of 238 PuO 2 powders is an important factor in determining the structural integrity of fuel pellets hot-pressed from the oxide powder. Understanding the evolution of particle size during aqueous processing is a first step in assuring control of particle size throughout the pellet formation process. Measured particle sizes are reported here, and discussed in terms of measured particle size changes occurring during calcining, observed aggregation of particulate, and particle morphology. Morphology and aggregation are related to surface energy, which governs granule formation and hot pressing behavior. Results are discussed in terms of reported dependence of oxide morphology on process temperatures and reagent concentrations.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Microsphere Plutonium-238 Oxide Fuel to Revolutionize New Radioisotope Power Systems and Heat Sources for Planetary Exploration

Microsphere 238PuO2 fuels have potential to provide performance and safety enhancements for future radioisotope heat and power systems (RPS) as well as enable more flexible and compact RPS designs. Improvements in RPS specific power and more flexible geometries were recently investigated by JPL and PNNL as part of a study on cryobot devices for exploring Ocean Worlds. Missions to penetrate ice and explore oceans, such as on Europa, will require RPS with high specific power within the vehicle to provide both heat and power. Such missions will be mass-constrained, and the energy required to penetrate the ice is highly dependent on cryobot size. Therefore, compact RPS geometries are needed to maximize heat and power while minimizing 238Pu inventory. Microsphere-based heat sources are an attractive way to obtain flexible geometries and high volumetric power loadings because they can fill a region of any size and shape provided fuel temperatures are kept below a threshold and launch/re-entry safety are not compromised. The sol-gel technique to produce 238PuO2 microsphere particles for heat sources has the benefit of preventing dust generation, as opposed to the current 238PuO2 powder/pellet processing method, reducing hazards in the fuel fabrication line. Microspheres can also be individually coated to enhance thermal conductivity, and/or reduce the likelihood of 238PuO2 fuel dispersal in an accident. Although PNNL has produced 238PuO2 microspheres using the sol-gel method, the application of coatings and their integrity over time has yet to be investigated. Continued R&D could demonstrate the feasibility of advanced, microspherebased heat sources and provide baseline data for planning future missions requiring new RPS with different heat source configurations.

Fleurial, Jean-Pierre↗

Distillation of Americium from Plutonium Americium Oxide

Understanding the changes that fuel undergoes inside a reactor and understanding the properties of recycled fuel to provide a foundation for the development of a sustainable nuclear fuel cycles are two of the main objectives of Fuel Cycle Research and Development (FCRD). Research on transmutation fuel aims to develop technologies needed to transmute the long-lived transuranic actinide isotopes contained in spent nuclear fuel into shorter-lived fission products, thereby decreasing both the volume of material requiring disposal and the long-term radiotoxicity of the waste. Since there is no recycled nuclear fuel available for study within the United States, studies of this type of fuel must be conducted on fabricated fuel. Americium is an important component of recycled fuel and, thus, is a vital additive in the fabrication process. Unfortunately, the supplies of pure americium metal are dwindling. Idaho National laboratory (INL) has acquired a stockpile of americium- bearing material from around the DOE complex which can be purified to supply the needs of the fuel fabrication process. In order to make this material usable, it must be distilled (or, in some cases, reduced from an oxide) to a material pure enough to be used in the fuel fabrication process. The americium distillation experiments were set up to develop a process to convert the available americium bearing material into pure americium metal. This work gives important insight into the best parameters to use in future americium distillation runs. Since future starting material is likely to contain significantly more oxide, it will be necessary to add a reducing agent such as lanthanum in order to reduce the oxide material prior to distillation. Early experiments show that the addition of lanthanum does not significantly change the purity of the end product. Soak time was found to be beneficial in producing a higher quantity of pure material. All experiments show that the material preferentially deposits on the walls of the crucible rather than on the cold finger as was originally intended. Future experiments will aim to deposit material on the cold finger rather than the crucible walls in order to make material retrieval easier as well as to increase yield. (authors)

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Microstructural characterization of plutonium oxalate and oxide particles by three-dimensional focused ion beam tomography

Focused ion beam (FIB) tomography was used to characterize three-dimensional (3D) internal microstructures of plutonium oxalate and oxide particles. Sequential two-dimensional (2D) sectioning and imaging using FIB and 3D image reconstruction were used to elucidate and distinguish internal pore microstructure and distribution in plutonium oxide particles calcined from plutonium oxalate precipitates. The results show that the plutonium oxide particles have a significant increase in pore volume fraction while retaining the exterior morphological shape of the corresponding oxalate precipitates. This technique enables the examination of the internal structure of radioactive microparticles for nuclear forensics that is not available with conventional microscopy.

36 MATERIALS SCIENCE↗

New reference materials for trace-levels of actinide elements in plutonium

In this report two plutonium oxides were prepared as unique reference materials for measurement of actinide elements present as trace constituents. Each reference material unit is approximately 200 mg of PuO 2 powder in a quartz glass bottle. Characterized attributes of the oxides included mass fractions of plutonium, americium, neptunium, and uranium. Isotope-amount ratios were also determined for plutonium and uranium, but neptunium and americium were observed to be monoisotopic 237 Np and 241 Am. Measurements for characterization and verification of the attributes show that plutonium and trace actinides are homogeneous with the exception of limited heterogeneity for uranium, primarily observed for the 238 U isotope. Model purification ages calculated from measured americium and uranium attribute values are consistent with material histories and indicate that these impurities are predominantly due to the decay of plutonium isotopes.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

MIS High-Purity Uranium/Plutonium Oxide Metal Oxidation Product SCP711-56 (SSR135): Final Report

A high-purity uranium/plutonium mixed oxide material from the Material Identification and Surveillance (MIS) Program inventory has been studied with regard to gas generation and corrosion in a storage environment. Sample SCP711-56 represents process plutonium oxides from mixed oxides at the Hanford Site, byproduct plutonium/uranium mixed oxides at the Rocky Flats Plant, Hanford Site mixed oxides at Savannah River, mixed oxides from alloy oxidation at Savannah River, scrap mixed oxides at Savannah River and plutonium/uranium oxide at Los Alamos National Laboratory that are currently stored in 3013 containers. After calcination to 950°C the material contains 17% fuel grade plutonium and 68% uranium with approximately 1.5% impurities and the remainder principally oxygen. This study followed over time the gas pressure of a sample with nominally 0.1 wt% water in a sealed container with an internal volume scaled to 1/500th of the volume of a 3013 container. Gas compositions were measured periodically over approximately 4 years. The maximum observed gas pressure was 115 kPa. The increase over the initial pressure of 83 kPa was primarily due to generation of carbon dioxide and nitrogen gases. A small amount of hydrogen was generated and oxygen was consumed. At the completion of the study, the internal components of the sealed container showed signs of corrosion, including pitting.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Re-evaluation of Moisture Controls During ARIES Oxide Processing, Packaging and Characterization

DOE-STD-3013 [1] requires limiting the relative humidity (RH) in the glovebox during processing of the oxide product for specific types of plutonium oxides. This requirement is mandated in order to limit corrosion of the stainless steel containers by deliquescence of chloride salts if present in the PuO2. DOE-STD-3013 also specifies the need to limit and monitor internal pressure buildup in the 3013 containers due to the potential for the generation of free H2 and O2 gas from the radiolysis of surfaceadsorbed water. DOE-STD-3013 requires that the oxide sample taken for moisture content verification be representative of the stabilized material in the 3013 container. This is accomplished by either limiting the time between sampling and packaging, or by control of the glovebox relative humidity (%RH). This requirement ensures that the sample is not only representative, but also conservative from the standpoint of moisture content.

36 MATERIALS SCIENCE↗

Plutonium metal vs. oxide determination with the pulse-shape-discrimination-capable plastic scintillator EJ-299-33

Neutron measurements can be used to distinguish plutonium in metal or oxide form, a capability that is of great interest in nuclear nonproliferation, treaty verification, and other applications. This paper describes measurements performed on well-characterized samples of plutonium oxide and plutonium metal using the pulse-shape-discrimination-capable plastic scintillator EJ-299-33. Results are compared to those obtained with a same-sized detector cell using the liquid scintillator EJ-309. The same optimized, digital pulse shape discrimination technique is applied to both detectors and the neutron pulse height distributions are compared. Results show that the EJ-299-33 plastics can be successfully used for plutonium measurements, where the gamma ray to neutron detection ratio is much higher than for typical radioactive sources. Results also show that EJ-299-33 detectors can be used to characterize plutonium samples, specifically to discriminate between plutonium metal and oxide.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

X-ray excited Auger transitions of Pu compounds

X-ray excited Pu core–valence–valence and core–core–valence Auger line-shapes were used in combination with the Pu 4f photoelectron peaks to characterize differences in the oxidation state and local electronic structure for Pu compounds. The evolution of the Pu 4f core-level chemical shift as a function of sputtering depth profiling and hydrogen exposure at ambient temperature was quantified. The combination of the core–valence–valence Auger peak energies with the associated chemical shift of the Pu 4f photoelectron line defines the Auger parameter and results in a reliable method for definitively determining oxidation states independent of binding energy calibration. Results show that PuO{sub 2}, Pu{sub 2}O{sub 3}, PuH{sub 2.7}, and Pu have definitive Auger line-shapes. These data were used to produce a chemical state (Wagner) plot for select plutonium oxides. This Wagner plot allowed us to distinguish between the trivalent hydride and the trivalent oxide, which cannot be differentiated by the Pu 4f binding energy alone.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

On the equilibrium isotopic composition of the thorium–uranium–plutonium fuel cycle

The equilibrium isotopic compositions and the times to equilibrium in the process of thorium–uranium–plutonium oxide fuel recycling in VVER-type reactors using heavy water mixed with light water are estimated. It is demonstrated thEhfat such reactors have a capacity to operate with self-reproduction of active isotopes in the equilibrium mode.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Americium Utilization Via Pyroelectrochemical Granulation and Vibrocompaction Technologies

An experiment in which americium is introduced into the composition of fuel pins with vibrocompacted uranium-plutonium oxide fuel is described within the scope of work performed on the development of a closed fuel cycle for a fast reactors. Possible directions of R&D work for validating the design, fabrication technology, and serviceability of fuel pins with fuel containing americium are examined. A variant based on the chemical-technological complex at the Research Institute for Atomic Reactors (NIIAR) is proposed for developing centralized production of americium burn-out elements for liquid-metal cooled fast reactors. The assimilated remote-controlled technologies of pyroelectrochemical granulation of oxide fuel compositions and vibrocompaction in radiation protected boxes as well as the automated equipment specially developed within the special federal program are proposed for manufacturing the burn-out elements.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Utilization of non-weapons-grade plutonium and highly enriched uranium with breeding of the {sup 233}U isotope in the VVER reactors using thorium and heavy water

A method for joint utilization of non-weapons-grade plutonium and highly enriched uranium in the thorium–uranium—plutonium oxide fuel of a water-moderated reactor with a varying water composition (D{sub 2}O, H{sub 2}O) is proposed. The method is characterized by efficient breeding of the {sup 233}U isotope and safe reactor operation and is comparatively simple to implement.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗