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At least 37 records · Page 2

In-field alpha spectrometry system for uranium enrichment verification of uranium hexafluoride

A portable In-Field Alpha Spectrometry (IFAS) system was developed to support on-site uranium enrichment determination for samples taken at facilities working with gaseous UF 6 . It consists of a modified commercial alpha spectrometer, a vacuum pump, a laptop computer, and associated connectors and cables. The IFAS uses specially designed Single-Use Destructive Assay (SUDA) samplers to capture gaseous UF 6 and convert and store it as UO 2 F 2 in a thin-film zeolite. To examine the quantitative performance of the IFAS system a large number of replicate SUDA samples was acquired for natural uranium (NU, 0.72 wt%, 23 samples), low enriched uranium 1 (LEU1, 2.33 wt% 235 U, 10 samples), and low enriched uranium 2 (LEU2, 4.62 wt% 235 U, 10 samples). The standard deviation (SD) values for uranium enrichment determination with the IFAS for NU, LEU1, and LEU2, in 20-hour assays, were 0.037 wt% 235 U, 0.063 wt% 235 U, and 0.072 wt% 235 U, respectively. In addition, a separate analysis suggests that comparable SD values can be achieved in less time, approximately 8-10 hours. For context, these SD values are well below the International Atomic Energy Agency’s International Target Values for the determination of uranium enrichment in non-destructive assay measurements.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Spectral properties of gaseous uranium hexafluoride at high temperature

A study to determine relative spectral emission and spectral absorption data for UF6-argon mixtures at elevated temperatures is discussed. These spectral data are required to assist in the theoretical analysis of radiation transport in the nuclear fuel-buffer gas region of a plasma core reactor. Relative emission measurements were made for UF6-argon mixtures over a range of temperatures from 650 to 1900 K and in the wavelength range from 600 to 5000 nanometers. All emission results were determined for a total pressure of 1.0 atm. Uranium hexafluoride partial pressures varied from about 3.5 to 12.7 mm Hg. Absorption measurements were attempted at 600, 625, 650 and 675 nanometers for a temperature of 1000 K. The uranium partial pressure for these determinations was 25 mm Hg. The results exhibit appreciable emission for hot UF6-argon mixtures at wavelengths between 600 and 1800 nanometers and no measurable absorption. The equipment used to evaluate the spectral properties of the UF6-argon mixtures included a plasma torch-optical plenum assembly, the monochromator, and the UF6 transfer system. Each is described.

Krascella, N. L.↗

Direct uranium enrichment assay in gaseous uranium hexafluoride with laser induced breakdown spectroscopy

A set of eleven U atomic emission lines, between 421.099 and 421.460 nm, were characterized for direct enrichment assay of gaseous UF 6 samples with laser induced breakdown spectroscopy (LIBS). Several iterative, multivariate nonlinear spectral-fitting algorithms were evaluated for their efficacies to extract the enrichment information from the measured LIBS spectra. Furthermore, wavelength-dependent weight factors, which take into consideration of the spectral-line position in the fitting model, the determined isotopic ratio, and the isotopic shift of the emission line, are essential for the spectral-fitting model to function adequately. The analytical accuracies and precision were typically within 0.5% in absolute [ 235 U/( 235 U + 238 U)] ratios.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Circulation system for flowing uranium hexafluoride cavity reactor experiments

Research related to determining the feasibility of producing continuous power from fissile fuel in the gaseous state is presented. The development of three laboratory-scale flow systems for handling gaseous UF6 at temperatures up to 500 K, pressure up to approximately 40 atm, and continuous flow rates up to approximately 50g/s is presented. A UF6 handling system fabricated for static critical tests currently being conducted is described. The system was designed to supply UF6 to a double-walled aluminum core canister assembly at temperatures between 300 K and 400 K and pressure up to 4 atm. A second UF6 handling system designed to provide a circulating flow of up to 50g/s of gaseous UF6 in a closed-loop through a double-walled aluminum core canister with controlled temperature and pressure is described. Data from flow tests using UF6 and UF6/He mixtures with this system at flow rates up to approximately 12g/s and pressure up to 4 atm are presented. A third UF6 handling system fabricated to provide a continuous flow of UF6 at flow rates up to 5g/s and at pressures up to 40 atm for use in rf-heated, uranium plasma confinement experiments is described.

Jaminet, J. F.↗

Formation of Aerosol Nanoparticles by Gas-Phase Hydrolysis Reaction of Uranium Hexafluoride

The aerosol physics of uranyl particle formation has been addressed in this research using advanced aerosol instrumentation and an aerosol dynamics model. Based on the research works, we conclude that the formation and growth of aerosol particles by gas-phase UF6 hydrolysis strongly depends on the availability of water molecules in our reactor conditions. The total number concentration of the UO 2 F 2 particulate material that could be produced in the hydrolysis reaction is also regulated primarily by the availability of water molecule concentration. The higher the water molecule concentration, the higher the number and the larger the size of UO 2 F 2 aerosol particles that could be produced in a reactor custom-built at ORNL. Although the aerosol reactor was enabling the study of particle formation kinetics, the instrumentation was still insufficient in characterizing the chemical composition of the produced particles as well as the time-dependent evolution of the particulate species. The temporal evolution could impact the eventual fate of the particles upon release to the environment (i.e., the physio-chemical transformation, transport, and removal). On uranyl particle formation kinetics, we found that the growth rates of aerosol particles appeared to approach a single number in the range of 0.05 ± 0.03 - 0.08 ± 0.04 nm/s, statistically, as the ω value becomes smaller than 1. The size of primary particles from the UF6 hydrolysis at water-deprived condition was estimated to be 3.6 ± 0.4 nm; the higher the availability of water molecules, the larger the primary particles. The ability to precisely control the availability of water molecules in the reaction could lead to the production of nearly monodispersed aerosol particles. In other words, the result suggests that one can precisely manipulate the size of UO 2 F 2 aerosol particles by controlling the water vapor availability and interaction of water molecules with U F6 in the reaction. This finding has significant implications in the engineering manufacturing of fuel powder materials and possibly to future development and deployment of an environmental sampling apparatus.

74 ATOMIC AND MOLECULAR PHYSICS↗

The spectral properties of uranium hexafluoride and its thermal decomposition products

This investigation was initiated to provide basic spectral data for gases of interest to the plasma core reactor concept. The attenuation of vacuum ultraviolet (VUV) radiation by helium at pressures up to 20 atm over path lengths of about 61 cm and in the approximate wavelength range between 80 and 300 nm was studied. Measurements were also conducted to provide basic VUV data with respect to UF6 and UF6/argon mixtures in the wavelength range between 80 and 120 nm. Finally, an investigation was initiated to provide basic spectral emission and absorption data for UF6 and possible thermal decomposition products of UF6 at elevated temperatures.

Krascella, N. L.↗

The emission characteristics of uranium hexafluoride at high temperatures

Relative emission measurements were made for UF6/Argon mixtures heated in a plasma torch over a range of temperatures from 800 to about 3600 K over a wavelength range from 80 to 600 nm. Total pressures were varied from 1 to approximately 1.7 atm. Similarly absorption measurements were carried out in the visible region from 420 to 580 nm over a temperature range from about 1000 to 1800 K. Total pressure for these measurements was 1.0 atm. The emission results exhibited relatively no emission at wavelengths below 250 nm over the range of temperatures investigated. At temperatures in excess of 1800 K an additional emission band centered at 310 nm appears and becomes more well defined at higher temperatures. Essentially no pressure effect was observed with respect to emission at pressures up to 1.7 atm.

Krascella, N. L.↗

Thermodynamic properties of UF sub 6 measured with a ballistic piston compressor

From experiments performed with a ballistic piston compressor, certain thermodynamic properties of uranium hexafluoride were investigated. Difficulties presented by the nonideal processes encountered in ballistic compressors are discussed and a computer code BCCC (Ballistic Compressor Computer Code) is developed to analyze the experimental data. The BCCC unfolds the thermodynamic properties of uranium hexafluoride from the helium-uranium hexafluoride mixture used as the test gas in the ballistic compressor. The thermodynamic properties deduced include the specific heat at constant volume, the ratio of specific heats for UF6, and the viscous coupling constant of helium-uranium hexafluoride mixtures.

Sterritt, D. E.↗

Plasma core reactor simulations using RF uranium seeded argon discharges

Experimental results are described in which pure uranium hexafluoride was injected into an argon-confined, steady-state, RF-heated plasma to investigate characteristics of plasma core nuclear reactors. The 80 kW (13.56 MHz) and 1.2 MW (5.51 MHz) rf induction heater facilities were used to determine a test chamber flow scheme which offered best uranium confinement with minimum wall coating. The cylindrical fused-silica test chamber walls were 5.7-cm-ID by 10-cm-long. Test conditions included RF powers of 2-85 kW, chamber pressures of 1-12 atm, and uranium hexafluoride mass-flow rates of 0.005-0.13 g/s. Successful techniques were developed for fluid-mechanical confinement of RF-heated plasmas with pure uranium hexafluoride injection.

Roman, W. C.↗

Radiation hot spot formation on UF 6 30B cylinders

The accurate material accountancy of a country's enriched uranium hexafluoride (UF 6 ) stockpiles is imperative to the International Atomic Energy Agency (IAEA) for determining appropriate material safeguards. Uranium hexafluoride is typically stored in large cylinders with enrichment verification typically performed with a NaI gamma detector using the enrichment meter method. This approach for calculating enrichment assumes that the UF 6 is homogeneous inside the cylinder. Here, the measurements and tests presented in this manuscript show that the UF 6 in cylinders left outside in the elements can experience fractionation, leading to inhomogeneity, and subsequent development of radiation hot spots. These hot spot locations can produce errant enrichment measurements. In dark-colored cylinders that experience significant surface heating from the sun, UF 6 sublimates off the cylinder walls, leaving only the uranium daughter products in a horizontal patch (stripe) along the cylinder's midline. This daughter patch is hypothesized to be the source of the radiation hot spots. The patch forms during the summer and tends to decay away during the winter, when solar intensity and temperatures are reduced.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Heterogeneity effects on nondestructive assay measurements of enrichment in UF 6 cylinders

A set of measurements were performed using multiple mechanically cooled HPGe detectors at six positions around a cylinder uranium hexafluoride to assess if matrix inhomogeneity is detectible and effects the determined apparent uranium enrichment. These measurements were performed on nine 30B cylinders of uranium hexafluoride. Six of the cylinders appeared to be homogeneous and had similar apparent measured uranium enrichment, as calculated by the FRAM software, at all positions. However, three cylinders appeared to have local inhomogeneity based on the observed results. This was manifested as very low apparent enrichments, often <10% of the declared enrichment, on select positions. The side with a low apparent enrichment shows elevated daughter isotope activity (e.g., elevated 1001 keV and 766 keV peak count rate) and slightly reduced 235 U activity (lower 185.7 keV count rate). We hypothesize that these heterogenous cylinders may have experienced asymmetric solar heating, which caused volatile UF 6 to sublime preferentially away from the warmed side. A similar phenomenon was observed at a second facility where dose rate measurements confirm that the “low-enriched side” of cylinders show elevated gamma ray dose rates, likely from the removal of UF 6 attenuation and concentration of daughter-products. Care should be taken during uranium enrichment verification when applying methods that include gamma-rays associated with daughter nuclides to the determination of uranium enrichment on cylinders that are stored in sunlight and have asymmetric dose readings around the cylinder.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗