Conversion of uranium hexafluoride and recovery of uranium from ionic liquids
Described are methods for the recovery of uranium from uranium hexafluoride dissolved directly into ionic liquids.
Hatchett, David W.↗
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Investigation of an r-f radiant energy source with uranium hexafluoride and tungsten hexafluoride injection.
An experimental investigation was conducted using the UARL 1.2-megw r-f induction heater to simulate thermal environment and fuel region characteristics expected in nuclear light bulb reactors. Argon was injected at the ends of the test chamber to provide radial-inflow vortex flow pattern. In some tests, simulated fuel consisting of a mixture of argon gas with either tungsten hexafluoride gas, uranium hexafluoride gas, or tungsten particles was injected into the discharge region from probes located at the centers of the end walls. The encouraging initial results obtained are discussed.
Roman, W. C.↗
Online monitoring the hydrolysis of uranium hexafluoride for intermediates by cryogenic layering and FTIR
Uranium hexafluoride (UF 6 ) is a commonly utilized material feedstock in uranium enrichment processes due to its high vapor pressure and ease of sublimation. When exposed to air, UF 6 undergoes spontaneous hydrolysis to form uranyl fluoride (UO 2 F 2 ) particulates which are utilized for the detection of undeclared nuclear activities by nuclear safeguards organizations. In this study, the kinetics of the hydrolysis reaction and how they relate to particle morphology of the product are still debated in the literature. Here, we report the direct, in situ observation of UF 6 reaction intermediates by cooling the reaction to cryogenic temperatures to significantly reduce the rate of hydrolysis. The reaction is then observable by Fourier transform infrared (FTIR) spectroscopy. The conversion of UF 6 to UOF 4 is observed as well as several other bands associated with possible long lived intermediate complexes. Chemometrics are used to further elucidate the reaction pathway from UF 6 to UO 2 F 2 .
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
Spectral emission characteristics near 646 nm and plasma properties of laser-induced plasma of gaseous uranium hexafluoride
We present a detailed investigation of the temporal evolution of line and continuum emissions in laser-induced breakdown spectroscopy (LIBS) of gaseous uranium hexafluoride (UF 6 ), focusing on the spectral region near 646 nm. Spectral emission features, signal-to-background ratios (SBRs) of selected uranium lines, and spectral linewidths were examined under varying UF 6 pressures (15–60 Torr) and laser pulse energies (10–60 mJ). Higher pressures and pulse energies enhanced continuum emission and reduced SBRs but did not cause significant spectral congestion. Additional studies with the use of different laser systems, including nanosecond-pulsed Nd:YAG lasers (at fundamental and various harmonics) and a femtosecond-pulsed Ti:sapphire laser, revealed long-lived plasma continua in all cases. This persistent continuum is attributed to a pseudo-continuum from overlapping molecular emissions, as its intensity scales linearly with electron number density, deviating from the expected quadratic dependence of classical ion–electron interactions for free-free and free-bound continuum emission. Based on plasma persistence time, SBR, U II/U I intensity ratios, and electronic excitation temperature, no fundamental advantage was found for femtosecond-pulsed lasers over conventional nanosecond-pulsed ones for UF 6 enrichment assay with direct LIBS measurement.
Laser-induced breakdown spectroscopy↗
Parametric analyses of planned flowing uranium hexafluoride critical experiments
Analytical investigations were conducted to determine preliminary design and operating characteristics of flowing uranium hexafluoride (UF6) gaseous nuclear reactor experiments in which a hybrid core configuration comprised of UF6 gas and a region of solid fuel will be employed. The investigations are part of a planned program to perform a series of experiments of increasing performance, culminating in an approximately 5 MW fissioning uranium plasma experiment. A preliminary design is described for an argon buffer gas confined, UF6 flow loop system for future use in flowing critical experiments. Initial calculations to estimate the operating characteristics of the gaseous fissioning UF6 in a confined flow test at a pressure of 4 atm, indicate temperature increases of approximately 100 and 1000 K in the UF6 may be obtained for total test power levels of 100 kW and 1 MW for test times of 320 and 32 sec, respectively.
Rodgers, R. J.↗
Studies of Helium Behavior in Uranium Hexafluoride
Several issues have arisen from experimental observations and/or theoretical postulation related to the behavior of helium in uranium hexafluoride (UF 6 ) matrices and how it may impact the ability to use this noble gas to quantify the fill date of the cylinder. A series of experiments was conducted to address several such issues, and the results and implications are reported here. Two issues relate to bias in the helium measurement due to ambient air from extraneous sources such as atmospheric air or from potential holdup in a large, activated alumina chemical trap. These issues are really a question of differential retention of helium versus three other inert gas isotopes (representative of other noble gases found in air) used as a calibration for air in leakage. Discernable bias was not detected in either case. Another issue had to do with helium potentially brought into the cylinder by a liquid UF 6 fill and subsequently released as the material solidifies and/or during storage. The solubility of helium in liquid UF 6 was measured to investigate this theory. The experiment quantified the potential magnitude of the initial helium contribution if present. The final issue was that of retention of helium in solid UF 6 . Investigation of this theory necessitated quantifying both the solubility and the diffusivity of helium in UF 6 . In one experiment, the solubility was measured at cryogenic temperature, allowing quantification of helium in solid UF 6 such as would be found in a cold trap. In a second experiment, transport of helium into and through a macroscopic plug of solid UF 6 was examined. The transport was very slight although apparently detectible. Effectively, only an upper limit to the transport could be determined, but that limit implied that helium holdup in solid UF 6 is a real possibility.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Uranium Hexafluoride Hydrolysis Reaction Dynamics from Cryogenic Layering, FTIR Spectroscopy, and Isotopic Substitution
The first direct evidence that the hydrolysis reaction of uranium hexafluoride (UF 6 ) follows multiple competing pathways which are driven by the ratio of water to UF 6 , temperature, and isotopic composition is presented. Using temperature dependent infrared spectroscopy, it is shown the hydrolysis can be prevented at temperatures below 150 K, and that water-rich environments promote the formation of uranium oxyfluoride intermediates. Spectral shifts reveal isomeric transitions and the growth of polymeric species, with reaction reversibility observed at high water concentrations. Additionally, controlled heating rates affect the emergence of intermediates. The final particulate product consistently forms as uranyl fluoride hydrate, though its morphology and spectral signature vary with reaction conditions and annealing. These findings help clarify long-standing uncertainties surrounding UF 6 hydrolysis.
Chemical reactions↗
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.↗
Understanding Uranium Hexafluoride (UF6) Chemistry for Nuclear Safeguards and Nonproliferation
Louis McNamara
Nonproliferation↗
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.↗
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 ↗
Gaseous fuel reactor research
The paper reviews studies dealing with the concept of a gaseous fuel reactor and describes the structure and plans of the current NASA research program of experiments on uranium hexafluoride systems and uranium plasma systems. Results of research into the basic properties of uranium plasmas and fissioning gases are reported. The nuclear pumped laser is described, and the main results of experiments with these devices are summarized.
Thom, K.↗
Vacuum ultraviolet spectra of uranium hexafluoride/argon mixtures
The transmission properties of room temperature helium at pressures up to 20 atmospheres were determined in the wavelength range from 80 to 300 nm. Similarly, the transmission properties of uranium hexafluoride at 393 K (pressures less than 1.0 mm) were determined in the wavelength range from 80 to about 120 nm. The results show that high pressure helium is sufficiently transparent in the vacuum ultraviolet region (provided trace contaminants are removed) to be utilized as a transparent purge gas in future fissioning gaseous uranium plasma reactor experiments. Absorption cross sections for uranium hexafluoride were calculated from the data between 80 and 120 nm and were of the order of 10 to the -17 power sq cm.
Krascella, N. L.↗
Recent measurements concerning uranium hexafluoride-electron collision processes
Scattering of electrons by UF6 molecules was studied at impact energies ranging from 5 to 100 eV and momentum transfer, elastic and inelastic scattering cross sections were determined. The measurements also yielded spectroscopic information which made possible to extend the optical absorption cross sections from 2000 angstroms to 435 angstroms. It was found that UF6 is a very strong absorber in the vacuum UV region. No transitions were found to lie below the onset of the optically detected 3.0 eV feature.
Trajmar, S.↗