TMS 2021: USE OF AN INFRARED SPECTROSCOPIC METHOD FOR ISOTOPIC ANALYSIS OF GASEOUS URANIUM HEXAFLUORIDE
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FESSLER, KIMBERLY A↗
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The Reduction and Recovery of Uranium Hexafluoride from 1-Methyl-1-Propylpiperidinium Bis(trifluoromethylsulfonyl)imide
Collaborative presentation between MSTS and UNLV.
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
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.↗
The Use of Heavy Gas for Increased Reynolds Numbers in Transonic Wind Tunnels
The use of a high molecular weight test gas to increase the Reynolds number range of transonic wind tunnels is explored. Modifications to a small transonic wind tunnel are described and the real gas properties of the example heavy gas (sulfur hexafluoride) are discussed. Sulfur hexafluoride is shown to increase the test Reynolds number by a factor of more than 2 over air at the same Mach number. Experimental and computational pressure distributions on an advanced supercritical airfoil configuration at Mach 0.7 in both sulfur hexafluoride and nitrogen are presented. Transonic similarity theory is shown to be partially successful in transforming the heavy gas results to equivalent nitrogen (air) results, provided the correct definition of gamma is used.
Anders, J. B.↗
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 ↗
Reactions of Atomic Thorium and Uranium Cations with SF 6 Studied by Guided Ion Beam Tandem Mass Spectrometry
The fundamental chemistry of the thorium and uranium fluorides continues to be an area of interest because of the use of thorium and uranium fluoride compounds in nuclear fuel systems. Here, we study the reaction of thorium cations with sulfur hexafluoride for the first time and revisit the reaction of uranium cations with sulfur hexafluoride. By using guided ion beam tandem mass spectrometry, we explore the reaction pathways that become accessible well above thermal energies (E ~ 0.04 eV). Overall, we find that both Th + and U + react very efficiently with SF 6 , approaching the collision limit at both thermal and elevated energies. Here, the primary products observed at low energies include Th 1–3 + , UF 1–4 + , and SF 1–4 + , all of which are formed in barrierless, exothermic processes. SF 5 + was also observed, although the pressure dependence of this channel reveals that SF 5 + forms exothermically through secondary reactions, which the energy dependences suggest result from reactions between ThF 2 + and UF 3 + with SF 6 . At higher energies, both AnF 3 + products are observed to decay to AnF + + F 2 and both SF 4 + and SF 2 + exhibit cross sections with endothermic features. For both systems, the rise in SF 4 + can be attributed to a secondary collision between AnF + with SF 6 on the basis of the pressure dependence of the SF 4 + channel at higher energies and the rise in SF 2 + appears to result from the decomposition of SF 3 + to SF 2 + + F.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
LiPF 6 under pressure: a symmetry-mode-based structural analysis
The lithium salt LiPF 6 is a key component in commercial lithium-ion battery (LIB) electrolytes. However, its structural properties under pressure remain unexplored, despite increasing interest in the effect of pressure on electrolyte behaviour, and a growing interest in high pressure synthesis of new Li-hexafluoride cathode materials. Here, we present the first high pressure neutron diffraction study of solid LiPF 6 up to 7.4 GPa. Refinements reveal that the ambient rhombohedral structure (space group R$\overline{3}$) remains stable throughout, with pressure accommodated primarily by tilting of the corner-shared LiF 6 and PF 6 octahedra and contraction of the LiF 6 units. In conclusion, this study establishes a foundation for understanding the phase behaviour of Li-based hexafluorides under extreme conditions.
25 ENERGY STORAGE↗
Lasers from fission
The feasibility of the nuclear pumping of lasers was demonstrated in three experiments conducted independently at three different laboratories. In this context nuclear pumping of lasers is understood to be the excitation of a laser by the kinetic energy of the fission fragments only. A description is given of research concerned with the use of nuclear energy for the excitation of gas lasers. Experimental work was supplemented by theoretical research. Attention is given to a nuclear pumped He-Xe laser, a nuclear pumped CO laser, and a neon-nitrogen laser pumped by alpha particles. Studies involving uranium hexafluoride admixture to laser media are discussed along with research on uranium hexafluoride-fueled reactors.
Schneider, R. T.↗
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.↗
CO2 laser-driven Stirling engine
A 100-W Beale free-piston Stirling engine was powered remotely by a CO2 laser for long periods of time. The engine ran on both continuous-wave and pulse laser input. The working fluid was helium doped with small quantities of sulfur hexafluoride, SF6. The CO2 radiation was absorbed by the vibrational modes of the sulfur hexafluoride, which in turn transferred the energy to the helium to drive the engine. Electrical energy was obtained from a linear alternator attached to the piston of the engine. Engine pressures, volumes, and temperatures were measured to determine engine performance. It was found that the pulse radiation mode was more efficient than the continuous-wave mode. An analysis of the engine heat consumption indicated that heat losses around the cylinder and the window used to transmit the beam into the engine accounted for nearly half the energy input. The overall efficiency, that is, electrical output to laser input, was approximately 0.75%. However, this experiment was not designed for high efficiency but only to demonstrate the concept of a laser-driven engine. Based on this experiment, the engine could be modified to achieve efficiencies of perhaps 25-30%.
Lee, G.↗
Evaluation of a storable fluorine based pilot for scramjets
An ignitor/pilot device for scramjet engines has been tested with C2H4, C2H6, and CH4 gaseous hydrocarbon fuels at Mach 2. The pilot was designed to operate with storable nontoxic propellants rather than hazardous pyrophorics; the pilot fluid is a mixture of ethylene, oxygen, and sulfur hexafluoride. The pilot reduced the minimum temperature at which all three hydrocarbon fuels ignited; a comparison was then conducted between combustion efficiency calculations for these test results and those of pilots using nitrogen in place of sulfur hexafluoride, and using silane-hydrogen (yielding equivalent energy). The nitrogen-substituted pilot exhibited the highest efficiency.
Diskin, G. S.↗
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↗
Cylinder Occupancy and Measurement Suite
This software automatically records data from the Unattended Cylinder Verification Station, determines the state of the instrument, captures images of uranium hexafluoride shipment cylinders, and determines their weight. The code has been developed primarily for the International Atomic Energy Agency, but this type of instrument could be of interest to any facility operator in the uranium supply chain that handles uranium hexafluoride shipment cylinders (e.g. the 30B and 48Y cylinder). Operators may be interested in having this instrument confirm shipper declared measurement values upon receipt of a cylinder. They may also use it to aid in process monitoring if the quantity of material in the cylinder changes due to a processing activity.
Stewart, Scott L↗
Fractionation of UF6 and daughter progeny in storage cylinders from external heating
Abstract Uranium hexafluoride (UF 6 ) is a significant concern for material accountancy and verification in the international safeguards community. Verification of the contents of UF 6 cylinders is generally attempted with gamma spectroscopy but the current methods assume a uniform, homogeneous UF 6 mass distribution within the cylinder. In this work, it was found experimentally and confirmed via modeling, that under an external heat load (the sun), the UF 6 and its daughter products undergo fractionation in the cylinder. This fractionation of the UF 6 and daughter products can cause an errant measurement of the enrichment of the cylinder when using the current verification methods.
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
Cell design for laser-induced breakdown spectroscopy measurements on reactive gas samples
Uranium hexafluoride (UF 6 ) is the primary material used for the enrichment of uranium in the production of light water nuclear reactor fuels worldwide. Accurate, rapid quantification of uranium isotopic composition in nuclear materials is required for safeguards programs and nonproliferation purposes. One potential technique for isotopic measurements in uranium species in the field is laser induced breakdown spectroscopy (LIBS). Safe and effective application of LIBS to UF 6 for enrichment measurements is uniquely challenging due to the chemical and physical properties of UF 6 , which necessitate specific handling procedures. The objective of this work is to design a cell for isotopic analysis of UF 6 that is (1) compatible with chemical and physical properties of UF 6 , (2) compatible with LIBS laser, and (3) portable-sized for nuclear safeguards applications. Along with cell design, initial testing of the cell for basic performance and chemical compatibility is performed. As designed and constructed, the portable gas cell was gas-tight, chemically compatible with UF 6 , and withstood long-duration laser exposure. In this work, the cell has proven capability for handling reactive gasses, such as UF 6 , with specification application to isotopic analysis.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Sensitivity of the simulation of passive neutron emission from UF 6 cylinders to the uncertainties in both 19 F(α,n) energy spectrum and thick target yield of 234 U in UF 6
Interest in safeguards verification measurements using passive thermal neutron counting to assay 235 U content in large 30B UF 6 canisters has grown in recent years. Here, the prohibitively high cost and impracticality of using reference 30B calibration cylinders extensively will likely make accurate simulations of increasing interest. Accuracy of the simulated response will define the confidence in the predicted response and the extent to which simulations can reasonably be relied upon. With 234 U driven 19 F(α, n) reactions being the main neutron source in low enriched UF 6 the uncertainties of the 19 F(α, n) energy spectrum and the thick target yield of 234 U in UF 6 propagate into the uncertainty in the predicted response and represent a major influence of basic nuclear data. Here sensitivity of the simulated total (Singles) and coincidence (Doubles) count rates are assessed for the Passive Neutron Enrichment Meter using six potential 19 F(α, n) neutron energy spectra over a range of enrichments and material distributions. The results indicate that variations in the Singles and Doubles due to simulated (α, n) neutron spectrum are less than 1.5% for this set of simulated neutron spectra, with dependence varying inversely with enrichment. Singles uncertainty is only slightly less than that of the thick target 19 F(α, n) yield corresponding to the primary neutron source, whereas the 19 F(α, n) yield dependence of the Doubles is reduced by the non-negligible 238 U(SF) coincident neutron emissions. Based on available thick target 19 F(α, n) yield estimates the uncertainty is on the order of 5%, establishing this as the main nuclear data limitation when simulating thermal neutron detectors response for 30B UF 6 storage cylinders. Based on these findings, it appears that the measurement and evaluation of the thick target 19 F(α, n) yield for uranium hexafluoride is due.
19F(α,n) neutron spectrum↗
Morphological Characterization of Uranyl Fluoride Particles via Atomic Force Microscopy
Uranium hexafluoride (UF 6 ) undergoes a rapid hydrolysis reaction when exposed to atmospheric water. In addition to producing hazardous HF gas, the hydrolysis reaction produces uranyl fluoride (UO 2 F 2 ), a radioactive solid phase particulate material. Because of the technological utility of UF 6 in the nuclear fuel cycle, understanding the transport properties of UO 2 F 2 aerosol produced via UF 6 hydrolysis is important for accident scenarios. Moreover, the fundamental chemical and physical properties of the UF 6 hydrolysis reaction are not completely understood. Recently, several experiments on the aerosol phase properties of UO 2 F 2 produced in this way have shown that under most relevant conditions, the particle size distribution (PSD) of UO 2 F 2 can be extremely small, approximately 3 to 5 nm, which is well below the threshold that can be routinely observed via scanning electron microscopy (SEM). Although readily observable in the aerosol phase, observation of nanometer-sized particles in the condensed phase (i.e. deposited on surfaces) remains a challenge. Here, in this study, we have used atomic force microscopy (AFM) to study the PSD and morphological characteristics of UO 2 F 2 deposited at low and high concentrations under different humidity conditions, a primary variable in the hydrolysis reaction. Here, we find strong agreement between PSD measured in the aerosol phase via scanning mobility particle sizing and PSD measured via AFM, with particle sizes peaked below 4 nm for low-humidity conditions. At higher humidity, the distribution is centered around 5 to 10 nm but extends up to 20 nm. These results are in stark contrast to previous measurements using SEM that show PSD on the order of 300- to 1000-nm particle sizes; moreover, these are the first direct measurements of individual particles of UO 2 F 2 having been produced via UF 6 hydrolysis deposited on surfaces. These measurements, therefore, open a new avenue for collecting and detecting UO 2 F 2 in the condensed phase and further refine the PSD, which is critical for environmental transport determinations.
Uranium hexafluoride↗