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At least 127 records · Page 7

Solid Sorbent Cost Sensitivity Analysis: A Framework for UNF Reprocessing Sorbent Cost Comparison

Solid sorbents have been the subject of research and development across the U.S. Department of Energy national laboratory complex for many years. They are generally accepted as a safer alternative to cryogenic distillation for noble gas capture, and they present an easier pathway in development of long-term waste forms after iodine capture. As more types of sorbents have been proposed for capture of volatile radionuclides, it has become necessary to compare them based on performance and cost criteria. This report details cost and performance information for three promising sorbents and provides a cost sensitivity analysis. The goal of this analysis is to establish a framework which can be utilized to directly compare future sorbents, with differing properties, to the sorbents discussed in this report. Direct comparison is instrumental to making informed decisions to efficiently guide research and minimize laborious detours. In all cases, sorbent capacity is a major cost driver as it influences the mass of sorbent, operational footprint, and disposal cost requirements., However, sorbent price can greatly increase the cost of a capture technology. For sorbents used in krypton capture, the purity of krypton released to storage is the highest cost driver.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Gas diffusion through variably-water-saturated zeolitic tuff: Implications for transport following a subsurface nuclear event

Noble gas transport through geologic media has important applications in the characterization of underground nuclear explosions (UNEs). Without accurate transport models, it is nearly impossible to distinguish between xenon signatures originating from civilian nuclear facilities and UNEs. Understanding xenon transport time through the earth is a key parameter for interpreting measured xenon isotopic ratios. One of the most challenging aspects of modeling gas transport time is accounting for the effect of variable water saturation of geological media. In this study, we utilize bench-scale laboratory experiments to characterize the diffusion of krypton, xenon, and sulfur hexafluoride (SF6) through intact zeolitic tuff under different saturations. Here, we demonstrate that the water in rock cores with low partial saturation dramatically affects xenon transport time compared to that of krypton and SF6 by blocking sites in zeolitic tuff that preferentially adsorb xenon. This leads to breakthrough trends that are strongly influenced by the degree of the rock saturation. Xenon is especially susceptible to this phenomenon, a finding that is crucial to incorporate in subsurface gas transport models used for nuclear event identification. We also find that the breakthrough of SF6 diverges significantly from that of noble gases within our system. When developing field scale models, it is important to understand how the behavior of xenon deviates from chemical tracers used in the field, such as SF6 (Carrigan et al., 1996). These new insights demonstrate the critical need to consider the interplay between rock saturation and fission product sorption during transport modeling, and the importance of evaluating specific interactions between geomedia and gases of interest, which may differ from geomedia interactions with chemical tracers.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Fission gas trapped in Chornobyl fuel microparticles reveals details of reactor operations

The isotopic ratios of fission gas would provide important source information of a nuclear fuel sample found in the environment. However, it is believed that during a reactor accident like Chornobyl all fission gas is lost and that the radioactive particles found in the Chornobyl Exclusion Zone today are depleted in gases by the initial explosion and subsequent fire. We disprove this hypothesis by detection and analysis of trapped krypton and xenon in these particles. Our analysis of krypton and xenon isotopes by noble gas mass spectroscopy in combination with resonance ionization mass spectrometry establishes that important information about reactor operations like age, neutron flux and plutonium fission fraction can still be reconstructed from individual micrometer-sized particles even after decades of weathering in the environment.

Chornobyl↗

Nonlinear ionization dynamics of hot dense plasma observed in a laser-plasma amplifier

Understanding the behaviour of matter under conditions of extreme temperature, pressure, density and electromagnetic fields has profound effects on our understanding of cosmologic objects and the formation of the universe. Lacking direct access to such objects, our interpretation of observed data mainly relies on theoretical models. However, such models, which need to encompass nuclear physics, atomic physics and plasma physics over a huge dynamic range in the dimensions of energy and time, can only provide reliable information if we can benchmark them to experiments under well-defined laboratory conditions. Due to the plethora of effects occurring in this kind of highly excited matter, characterizing isolated dynamics or obtaining direct insight remains challenging. High-density plasmas are turbulent and opaque for radiation below the plasma frequency and allow only near-surface insight into ionization processes with visible wavelengths. Here, the output of a high-harmonic seeded laser-plasma amplifier using eight-fold ionized krypton as the gain medium operating at a 32.8 nm wavelength is ptychographically imaged. A complex-valued wavefront is observed in the extreme ultraviolet (XUV) beam with high resolution. Ab initio spatio-temporal Maxwell–Bloch simulations show excellent agreement with the experimental observations, revealing overionization of krypton in the plasma channel due to nonlinear laser-plasma interactions, successfully validating this four-dimensional multiscale model. This constitutes the first experimental observation of the laser ion abundance reshaping a laser-plasma amplifier. The presented approach shows the possibility of directly modelling light-plasma interactions in extreme conditions, such as those present during the early times of the universe, with direct experimental verification.

36 MATERIALS SCIENCE↗

Staged Z-pinch modeling of high and low atomic number liners compressing deuterium targets using parameters of the Z pulsed power facility

The staged Z-pinch is a potentially transformative magneto-inertial fusion energy concept where a high atomic number liner implodes on a deuterium or deuterium-tritium target using multi-MA pulsed current. Over the past several years, this concept was studied experimentally on 1 MA facilities with argon or krypton gas puffs compressing a magnetized deuterium target. Consistent thermonuclear neutron yield of 1010 per shot was measured with krypton liners. In this paper, we investigate the fusion performance of deuterium targets of varying density undergoing compression with low (beryllium) and high atomic number liners (silver, tantalum) using parameters of the Z pulsed power facility. Silver and tantalum liners create strong shocks that preheat the target plasma above 100 eV and pile up liner material at the liner-target interface. The increased mass density at the interface creates strong ram pressure just before the pinch stagnation time. The target plasma is heated to 2–4 keV, in contrast to the < 0.5 kV temperature calculated for the beryllium case. The high atomic number liners produce neutron yield orders of magnitude higher than the yield from the low atomic number liner.

Ruskov, E. (ORCID:0000000336724580)↗

Two-photon absorption laser induced fluorescence measurements of absolute neutral deuterium density, temperature, and bulk flow in Proto-MPEX

Neutral particle control is critical for fusion fueling and confinement. Neutral diagnostics for fusion-relevant plasmas are commonly restricted to line-integrated or ex situ methods. A non-perturbative, two-photon absorption laser induced fluorescence (TALIF) diagnostic is implemented on the Prototype Material Plasma Exposure eXperiment (Proto-MPEX) to probe neutral atomic deuterium in a fusion-relevant plasma at 1 cm intervals along the radius of the vacuum vessel. The diagnostic is situated ~20 m from the vacuum vessel, and a signal is collected along the laser injection axis, requiring only one line-of-sight. TALIF measurements are absolutely calibrated using xenon and krypton. Absolute atomic densities derived from xenon calibration are compared to absolute atomic densities derived from krypton calibration. In this work, preliminary measurements of absolute atomic deuterium density, temperature, and local bulk flow dependence on radial location and input power in Proto-MPEX are presented. Neutral atomic deuterium velocity distribution functions are measured throughout a one-second plasma pulse with a time resolution of 250 ms.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Strength, deformation, and the fcc–hcp phase transition in condensed Kr and Xe to the 100 GPa pressure range

The rare gas solids exhibit systematic differences in crystal structure, phase transition conditions, bond strength, and other physical properties. The physical properties of heavy rare gas solids krypton and xenon are modified by the martensitic phase transition from face-centered cubic to hexagonal close packed structure over a broad pressure range. Crystal structure, strength, and plastic deformation of krypton and xenon have been investigated at 300 K using compression in the diamond-anvil cell with synchrotron angle-dispersive x-ray diffraction and complementary ruby fluorescence spectroscopy for Xe. Stacking faults indicative of the fcc–hcp phase transition are observed at pressures at and above 1.23 ± 0.05 and 1.9 ± 0.6 GPa in Kr and Xe, respectively. The transition remains incomplete in both solids to pressures greater than 100 GPa. Strength determined from stress measurements in Pt and ruby standards at pressures up to 111 GPa and complemented by observations of strain and texture measurements obtained by x-ray diffraction in the radial geometry to 100 GPa indicates similar or higher strength than Ar at all conditions, with significant stiffening at 15–20 GPa. Radial diffraction data reveal the persistence of broad highly textured fcc diffraction lines to 101 GPa in Xe, suggesting that the axial measurements may underestimate the metastable persistence of the fcc phase due to biased sampling of hcp crystallites resulting from preferred crystallite orientation. Kr and Xe are compared with He, Ne, and Ar for a systematic understanding of physical properties and phase equilibria of rare gas solids.

Compressive stress↗

Mechanisms of Retention and Transport of Fission Products in Virgin and Irradiated Nuclear Graphite

To fulfill the design and licensing requirements for advanced reactors, the U.S. Department of Energy (DOE) is specifically interested in targeted research to quantify the mechanisms of fission product transport and retention in graphitic grades that will likely be used in next-generation very/high temperature reactors, fluoride salt-cooled high temperature reactors and molten salt reactors. We have examined an integrated experimental-computational approach to determine the diffusivities of selected fission products – ruthenium (Ru) and silver (Ag) in five nuclear graphite grades – POCO AXF-5Q, POCO ZXF-5Q, PCEA, IG110, and NBG-18. Experimental investigation for diffusion of other fission products (iodine, cesium, and krypton) in graphite could not be carried out due to extreme evaporation due to high vapor pressure, despite several attempts incorporating various experimental schemes. Experimental investigation with irradiated graphite could not be carried out because necessary approval to transport irradiated graphite could not be obtained due to procedural reasons at ORNL and national policy change in UK. An effort was made to “produce” by ion sputtering, but it was discontinued because the outcome did not adequately represent irradiated graphite. Thin film and “cup-and-cap” methods were employed to deposit fission products, diffusion annealed were carried out in an argon atmosphere, and concentration profiles were determined by dynamic secondary ion mass spectroscopy depth profiling technique. Regardless of graphite type, anomalous diffusion behavior of Ru (i.e., lower than expected based on Arrhenius temperature dependence) at an intermediate temperature, around 600 to 700 °C, was observed. Diffusion behavior of silver on the other hand agreed well to the Arrhenius temperature dependence although the excessive evaporation of silver hampered the accurate determination of diffusivities at temperature higher than 900 °C. In general, silver was observed to diffuse faster than Ru in the temperature range compared from 500 to 900 °C, had consistently had higher pre-exponential factor corresponding to higher jump frequency. To understand the abnormal diffusional behavior of Ru in graphite in intermediate temperature range, a detailed microstructural analysis was carried out. Clustering of Ru into particles on the surface of graphite was observed around 700 °C corresponding to de-wetting and spheroidization. This change would influence the boundary condition of diffusion, although features of clustering was much smaller (<1 mm) than the SIMS raster size (120 x 120 mm). Raman spectroscopy also demonstrated that Raman peak intensity for Ru decreased significantly for samples annealed higher than 700 °C and presence of Ru in graphite altered the crystallinity of graphite. To further elucidate the abnormal diffusion behavior observed in intermediate temperature investigated, the vibrational properties of graphene, bilayer graphene and Kr atoms in bilayer graphene were investigated with molecular dynamics. Krypton, which is a fission product, was introduced between a bilayer graphene system to evaluate (i) whether the phonon dispersion curves change with high temperature in bilayer graphene (ii) whether the addition of Kr atoms between the bilayer introduces any significant change in the vibrational properties, and (iii) whether any change in the vibrational properties can be correlated to the diffusive behavior of Kr atoms. The results show that the Kr atoms indeed exhibit an anomalous diffusive behavior at 550°C. Phonon analysis shows that a few phonon frequencies are enhanced as much as 20 to 30 % with the addition of just 0.2 at.% Kr. So, this may explain the unexpected self-diffusivity of fission products.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Operation of an electron-bombardment ion source using various gases

An electron-bombardment ion thruster of the SERT 2 type was operated with xenon, krypton, argon, neon, nitrogen, helium, and carbon dioxide. The discharge performance with xenon, krypton, and argon was similar to that obtained previously with mercury. Mass spectrometer data indicated that the xenon contained no significant multiple ionization. Restriction of the beam area, with an associated decrease in discharge potential, was necessary to reduce multiple ionization with argon to a negligible level. This modification also resulted in more stable operation of the thruster. Performance with the remaining gases was poor because the basic thruster designed was optimized for operation with mercury.

Byers, D. C.↗

Electron-bombardment ion source operation using various gases.

Description of a modified flight-type SERT II ion thruster operated with xenon, krypton, argon, neon, nitrogen, helium, and carbon dioxide. The discharge performance with xenon, krypton, and argon was found to be similar to that obtained previously with mercury. Mass spectrometer data indicated that xenon could be operated efficiently with no significant multiple ionization. Restriction of the beam area, with an associated decrease in discharge potential, was necessary to reduce multiple ionization with argon to a negligible level. This modification also resulted in more stable operation of the thruster. Performance with the remaining gases was poor, but some future performance improvements may be realizable.

Byers, D. C.↗

Driving lamps by induction

An electrodeless lamp circuit with a coil surrounding a krypton lamp is driven by an RF input source. A coil surrounding a mercury lamp is tapped across the connection of the input central to the krypton-lamp coil. Each coil is connected in parallel with separate capacitors which form resonant circuits at the input frequency.

Laue, H. H.↗

Rare-gas analyses on neutron irradiated Apollo 12 samples.

Argon, krypton, and xenon from stepwise heating of five Apollo 12 rocks that had been irradiated to a neutron fluence of about 10 to the 19th neutrons/sq cm were analyzed mass-spectrometrically. The Ar40-Ar39 ages were determined and range from 3.18 plus or minus 0.06 x 10 to the 9th years to 3.32 plus or minus 0.06 x 10 to the 9th years. Trace elements Ba, Br, I, and U were measured via the neutron-induced reactions that produce isotopes of krypton and xenon. The following concentration ranges were observed: Ba, 46 to 70 ppm; Br, 48 to 146 ppb; I, 16 to 73 ppb; and U, 170 to 247 ppb.

Alexander, E. C., Jr.↗

The atmosphere of Mars near the surface - Isotope ratios and upper limits on noble gases

Several analyses of the Martian atmosphere have been carried out with the mass spectrometer in the molecular-analysis experiment. The ratios of abundant isotopes of carbon and oxygen are within 10 per cent of terrestrial values, whereas nitrogen-15 is considerably enriched on Mars. Argon-38 has been detected, and new limits on abundances of krypton and xenon have been set. The limit on krypton is sufficiently low to suggest that the inventories of volatile substances on Mars and on earth may be distinctly different.

Biemann, K.↗

Volumetric direct nuclear pumped laser

A volumetric direct nuclear pumped laser was developed in which the gas is a mixture of He-3 and a minority gas from the group of argon, krypton, xenon, chlorine and fluorine. The mixture of He-3 and the minority gas produces lasing with a minority gas concentration of from 0.01 to 10 percent argon, 1 percent krypton, 0.01 to 5 percent xenon and small concentrations of chlorine or fluorine.

Jalufka, N. W.↗

Quantum-chemical modeling of boron and noble gas dopants in silicon

The electron effects of the presence of boron and noble gas dopants in a model silicon lattice were investigated using a self-consistent charge extended Hueckel program. The extent of electronic interaction of the noble gas with the lattice is given by: Kr greater than Ar greater than Ne. Theoretically, boron diffusion in the presence of neon, argon or krypton was examined using a self-consistent charge extended Hueckel program. The net energy of interaction between boron and neon is strongly repulsive while argon-boron exhibits a region of relative stability; krypton exhibits behavior similar to argon though no region of stability was found for the range of separations used in the calculations. Finally, it is noted, from the relative energy of the topmost filled molecular orbital associated with boron (in an interstitial position), that activation of the boron does not require boron movement but can be accomplished by indirect transitions.

Aronowitz, S.↗

Development of a mass spectrometer system for the measurement of inert gases in meteorites

The study of the inert gases in meteorites has provided many clues as to the origin and evolution of the solar system. Particularly crucial and complex are the gases krypton and xenon. To accurately measure the isotopic compositions of these gases requires a mass spectrometer of high sensitivity and resolution. A previously unused and largely untested mass spectrometer system was brought to the point where it was ready for routine sample analyses. This involved, among other things, focusing the ion beam for optimal peak shape and sensitivity, documenting the instrument's response to a series of characteristic tests such as multplier gain checks, and interfacing the instrument to a computer to run the sample analyses. Following this testing and setting up, three iron meteorite samples were to be analyzed for argon, krypton, and xenon. The three samples were shown in prior work to possibly contain primordial heavy inert gases. Although these analyses have not yet been carried out, it is anticipated that they will be completed in the near future.

Palma, R. L.↗

A study of single and binary ion plasma expansion into laboratory-generated plasma wakes

Plasma expansion into the wake of a large rectangular plate immersed in a collisionless, supersonic plasma was investigated in laboratory experiments. The experimental conditions address both single ion and binary ion plasma flows for the case of a body whose size is large in comparison with the Debye length, when the potential difference between the body and the plasma is relatively small. A new plasma source was developed to generate equi-velocity, binary ion plasma flows, which allows access to new parameter space that have previously been unavailable for laboratory studies. Specifically, the new parameters are the ionic mass ratio and the ionic component density ratio. In a series of experiments, a krypton-neon plasma is employed where the ambient density ratio of neon to krypton is varied more than an order of magnitude. The expansion in both the single ion and binary ion plasma cases is limited to early times, i.e., a few ion plasma periods, by the combination of plasma density, plasma drift speed, and vacuum chamber size, which prevented detailed comparison with self-similar theory.

Wright, Kenneth Herbert, Jr.↗

Volatile inventory of Mars-2: Primordial sources and fractionating processes

The total volatile inventory of Mars has been modeled using meteoritic and presumed primordial abundances in the early solar system. Evidence is presented which indicates that the elemental abundances of the noble gases on Earth and Mars are similar, and their ratios are comparable to those in average carbonaceous chondrites with the exception of xenon and krypton. In order to account for presently observed variations in gas abundances, two primordial sources were used. One was the solar composition similar to the solar wind, and the other of carbonaceous grains that were the source for trace exotic components. For Mars, a model in which the early, high solar EUV flux with continued hydrogen production by differentiation results in mass fractionation of the primordial atmosphere, early depletion of xenon, and later depletion of gases lighter than krypton. The result is that the primordial Mars water inventory may have been on the order of 20 to 30 km if spread over the planet.

Pepin, R. O.↗