Noble Gas Capture [Slides]
Presentation slides detailing campaign activities and planning.
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
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Fine-Tuning Microporosity of Crystalline Vanadomolybdate Frameworks for Selective Adsorptive Separation of Kr from Xe
Selective adsorptive capture and separation of chemically inert krypton (Kr) and xenon (Xe) noble gases with very low ppmv concentrations in air and industrial off-gases constitute an important technological challenge. Here, using a synergistic combination of experiment and theory, the microporous crystalline vanadomolybdates (MoVO x ) as highly selective Kr sorbents are studied in detail. By varying the Mo/V ratios, we show for the first time that their one-dimensional (1D) pores can be fine-tuned for the size-selective adsorption of Kr over the larger Xe with selectivities reaching >100. Using extensive electronic structure calculations and grand canonical Monte Carlo simulations, the competition between Kr uptake with CO 2 and N 2 was also investigated. As most materials reported so far are selective toward the larger, more polarizable Xe than Kr, this work constitutes an important step toward robust Kr-selective sorbent materials. Furthermore this work highlights the potential use of porous crystalline transition metal oxides as energy-efficient and selective noble gas capture sorbents for industrial applications.
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
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↗
Xenon Isotopic Analysis of Individual Intermediate Particles From the OSIRIS-REx Sample of Asteroid Bennu
The OSIRIS-REx mission sampled material from the B-type asteroid Bennu and delivered the sample to Earth on 24 September 2023. Here we present initial xenon isotopic analysis of individual intermediate particles of Bennu material collected by the OSIRIS-REx mission. Noble gases are key tracers of Solar System evolution. Xenon is particularly useful among the noble gases because its nine isotopes allow multiple contributing sources to be unambiguously identified. The sun, asteroids (as measured in meteorites), and comets (measured in the coma of comet 67P) have distinct xenon isotopic signatures reflecting different mixtures of nucleosynthetic components. In addition, 129 I, 238 U, and 244 Pu decay with different half-lives, producing characteristic xenon signatures. Exposure of samples containing light rare earth elements and barium to cosmic rays produces xenon from spallation and secondary neutron capture reaction. Noble gas analyses help address several of the driving hypotheses of the mission [9]. Particle-by-particle analysis can elucidate the diversity of material present and reveal distinct noble gas compositions, including the potential to detect presolar or cometary noble gas signatures on a small scale. The isotopic signature provides a fingerprint that can be used to constrain the sources of volatiles in planetary reservoirs and combined with other information (e.g. mineralogy and petrology of the material analyses) contributes to our understanding of the initial constituents, formation, and history of Bennu and its parent asteroid.
S A Crowther↗
Degassing history of Mars from Martian atmosphere samples
A comparison of the abundances of Ar-40 and He-4 (radiogenic) in various terrestrial planetary atmospheres provides clues to the volcanic and tectonic histories of the planets while the amount of primordial noble gases in the planetary atmospheres provides clues to the quantities of volatile rich materials captured by each planet. The noble gas contents of Mars, Earth, and Venus clearly show that the absolute abundances of isotopes of gases are directly proportional to the amounts of degassed CO2 into the planetary atmosphere. Several basic geological units can be seen on the global geological map of Mars. The enormous size of volcanic and tectonic structures of Mars, despite its smaller size, provide invaluable clues to the degassing history of Mars. Therefore, the collection of samples of Martian atmosphere and soil volatiles is imperative to understand the origin and evolution of the atmosphere and its interaction with the Martian surface. Surface properties of Martian rocks, soils, breccias, and regolith and their chemistry are also generic to any discussion on the origin and evolution of the atmosphere of Mars. The differences in absolute abundances of gases in the planetary atmospheres are amenable to many alternative interpretations. These alternative interpretations can be tested by imposing additional constraints derived from the isotopic results of noble gases in the atmospheres of the planets.
Rao, A. S. P.↗
ASC Poster - Concentration of Xe from Simulated Dissolver Off-gas Streams Utilizing a Solid Sorbent, AgZ-PAN
Idaho National Laboratory (INL) has developed and tested engineered sorbents to separate and capture volatile fission products such iodine (I), xenon (Xe), and krypton (Kr) from off-gas streams. As noble gases, Xe and Kr can be difficult to capture and separate. Historically, cryogenic distillation has been used to execute the separation, but this method can pose significant hazards. INL has successfully developed two sorbents for Xe and Kr capture, silver mordenite polyacrylonitrile (AgZ-PAN) and hydrogen mordenite polyacrylonitrile (HZ-PAN). Adsorption studies to date successfully separated and captured Xe from carrier gas streams, but those studies focused primarily on initial separation and capture. In addition, the ability to concentrate Xe through multiple adsorption and desorption cycles has not been studied and therefore is the focus on this presentation. Concentrating Xe during desorption is ideal to produce Xe that can be used for commercial and research applications.
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
Understanding MOF Gas Entrapment Through Modeling
Metal organic frameworks (MOF) were created for the capture of noble gases (NG). They were tested to see which would be the most efficient and selective. MOFs are synthetic materials that are used in a variety of purposes: gas separations, catalysis reactions, drug delivery, and gas storage. In a previous study, there was an extremely long retention time of NG within the Ca-MOF material. Between 30-65 % of the NG was never recovered even under vacuum and at 150 °C. An understanding of this retention at a fundamental level is needed for utilizing the MOF material in industry or other applications
Metal organic frameworks↗
Anomalous krypton in the Allende meteorite
The reported investigation provides important new data for the heavy noble gases, especially Kr, in the Allende meteorite. The data are used to criticize the original model of Lewis et al. (1975) based on the noble gas data of these researchers. The conclusions reached in the investigation support alternative models which have been mainly based on Xe data by Lewis et al. (1975, 1977). Because of the relatively high noble gas abundances in the separates studied, disturbance from nuclear effects occurring in situ such as spallation and neutron capture is insignificant, offering an opportunity to study primordial Ar, Kr, and Xe. The isotopic and abundance data obtained from the samples largely confirm the noble gas results of Lewis et al. (1975, 1977) where isotopic correlations agree with the correlations of the considered samples. It is found that both Kr and Xe data are consistent with a two component mixture of 'ordinary' as well as 'anomalous' planetary gases.
Frick, U.↗
Nucleogenic noble gas components in the Cape York iron meteorite
The paper reports data on neutron capture products of the secondary cosmic ray component, the inferred proton and neutron fluences, and the identification of double beta decay of Se-82 in heavily shielded samples of the Cape York iron meteorite. One purpose of this study is to develop a new chronometer for cosmic ray exposure, based on the nuclides I-129 (16 My half-life) and Xe-129 from low energy cosmic ray reactions on Te. The abundance ratio of these two nuclides permits the determination of an (effective) exposure age of 93 + or - 16 My, which represents the first exposure age datum of Cape York. The very small concentrations of spallogenic Ar-38 = 6.5 x 10 to the -10th cu cm STP/g in the metal and troilite (per g Fe) document the heavily shielded locations of the sample. An excess of Xe-129 in the troilite is shown to be entirely due to the decay of cosmic-ray-produced I-129. On the other hand, an inclusion in the troilite reveals the presence of Xe-129 from extinct I-129 and documents its about 4.5 Gy formation age. Mono-isotopic excess of Kr-82 is identified as due to beta-beta-decay of Se-82 with an inferred half-life of 1.0 x 10 to the 20th y. This represents the first beta-beta-decay product observed in a meteorite.
Murty, S. V. S.↗
The low-energy secondary cosmic ray flux: Detectors in iron meteorites
The cosmic ray-produced nuclides in the interiors of very large bodies are mainly due to secondary particle reactions. The records of low-energy products, specifically the neutron capture products in meteorites, may provide new information regarding multi-stage irradiation and parent body break-ups. Noble gas nuclides, in general, are the best candidates for these investigations. The troilite nodules of iron meteorites contain very low amounts of trapped gas and, because of their elemental abundance systematics of suitable target elements for low energy production of noble gas nuclides, they are ideal candidates for this purposes. Results of a study of noble gases and nitrogen in a troilite nodule of the Cape York iron are presented.
Murty, S. V. S.↗
Characterizing Uranus with an Ice giant Planetary Origins Probe (Ice-POP)
We now know from studies of planetary transits and microlensing that Neptune-mass planets are ubitquitous and may be the most common class of planets in the Galaxy. As such it is crucial that we understand the formation and evolution of the ice giant planets in our own solar system so that we can better understand planet formation throughout the galaxy. An entry probe mission to Uranus would help accomplish this goal. In fact the Planetary Decadal Survey recommended a Uranus orbiter with entry probe but did not explore in detail the specifications for the entry probe. NASA Ames is currently studying thermal protection system requirements for such a mission and this has led to questions regarding the minimum interesting science payload of such an entry probe. The single most important in-situ measurement for an ice giant entry probe is a measurement of atmospheric composition. For Uranus this would specifically include the methane and noble gas abundances. An in situ measurement of the methane abundance, from below the methane cloud, would constrain the atmospheric carbon abundance, which is believed to be roughly 30 to 50 times solar. There are hints from the transiting planets that extrasolar ice giants show comparable or even greater enhancements of heavy elements compared to their primary stars. However the origin of this carbon enhancement is controversial. Is Uranus a "failed core" of a larger gas giant or was the atmosphere enhanced by accretion of icy planetesimals' Constraining atmospheric abundances of C and perhaps S or even N from below 5 bars would provide badly needed data to address such issues. A measurement of the N abundance would provide clues on the origin of the planetesimals that formed Uranus. Low N-abundance indicates planetesimals from 'warmer' regions where N was mainly in form of NH3, whereas a strong enrichment could indicate planetesimals / cometary material from the colder outer regions of the nebula. Furthermore CO and HCN have been detected in Neptune but not in Uranus. A measurement of the abundance of either would constrain the source mechanisms for these molecules (exogenic or internal). A major surprise from the Galileo Entry Probe was that the heavier noble gases Ar, Kr, and Xe are enhanced in Jupiter's atmosphere at a level comparable to what was seen for the chemically active volatiles N, C, and S. It had been generally expected that Ar, Kr, and Xe would be present in solar abundances, as all were expected to accrete with hydrogen during the gravitational capture of nebular gases. Enhanced abundances of Ar, Kr, and Xe is equivalent to saying that these noble gases have been separated from hydrogen. There are several mechanisms that could accomplish this but these hypotheses require further testing. Measurement of noble gas abundances in an ice giant would constrain the planetary formation and nebular mechanisms responsible for this enhancement. Standard three-layer models of Uranus find that the outer, predominantly H/He layer of Uranus does not reach pressures high enough (approximately 1 Mbar) for H2 to transition to liquid metallic hydrogen. However, valid models can also be constructed with a smaller intermediate water-rich layer, with hydrogen then reaching the metallic hydrogen phase. If this occurs, He should phase separate from the hydrogen and ``rain out," taking along a substantial abundance of Ne, as suggested for Jupiter (and likely also for Saturn). Hence He and Ne depletions could be probes of the planet's structure in the much deeper interior. A determination of Uranus' atmospheric abundances, particularly of the noble gasses, is thus critical to understanding the formation of Uranus, and giant planets in general. These measurements can only be performed with an entry probe. The second key measurement would be a temperature-pressure sounding to provide ground truth for remote measurements of atmospheric temperature and composition and to constrain the internal heat flow. This would also establish that the methane abundance measurements have indeed been made below any possible methane cloud. Finally an ultra stable oscillator would measure wind speeds and constrain atmospheric dynamics. In our presentation we will discuss the importance of all of these measurements and argue that an entry probe is a crucial component of any ice giant mission.
Marley, Mark S.↗
In Situ Measurement of Atmospheric Krypton and Xenon on Mars with Mars Science Laboratory
Mars Science Laboratorys Sample Analysis at Mars (SAM) investigation has measured all of the stable isotopes of the heavy noble gases krypton and xenon in the martian atmosphere, in situ, from the Curiosity Rover at Gale Crater, Mars. Previous knowledge of martian atmospheric krypton and xenon isotope ratios has been based upon a combination of the Viking missions krypton and xenon detections and measurements of noble gas isotope ratios in martian meteorites. However, the meteorite measurements reveal an impure mixture of atmospheric, mantle, and spallation contributions. The xenon and krypton isotopic measurements reported here include the complete set of stable isotopes, unmeasured by Viking. The new results generally agree with Mars meteorite measurements but also provide a unique opportunity to identify various non-atmospheric heavy noble gas components in the meteorites. Kr isotopic measurements define a solar-like atmospheric composition, but deviating from the solar wind pattern at 80Kr and 82Kr in a manner consistent with contributions originating from neutron capture in Br. The Xe measurements suggest an intriguing possibility that isotopes lighter than 132Xe have been enriched to varying degrees by spallation and neutron capture products degassed to the atmosphere from the regolith, and a model is constructed to explore this possibility. Such a spallation component, however, is not apparent in atmospheric Xe trapped in the glassy phases of martian meteorites.
Conrad, P. G.↗
Reference Atmosphere for Mercury
We propose that Ar-40 measured in the lunar atmosphere and that in Mercury's atmosphere is due to current diffusion into connected pore space within the crust. Higher temperatures at Mercury, along with more rapid loss from the atmosphere will lead to a smaller column abundance of argon at Mercury than at the Moon, given the same crustal abundance of potassium. Because the noble gas abundance in the Hermean atmosphere represents current effusion, it is a direct measure of the crustal potassium abundance. Ar-40 in the atmospheres of the planets is a measure of potassium abundance in the interiors, since Ar-40 is a product of radiogenic decay of K-40 by electron capture with the subsequent emission of a 1.46 eV gamma-ray. Although the Ar-40 in the Earth's atmosphere is expected to have accumulated since the late bombardment, Ar-40 in the atmospheres of Mercury and the Moon is eroded quickly by photoionization and electron impact ionization. Thus, the argon content in the exospheres of the Moon and Mercury is representative of current effusion rather than accumulation over the lifetime of the planet.
Killen, Rosemary M.↗
Integrated Molten Salt Reactor Modeling Capabilities in NEAMS Thermal Hydraulics Tools
The DOE neams program supports a full range of computational thermal fluids analysis capabilities and code developments for a broad range of advanced reactor concepts. The research and development approach under the thermal fluids technical area synergistically combines three length and time scales in a hierarchical multi-scale approach. To enable multi-scale thermal fluids capability using these codes, a key joint effort has been underway to develop an integrated system- and engineering-scale thermal fluids analysis capability, through integration of SAM and Pronghorn codes, both based on the MOOSE framework. This report summarizes recent advances in developing an integrated system- and engineering-scale modeling capability for the msr concept, which has gained significant interest in recent years. A consistent framework was established by coupling Pronghorn and SAM through the Saline interface, with thermophysical properties provided by the Molten Salt Thermal Property Database (MSTDB-TP). Further improvements were made to the coupling schemes and domain-overlapping strategies, enhancing the stability and robustness of multi-code simulations. Verification and validation efforts demonstrate the accuracy of this integration across a range of benchmark problems, including one-dimensional heated pipe flows, three-dimensional natural convection loops with evolving isotopic compositions, and \gls{msre} demonstration cases. Within Pronghorn, new capabilities were introduced to model corrosion and noble-metal plating phenomena, supported by an extended thermal-hydraulics framework and refined turbulence treatments. To capture two-phase flow behavior, a multiphase Euler–Euler model was implemented in Pronghorn, including advanced closure relations, high-resolution advection techniques, and capillary force reconstruction. Preliminary verification cases confirm the fidelity of the approach, while planned validation efforts target canonical multiphase benchmarks and application to msr components such as the msre pump bowl. Finally, updates to SAM’s msr mass transfer modeling were extended to consider noble gas migration into porous structures like graphite. The point kinetics model was updated to include reactivity feedback contributions from any defined species, such as xenon. The gas transport model was expanded for applicability to gas mixtures, bubble efflux phenomena, and species transport between liquid and gas phases. A selection of multi-scale Sherwood number correlations from MOSCATO/NekRS and multi-phase correlations from literature have been added for improved accuracy in calculating mass transfer coefficients. A companion effort on developing system-level redox corrosion has also been incorporated into SAM. Collectively, these enhancements strengthen the predictive capability of SAM and Pronghorn for simulating MSR thermal-hydraulics, corrosion, multiphase behavior, and fission-product transport, providing a more complete toolset for design, safety analysis, and licensing support of next-generation \gls{msr}s.
42 - ENGINEERING↗
Noble gases in meteorites and terrestrial planets
Terrestrial planets and chondrites have noble gas platforms that are sufficiently alike, especially Ne/Ar, that they may have acquired their noble gases by similar processes. Meteorites presumably obtained their noble gases during formation in the solar nebula. Adsorption onto C - the major gas carrier in chondrites - is the likely mechanism for trapping noble gases; recent laboratory simulations support this hypothesis. The story is more complex for planets. An attractive possibility is that the planets acquired their noble gases in a late accreting veneer of chondritic material. In chondrites, noble gases correlate with C, N, H, and volatile metals; by Occam's Razor, we would expect a similar coupling in planets. Indeed, the Earth's crust and mantle contain chondritic like trace volatiles and PL group metals, respectively and the Earth's oceans resemble C chondrites in their enrichment of D (8X vs 8-10X of the galactic D/H ratio). Models have been proposed to explain some of the specific noble gas patterns in planets. These include: (1) noble gases may have been directly trapped by preplanetary material instead of arriving in a veneer; (2) for Venus, irradiation of preplanetary material, followed by diffusive loss of Ne, could explain the high concentration of AR-36; (3) the Earth and Venus may have initially had similar abundances of noble gases, but the Earth lost its share during the Moon forming event; (4) noble gases could have been captured by planetestimals, possibly leading to gravitational fractionation, particularly of Xe isotopes and (5) noble gases may have been dissolved in the hot outer portion of the Earth during contact with a primordial atmosphere.
Wacker, J. F.↗
Production rates of neon xenon isotopes by energetic neutrons
As a first step in an experimental program to study the behavior of noble gases produced in situ in minerals, a suite of minerals and pure chemicals were irradiated with 14.5 MeV neutrons at LLNL's Rotating Target Neutron Source (RTNS-II) and production rates for noble gases were determined. While neutron effects in meteorites and lunar samples are dominated by low-energy neutron capture, more energetic cosmic-ray secondary neutrons can provide significant depth-dependent contributions to production of cosmogenic nuclides through endothermic reactions such as (n,2n), (n,np), (n,d) and (n,alpha). Production rates for nuclides produced by cosmic-ray secondary neutrons are therefore useful in interpreting shielding histories from the relative abundances of cosmogenic nuclides. Absolute production cross sections were calculated from isotope dilution analyses of NaCl, Mg, CsCl, and Ba(NO3)2 samples, assuming purity, stoichiometry, and quantitative noble gas retention and extraction. Relative production cross sections determined from neon isotopic ratios in the mineral samples were also considered in evaluating the neon production cross sections. Results are presented.
Leich, D. A.↗
Isotopic Evidence for a Martian Regolith Component in Martian Meteorites
Noble gas measurements in gas-rich impact-melt (GRIM) glasses in EET79001 shergottite showed that their elemental and isotopic composition is similar to that of the Martian atmosphere [1-3]. The GRIM glasses contain large amounts of Martian atmospheric gases. Those measurements further suggested that the Kr isotopic composition of Martian atmosphere is approximately similar to that of solar Kr. The (80)Kr(sub n) - (80)Kr(sub M) mixing ratio in the Martian atmosphere reported here is approximately 3%. These neutron-capture reactions presumably occurred in the glass-precursor regolith materials containing Sm- and Br- bearing mineral phases near the EET79001/ Shergotty sites on Mars. The irradiated materials were mobilized into host rock voids either during shock-melting or possibly by earlier aeolian / fluvial activity.
Rao, M. N.↗
The Interstellar Gas Experiment: Analysis in progress
The Interstellar Gas Experiment (IGE) exposed thin metallic foils aboard the LDEF spacecraft in low Earth orbit in order to collect neutral interstellar particles which penetrate the solar system due to their motion relative to the sun. By mechanical penetration these atoms were imbedded in the collecting foils along with precipitating magnetospheric ions and, possibly, with ambient atmospheric atoms. During the entire LDEF mission, seven of these foils collected particles arriving from seven different directions as seen from the spacecraft. After the foils were returned to Earth, a mass spectrometric analysis of the noble gas component of the trapped particles was begun. The isotopes of He-3, He-4, Ne-20, and Ne-22 were detected. We have given a first account of the experiment. In order to infer the isotopic ratios in the interstellar medium from the concentrations found in the foils, several lines of investigation had to be initiated. The flux of ambient atmospheric noble gas atoms moving toward the foils due to the orbital motion of LDEF was estimated by detailed calculations. Any of these particles which evaded the baffles in the IGE collector could be entrapped in the foils as a background flux. However, the calculations have shown that this flux is negligible, which was the intent of the experiment hardware design. This conclusion is supported by the measurements. However, both the concentration of trapped helium and its impact energy indicate that the flux of magnetospheric ions which was captured was larger than had been expected. In fact, it appears that the magnetospheric particles constitute the largest fraction of the particles in the foils. Since little is known about this particle flux, their presence in the IGE foils appears fortunate. The analysis of these particles provides information about their isotropic composition and average flux.
Buehler, F.↗