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At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

2D Nitrogen‐Doped Graphene Materials for Noble Gas Separation

Abstract Noble gases, notably xenon, play a pivotal role in diverse high‐tech applications. However, manufacturing xenon is an inherently challenging task, due to its unique properties and trace abundance in the Earth's atmosphere. Consequently, there is a pressing need for the development of efficient methods for the separation of noble gases. Using mild fluorographene chemistry, nitrogen‐doped graphene (GNs) materials are synthesized with abundant aromatic regions and extensive nitrogen doping within the vacancies and holes of the aromatic lattice. Due to the organized interlayer “nanochannels”, nitrogen functional groups, and defects within the two‐dimensional (2D) structures, GNs exhibits effective selectivity for Xe over Kr at low pressure. This enhanced selectivity is attributed to the stronger binding affinity of Xe to GN compared to Kr. The adsorption is governed by London dispersion forces, as revealed by theoretical calculations using symmetry‐adapted perturbation theory (SAPT). Investigation of other GNs differing in nitrogen content, surface area, and pore sizes underscores the significance of nitrogen functional groups, defects, and interlayer nanochannels over the surface area in achieving superior selectivity. This work offers a new perspective on the design and fabrication of functionalized graphene derivatives, exhibiting superior noble gas storage and separation activity exploitable in gas production technologies.

Šedajová, Veronika↗
DOE OSTI2022

Noble gas adsorption to tuff

For this report a method was developed to measure trace noble gas element adsorption to the surfaces of geologic materials in the presence of a background gas that could potentially compete for surface adsorption sites. Adsorption of four noble gas elements (Ne, Ar, Kr, and Xe) at a concentration of 100 ppm in helium and nitrogen were measured on a sample of crushed tuff at 0, 15, 30, and 45°C. In addition, Ne, Ar, Kr, and Xe at 250 ppm and 500 ppm in nitrogen at 15°C were measured. Noble gas adsorption was found to increase with increasing atomic mass and decreasing temperature. It was also observed that the relative increase in noble gas element adsorption with decreasing temperature tends to increase with increasing atomic mass. Noble gas adsorption from nitrogen was approximately an order of magnitude greater than for the noble gases in helium. As the noble gas concentrations in nitrogen increased, adsorption increased in a slightly non-linear fashion which could be modeled using a Freundlich isotherm. For noble gas concentrations that were ≤100 ppm Henry's Law constant were calculated.

58 GEOSCIENCES↗
DOE OSTI2021

Investigating Fracture Network Deformation Using Noble Gas Release

We investigate deformation mechanics of fracture networks in unsaturated fractured rocks from subsurface conventional detonation using dynamic noble gas measurements and changes in air permeability. We dynamically measured the noble gas isotopic composition and helium exhalation of downhole gas before and after a large subsurface conventional detonation. These noble gas measurements were combined with measurements of the subsurface permeability field from 64 discrete sampling intervals before and after the detonation and subsurface mapping of fractures in borehole walls before well completion. We saw no observable increase in radiogenic noble gas release from either an isotopic composition or a helium exhalation point of view. Large increases in permeability were observed in 13 of 64 discrete sampling intervals. Of the sampling intervals which saw large increases in flow, only two locations did not have preexisting fractures mapped at the site. Given the lack of noble gas release and a clear increase in permeability, we infer that most of the strain accommodation of the fractured media occurred along previously existing fractures, rather than the creation of new fractures, even for a high strain rate event. These results have significant implications for how we conceptualize the deformation of rocks with fracture networks above the percolation threshold, with application to a variety of geologic and geological engineering problems.

Gardner, W. Payton↗
DOE OSTI2020

Hawaii Play Fairway Analysis: Noble Gas Raw Data for Hawaii, Maui, Oahu, Kauai, and Lanai islands

Noble gas raw data for the Hawaiian islands of Big Island, Maui, Oahu, Lanai, and Kauai. Based on results from prior phases of the Hawaii Play Fairway Analysis, this project targeted 66 wells on the islands of Hawaii, Maui, Lanai, Oahu, and Kauai for sampling of dissolved noble gases, trace metals, common ions, and the stable isotopes 2H and 18O. Ultimately, 23 of the 66 well targets were sampled. Noble gas data from this study is supplemented with data shared by the United States Geologic Survey for the summit of Kilauea, and by the geothermal energy company Ormat Technologies Inc. for their geothermal power plant Puna Geothermal Venture on the Lower East Rift of Kilauea, and for their exploration of Kona and Hualalai on Hawaii, as well as the Southwest Rift of Haleakala on Maui. The noble gas helium is used as an indicator of geothermal heat when excess 3He and/or 4He is present when compared to the atmospheric ratio of those isotopes (R/Ra). R/Ra is minimally affected by dilution and transport, allowing even those wells not perfectly situated over a geothermal system to indicate a geothermal anomaly. R/Ra anomalies are present on every island in this study. There is a strong correlation between R/Ra anomalies and proximity to rift zones and calderas. The Hawaii Play Fairway project was funded by the U.S. Department of Energy Geothermal Technologies Office (award DE-EE0006729). For more information, see Colin Ferguson's Master of Science thesis "Exploration for Blind Geothermal Resources in the State of Hawaii Utilizing Dissolved Noble Gasses in Well Waters."

15 GEOTHERMAL ENERGY↗
DOE OSTI2020

Effects of natural zeolites on field-scale geologic noble gas transport

Improving predictive models for noble gas transport through natural materials at the field-scale is an essential component of improving US nuclear monitoring capabilities. Several field-scale experiments with a gas transport component have been conducted at the Nevada National Security Site (Non-Proliferation Experiment, Underground Nuclear Explosion Signatures Experiment). However, the models associated with these experiments have not treated zeolite minerals as gas adsorbing phases. This is significant as zeolites are a common alteration mineral with a high abundance at these field sites and are shown here to significantly fractionate noble gases during field-scale transport. This fractionation and associated retardation can complicate gas transport predictions by reducing the signal-to-noise ratio to the detector (e.g. mass spectrometers or radiation detectors) enough to mask the signal or make the data difficult to interpret. Omitting adsorption-related retardation data of noble gases in predictive gas transport models therefore results in systematic errors in model predictions where zeolites are present.Herein is presented noble gas adsorption data collected on zeolitized and non-zeolitized tuff. Experimental results were obtained using a unique piezometric adsorption system designed and built for this study. Data collected were then related to pure-phase mineral analyses conducted on clinoptilolite, mordenite, and quartz. These results quantify the adsorption capacity of materials present in field-scale systems, enabling the modeling of low-permeability rocks as significant sorption reservoirs vital to bulk transport predictions.

58 GEOSCIENCES↗
DOE OSTI2023

Short-lived noble gas effluent trends from a research reactor

An understanding of anthropogenic sources of radioactive noble gases in the atmosphere is needed to enhance the discrimination ability of the International Monitoring System's sensors. These sources include commercial and research nuclear reactors and medical isotope production facilities. While abiding by local environmental ordinances these facilities all emit noble gas radioisotopes through normal operation. Here, this research presents measurements and analysis of noble gas isotopes ( 41 Ar, 135 Xe, 135m Xe, 137 Xe, 138 Xe, 87 Kr, 88 Kr, and 89 Kr) made directly at the stack of the High Flux Isotope Reactor (HFIR) at Oak Ridge National Laboratory. The Xe and Kr noble gases are concurrently observed with 41 Ar, a neutron activation product, when the reactor is operational. The magnitude of the Xe and Kr noble gases released is not constant over the HFIR cycle, but they temporally match the 41 Ar trend. An isotope activity ratio analysis of these shorter lived isotopes combined with the observation of the cycle's temporal trend helps understand the noble gas production mechanism at the HFIR. Isotopes with short half-lives are not useful for long-range environmental monitoring. However, these measurements could potentially be combined with atmospheric modeling to predict the background source term of the longer-lived Xe ratios at a monitoring station.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗
DOE OSTI2025

Optimal strategies for optical quantum memories using long-lived noble-gas spins

Nuclear spins of noble gases exhibit exceptionally long coherence times and can potentially serve as a long-lived storage medium for quantum information. We analyze and compare the performance of two mechanisms for mapping the quantum state of light onto the collective spin state of noble gases. The first mechanism utilizes collisional exchange with the electronic spin state of metastable noble-gas atoms, while the second relies on spin-exchange collisions with ground-state alkali-metal atoms. We describe the operation of an optical quantum memory relying on these two mechanisms using a compact model and study strategies that optimize the memory storage efficiency. Through numerical simulations, we identify optimal sequences for storing optical signals with different signal bandwidths and electronic spin relaxation rates. This work highlights the qualitative difference between the two approaches for using noble gases as long-lived quantum memories at noncryogenic conditions and outlines the regimes in which they are expected to be efficient.

atomic ensemble↗
DOE OSTI2022

Using groundwater noble gas measurements to confirm paleorecharge hypotheses at Pahute Mesa, Nevada National Security Site, Nevada, USA

Pahute Mesa (Nevada, USA) was the site of 85 underground nuclear tests between 1965 and 1992 whose residual radio-chemical inventory poses a contaminant threat to local groundwater resources. To assess the fate and transport of these radionuclides in groundwater, several geochemical studies, including this one, have been conducted to understand long-term groundwater flow patterns at, and downgradient of, Pahute Mesa. Groundwater samples from the Pahute Mesa area at the Nevada National Security Site were analyzed for noble gases ( 3 He/ 4 He isotopic ratio and He, Ne, Kr, Ar and Xe concentrations) to infer groundwater recharge temperatures and provide additional evidence in support of groundwater flow patterns and the presence of late-pluvial Pleistocene groundwater. These data confirm recent findings (based on groundwater geochemistry and isotope compositions) that most recharge in the area occurred under temperature conditions much cooler than are found today, except near major drainages where ephemeral run of continues to recharge shallow groundwater. These noble gas data indicate that noble gas recharge temperatures and terrigenic He components have been reset where groundwater has flowed upward over barriers formed by caldera margins, or near the regional discharge area (Oasis Valley) where shallow groundwater has interacted with shallow soil gas. This evidence from groundwater noble gas measurements, in combination with other isotopic and geochemical studies, supports the current understanding of the unusual hydrogeology and recharge history of Pahute Mesa.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Examining the potential for detecting simultaneous noble gas and aerosol samples in the international monitoring system radionuclide network

The purpose of the Comprehensive Nuclear-Test-Ban Treaty (CTBT) is to establish a legally binding ban on nuclear weapon test explosions or any other nuclear explosions. The Preparatory Commission for the CTBT Organization (CTBTO PrepCom) is developing the International Monitoring System (IMS) that includes a global network of 80 stations to monitor for airborne radionuclides upon entry into force of the CTBT. All 80 radionuclide stations will monitor for particulate radionuclides and at least half of the stations will monitor for radioxenon. The airborne radionuclide monitoring is an important verification technology both for the detection of a radionuclide release and in the determination of whether the release event originates from a nuclear explosion as opposed to an industrial use of nuclear materials. Nuclear power plants and many medical isotope production facilities release radioxenon into the atmosphere. Low levels of a few particulate isotopes, such as iodine, may also be released. Detections of multiple isotopes are useful for screening the radionuclide samples for relevance to the Treaty. This paper examines the anticipated joint detections in the IMS of noble gas and particulate isotopes from underground nuclear explosions where breaches in the underground containment vents from low levels to up to 1% of the radionuclide inventory of the resulting fission products to the atmosphere. Detection probabilities are based on 844 simulated release events spaced out at 17 release locations and one year in time. Six different release (venting) scenarios, including two fractionated scenarios, were analyzed. When ranked by detection probability, 11 particulate isotopes and one noble gas isotope ( 133 Xe) appear in the top 20 isotopes for all six release scenarios. Using the 11 particulate isotopes and the one noble gas isotope, the IMS has nearly the same detection probability as when 45 particulate and 4 noble gas isotopes are used. Thus, a limited list of relevant radionuclides may be sufficient for treaty verification purposes. The probability that at least one particulate and at least one radioxenon isotope would be detected in the IMS from the release events ranged from 0.15 to 0.86 depending on the release scenario.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗
DOE OSTI2024

133Xe Noble Gas Mass Spectrometry Measurement for High Purity Germanium Detector Performance Verification

Idaho National Laboratory produces quality control standards for laboratories that operate xenon radionuclide monitoring systems. Activities reported with each quality control standard are quantified using high purity germanium detectors. A collection of measurement capabilities are being set up at Idaho National Laboratory to establish an in-house high purity germanium detector performance verification system, with noble gas mass spectrometry being one of these measurement capabilities. The first noble gas mass spectrometry and high purity germanium measurement comparison is presented here. A Xe-133 gas sample was prepared and the activity was quantified with high purity germanium detectors. The Xe-133 sample was diluted with a known quantity of isotopically enriched Xe-126 gas; the resulting Xe-133 : Xe-126 atom ratio was calculated to be 1.15x10-4 +/- 2% at reference time t. An aliquot of this gas sample containing approximately 10 million Xe-133 atoms was introduced into a ThermoFisher Scientific Helix MC Plus noble gas mass spectrometer for analysis. The measured Xe-133 : Xe-126 atom ratio was determined to be 1.10x10-4 +/- 2% (1-sigma uncertainty) at reference time t, about 4.3% lower than the atom ratio determined with the measured high purity germanium activity.

46 - INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AN↗
DOE OSTI2021

Metal Organic Frameworks for Noble Gas Management in the Liquid Fluoride Thorium Reactor (LFTR) (CRADA 459)

The purpose of this project is to demonstrate the novel class of materials known as metal organic frameworks (MOFs) to capture Xe selectively from simulated LFTR off gas. This will establish the viability of designing a dramatically improved approach to noble gas management as compared to activated carbon. However, there are significant data gaps that need to be addressed in order to deploy this technology for LFTRs that include i) converting MOF powders into engineered forms to produce mechanically robust particles, ii) the radiation stability and associated mechanism of degradation (if any) upon irradiation of these sorbent materials and iii) demonstration and comparison to activated carbon of the noble gas separation from simulated LFTR gas stream.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗
DOE OSTI2024

Short communication: Cosmogenic noble gas depletion in soils by wildfire heating

Measurements of cosmic-ray-produced beryllium-10, neon-21, and helium-3 in quartz in a soil profile from a forested landscape in the Oregon Coast Range show that the cosmogenic noble gases 21 Ne and 3 He are depleted relative to 10Be in the shallow subsurface. The noble gases are mobile in mineral grains via thermally activated diffusion and 10 Be is not, implying that noble gas depletion is the result of surface heating by wildfires and subsequent mixing of partially degassed quartz downward into the soil. Cosmogenic noble gas depletion by wildfire heating of soils is a potential means of estimating wildfire intensity and/or frequency over pre-observational timescales.

58 GEOSCIENCES↗
DOE OSTI2021

Binding of noble gas atoms by superhalogens

Because of their closed shells, noble gas (Ng) atoms (Ng = Ne, Ar, Kr, and Xe) seldom take part in chemical reactions, yet finding such mechanisms not only is of scientific interest but also has practical significance. Following a recent work by Mayer et al. [Proc. Natl. Acad. Sci. U. S. A. 116, 8167–8172 (2019)] on the room temperature binding of Ar to a superelectrophilic boron site embedded in a negative ion complex, B 12 (CN) 11 - , we have systematically studied the effect of cluster size and terminal ligands on the interaction of Ng by focusing on B 12 X 11 (Ng) (X = H, CN, and BO) and B 12 X 10 (Ng) 2 (X = CN and BO) whose stabilities are governed by the Wade–Mingos rule and on C 5 BX 5 (Ng) (X = H, F, and CN) and C 4 B 2 (CN) 4 (Ng) 2 whose stabilities are governed by the Huckel’s aromaticity rule. Our conclusion, based on density functional theory, is that both the cluster size and the terminal ligands matter—the interaction between the cluster and the Ng atoms becomes stronger with increasing cluster size and the electron affinity of the terminal ligands. Our studies also led to a counter-intuitive finding—removing multiple terminal ligands can enable electrophilic centers to bind multiple Ng atoms simultaneously without compromising their binding strength.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Noble gas insights into early impact delivery and volcanic outgassing to Earth's atmosphere: A limited role for the continental crust

Earth's atmosphere, crust and mantle have evolved together through continuous geochemical exchange throughout Earth's history. Constraints on the transport of volatile elements and compounds between these reservoirs are crucial for understanding how Earth could have stayed habitable for extended periods of time. In this work, we present a new forward model of He, Ne and Ar in the mantle, crust and atmosphere. We explore concentrations of noble gases at the end of accretion, bulk silicate Earth K/U ratios, crustal growth scenarios, and upper mantle processing rates throughout Earth's history. We search for parameter combinations that simultaneously satisfy observational constraints on present-day mantle 4 He/ 3 He and 40 Ar/ 36 Ar (sensitive to mantle outgassing and continental crust growth, which depletes the mantle of U, Th and K), atmospheric 20 Ne/ 22 Ne (which tracks the mix of outgassed vs. delivered Ne in the atmosphere), and atmospheric 40 Ar/ 36 Ar in the past and today (sensitive to volatile delivery, mantle outgassing and crustal growth). Leveraging this intertwined set of noble gas abundances and isotopic compositions yields new constraints on initial noble gas abundances in the mantle and on the proportions of atmospheric volatiles originating from delivery by impact degassing, mantle outgassing, and degassing of the continental crust. We find that atmospheric Ar isotopic evolution is primarily sensitive to the mantle processing rate history; the atmospheric Ar isotopic record should therefore not be used to reconstruct continental crust growth, but instead provides valuable insights into mantle processing rates. Our model predicts a measurably low 20 Ne/ 22 Ne ratio of ~9.7 in Archean atmospheric samples. Most of atmospheric primordial 36 Ar was directly delivered by chondritic bodies and not transferred to the atmosphere during an intense early episode of mantle outgassing. Nitrogen delivered by impact degassing could account for the present-day atmospheric nitrogen inventory.

58 GEOSCIENCES↗
DOE OSTI2024

Metal Organic Frameworks for Noble Gas Isotope Harvesting at FRIB (Final Technical Report)

This project was a collaborative effort between Lawrence Livermore National Laboratory (LLNL) and Michigan State University (MSU) to investigate the use of promising metal organic frameworks (MOFs) for radioactive noble gas capture, with a focus on harvesting exotic radiokryptons from FRIB. After screening several candidate materials, two MOFs were selected for testing: SIFSIX-3Cu and SBMOF-1. Further evaluation showed that although SIFSIX-3Cu has a high selectivity for Kr, SBMOF-1 is less sensitive to the humidity that is present in the FRIB harvesting system and is more readily integrated into the harvesting infrastructure. SBMOF-1 was then evaluated for temperature-dependent Kr and Xe uptake in order to determine the sorption enthalpy. The SBMOF-1 data led to the design of a noble gas capture system that will be fabricated and put into service for isotope harvesting at FRIB as part of a separate project.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗