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At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Krypton Concentration using HZ-PAN

Idaho National Laboratory (INL) has developed and tested engineered sorbents to separate and capture volatile fission products such iodine, 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. However, performing this separation from bulk air streams is expensive and can pose significant hazards. INL has successfully developed two different sorbents for Xe and Kr capture, silver mordenite polyacrylonitrile and hydrogen mordenite polyacrylonitrile (HZ-PAN). Adsorption studies to date successfully separated and captured Kr from carrier gas streams, but those studies focused primarily on initial separation and capture. Successful utilization in a used nuclear fuel (UNF) reprocessing facility, however, requires further concentration of the Kr to minimize long term storage volumes. This study focuses on the concentration of Kr utilizing HZ PAN as the concentrating media. Concentrating Kr during desorption is ideal for two reasons: one, to produce Kr that can be used for commercial and research applications, or two, to minimize the volume of the radioactive gaseous waste stream for disposal. This report investigates the Kr concentrating potential of HZ-PAN by running multiple Kr adsorption-desorption cycles, collecting the desorbed effluent from a saturated HZ-PAN column, and loading it onto a fresh column. This study demonstrates that four adsorption-desorption cycles can transform a 150 ppmv Kr stream into a 37.5% Kr stream, an overall concentration factor of 2497. Each concentration step results in successively smaller volumes desorbed, reducing volume by a factor of approximately 40,000. Depending on the operational goals, during desorption one could collect smaller volume fractions of high concentration Kr (~ 67%). This demonstration should be considered proof-of-concept. Further refinement is necessary to develop optimum operating schemes to integrate into UNF off-gas treatment.

12 - MGMT OF RADIOACTIVE AND NON-RADIOACTIVE WASTE↗
NASA NTRS1981

Krypton and xenon in the atmosphere of Venus

The paper reports a determination by the Pioneer Venus large probe neutral mass spectrometer of upper limits to the concentration of krypton and xenon along with most of their isotopes in the atmosphere of Venus. The upper limit to the krypton mixing ratio is estimated at 47 ppb, with a very conservative estimate at 69 ppb. The probable upper limit to the sum of the mixing ratios of the isotopes Xe-128, Xe-129, Xe-130, Xe-131, and Xe-132 is 40 ppb by volume, with a very conservative upper limit three times this large.

Donahue, T. M.↗
NASA NTRS1972

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.↗
NASA NTRS1978

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.↗
DOE OSTI2024

In-situ two-dimensional temperature measurements using x-ray fluorescence spectroscopy in laminar flames with high silica particle concentrations

X-ray fluorescence spectroscopy (XRF) was used to measure temperatures and study mixing, for the first time in silica particle synthesis flames. Hexamethyldisiloxane (HMDSO) and trimethylsilanol (TMSO) were the particle precursors. A multi-element diffusion burner was used to produce a flat methane flame, and the precursors, dilute in inert gas, were injected via a central jet. Krypton was the fluorescent medium at 3.2 % concentration by volume. Scans with Kr in the central flow and not in the main flow were made to assess the mixing effects between the central and main gas flows. When HMDSO or TMSO were added, a secondary diffusion flame formed between the jet and the main methane flame. The results revealed a dramatic change in the centerline temperature profile of the jet gases when HMDSO or TMSO were added. The main methane flame stoichiometry also affected the temperature profiles. The results show HMDSO and TMSO reactions are initiated in a lowtemperature and low-oxygen concentration region of the jet where thermal decomposition is not expected to be significant. Reaction of the particle precursors is therefore attributed to radical transport from the main methane flame. In the current work, particle number densities of up to 270 g/m 3 locally are estimated. Thus, the study also demonstrates the capability of the XRF technique for high spatial fidelity measurements in flames with high concentrations of condensed-phase particles, leveraging the attribute that the XRF signal is generally not impacted by condensed-phase interferences. In conclusion, the observations and data obtained in this study inform likely reaction pathways for this important class of siloxane compounds.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Concentration of Kr from Simulated Dissolver Off-Gas Streams Utilizing a Solid Sorbent, HZ-PAN

Idaho National Laboratory (INL) has developed and tested engineered sorbents to separate and capture volatile fission products such iodine, xenon (Xe), and krypton (Kr) from off-gas streams. A study was conducted using a solid sorbent, HZ-PAN, to concentrate Kr from a simulated dissolver off-gas stream. The study demonstrates that four adsorption-desorption cycles can transform a 150 ppmv Kr stream into a 37.5% Kr stream, an overall concentration factor of 2497.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
NASA NTRS1988

Solar, planetary, and other inert gases in two sieve fractions of a disaggregated Allende sample - A study by stepwise heating extraction

Inert gases released by stepwise heating of unaltered, strongly magnetic, and weakly magnetic samples from the 0-64 micron and the 105-250 micron fractions of a disaggregated and sieved sample of the Allende meteorite reveal the occurrence of both solar and planetary neon. The origin of the solar neon is thought to be implantation of solar wind ions. The origin of the planetary neon remains unresolved. Heavy isotope enriched components of krypton and xenon have been detected and there are some indications that a light krypton component may also be present. Other than a larger concentration of Xe-129 in the weakly magnetic samples, the signatures of the magnetic separates are isotopically very similar.

Palma, R. L.↗
DOE OSTI2024

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↗
DOE OSTI2024

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↗
DOE OSTI2025

Preferential adsorption of noble gases in zeolitic tuff with variable saturation: A modeling study of counter-intuitive diffusive-adsorptive behavior

Noble gas transport through geologic media has important applications in the prediction and characterization of measured gas signatures related to underground nuclear explosions (UNEs). Retarding processes such as adsorption can cause significant species fractionation of radionuclide gases, which has implications for measured and predicted signatures used to distinguish radioxenon originating from civilian nuclear facilities or from UNEs. Accounting for the effects of variable water saturation in geologic media on tracer transport is one of the most challenging aspects of modeling gas transport because there is no unifying relationship for the associated tortuosity changes between different rock types, and reactive transport processes such as adsorption that are affected by the presence of water likewise behave differently between gas species. In this study, we perform numerical diffusive-adsorptive transport simulations to estimate gas transport parameters associated with bench-scale laboratory diffusion cell experiments measuring breakthrough in zeolitic and non-zeolitic rocks for a gaseous mixture of xenon, krypton, and SF 6 at varying degrees of water saturation (S w ). Counter-intuitive transport behavior was observed in the zeolitic rock experiments whereby breakthrough concentrations were significantly higher when the core was partially saturated (S w = 17 %) than under dry (S w = 0 %) conditions. Breakthrough of xenon was especially retarded in the dry core – likely due to comparatively high affinity of xenon for zeolitic adsorption sites – and estimated effective diffusion coefficients for all gases were approximately an order of magnitude lower than what is predicted by porosity-tortuosity models. We propose the counter-intuitive behavior observed is because water infiltration of zeolite nanopores reduces both the adsorptive capacity of the rock and the tortuosity of connected flow paths. We developed a two-site competitive kinetic Langmuir adsorption reaction for the porous media transport simulator in order to constrain transport parameters within zeolitic tuff, where differential adsorption to zeolite and non-zeolite pores was observed. We determined that liquid saturation-dependent diffusive-adsorptive transport is affected by subtle and at times competing processes that are specific to different gases, which have a significant overall influence on effective transport parameters.

58 GEOSCIENCES↗
DOE OSTI2026

Hydrogen Recombiner Catalyst Evaluations for Waste Storage

Radiolysis of water in nuclear waste storage generates hydrogen gas that can accumulate within sludge style waste and be rapidly released during agitation events, creating a significant flammability hazard. Engineering controls are therefore required to limit hydrogen concentrations during both quiescent storage and transient disturbances. Catalytic recombination of hydrogen in waste storage offgas is a proven mitigation strategy, maintaining hydrogen levels below flammability limits and managing sudden concentration spikes. Conventional recombiners rely on platinum and/or palladium catalysts, with development efforts focused on extending service life, increasing active surface area, and ensuring safe deployment in radioactive environments. Savannah River National Laboratory (SRNL) is evaluating a newly developed hydrogen recombiner catalyst from Canadian Nuclear Laboratories as a cost-effective and durable alternative for nuclear waste applications. Testing was conducted in SRNL’s Shielded Cells facility, which enables reduced-scale experimental modeling under radiation fields and near-use-case conditions relevant to radioactive waste storage. Catalyst performance was evaluated using a custom offgas characterization system designed for near-zero flow conditions. The experimental apparatus consisted of a gas-tight 2.7 L PTFE vessel equipped with temperature monitoring, gas flow controls, and a variable-speed mixer to simulate sludge agitation. Offgas composition was monitored using a dedicated gas chromatograph with argon carrier gas and a krypton internal standard. Measurements were obtained for an empty vessel, the vessel containing a well characterized radioactive tank waste sample, and the same configuration with the candidate catalyst installed. Results demonstrate that the new catalyst effectively reduced hydrogen concentrations in the offgas within the constraints of the experimental design. In addition to confirming catalytic activity, the testing provided valuable insights into experimental optimization and considerations for future performance evaluations. These findings support the potential scalability of the technology and highlight its applicability to broader nuclear waste management operations, offering improved safety and reduced operational costs through enhanced catalyst durability and lower replacement frequency.

Tener, Zachary P. [Savannah River National Laborat↗
DOE OSTI1968

Kryptonate Hydrogen Detection System (Final Report)

A prototype model of a multipurpose instrument which demonstrates the applicability of the Kryptonate® technique for detecting hydrogen gas was developed. This report describes the construction of the instrument and presents a laboratory evaluation of its performance. Performance was excellent. The instrument was designed to detect hydrogen in air at concentrations of 0-3% by volume, and to detect hydrogen in nitrogen or other inert gas at concentrations of 0-10% by volume. Other detection levels (both higher and lower) could be set if required. Ultimate response times can be made of the order of 0.5 seconds. The instrument is an all solid state device operating from 120V 60 Hz power source. The instrument has been designed to enable modifications to be made with a minimum amount of difficulty.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
NASA NTRS2012

Numerical Investigation of PLIF Gas Seeding for Hypersonic Boundary Layer Flows

Numerical simulations of gas-seeding strategies required for planar laser-induced fluorescence (PLIF) in a Mach 10 air flow were performed. The work was performed to understand and quantify adverse effects associated with gas seeding and to compare different flow rates and different types of seed gas. The gas was injected through a slot near the leading edge of a flat plate wedge model used in NASA Langley Research Center's 31- Inch Mach 10 Air Tunnel facility. Nitric oxide, krypton, and iodine gases were simulated at various injection rates. Simulation results showing the deflection of the velocity field for each of the cases are presented. Streamwise distributions of velocity and concentration boundary layer thicknesses as well as vertical distributions of velocity, temperature, and mass distributions are presented for each of the cases. Relative merits of the different seeding strategies are discussed.

Johanson, Craig T.↗
NASA NTRS2015

Investigation of Gas Seeding for Planar Laser-Induced Fluorescence in Hypersonic Boundary Layers

Numerical simulations of the gas-seeding strategies required for planar laser-induced fluorescence in a Mach 10 (approximately Mach 8.2 postshock) airflow were performed. The work was performed to understand and quantify the adverse effects associated with gas seeding and to assess various types of seed gas that could potentially be used in future experiments. In prior experiments, NO and NO2 were injected through a slot near the leading edge of a flatplate wedge model used in NASA Langley Research Center's 31 in. Mach 10 air tunnel facility. In this paper, nitric oxide, krypton, and iodine gases were simulated at various injection rates. Simulations showing the deflection of the velocity boundary layer for each of the cases are presented. Streamwise distributions of velocity and concentration boundary-layer thicknesses, as well as vertical distributions of velocity, temperature, and mass distributions, are presented for each of the cases. A comparison between simulated streamwise velocity profiles and experimentally obtained molecular tagging velocimetry profiles using a nitric oxide seeding strategy is performed to verify the influence of such a strategy on the boundary layer. The relative merits of the different seeding strategies are discussed. The results from a custom solver based on OpenFOAM version 2.2.1 are compared against results obtained from ANSYS® Fluent version 6.3.

Arisman, C. J.↗
NASA NTRS1974

Investigation of nitric oxide decomposition in the temperature range 2500-4100 K

The decomposition of nitric oxide has been studied in the temperature range 2500-4100 K using a shock-tube technique. The principle result of the study was the determination of the rate constant (k) for the reaction O + NO yields N + O2. Mixtures of NO and N2O diluted in argon or krypton were heated by incident shock waves and the infrared emission from the fundamental vibration-rotation band of NO at 5.3 microns was used to monitor the time-varying NO concentration. The experimental values of k are fit closely by the expression k = (2.36 times 10 to the 9th power) x T x exp(-38,640/RT) cm cu/mole-sec, which also provides a good fit to previous data at higher and lower temperatures.

Flower, W. L.↗
NASA NTRS1974

Kinetics of the reaction of nitric oxide with hydrogen

Mixtures of NO and H2 diluted in argon or krypton were heated by incident shock waves, and the infrared emission from the fundamental vibration-rotation band of NO at 5.3 microns was used to monitor the time-varying NO concentration. The reaction kinetics were studied in the temperature range 2400-4500 K using a shock-tube technique. The decomposition of nitric oxide behind the shock was found to be modeled well by a fifteen-reaction system. A principle result of the study was the determination of the rate constant for the reaction H + NO yields N + OH, which may be the rate-limiting step for NO removal in some combustion systems. Experimental values of k sub 1 were obtained for each test through comparisons of measured and numerically predicted NO profiles.

Flower, W. L.↗
NASA NTRS1975

Kinetics of the reaction of nitric oxide with hydrogen

The reaction of nitric oxide with hydrogen has been studied in the temperature range 2400-4500 K using a shock-tube technique. Mixtures of NO and H2 diluted in argon or krypton were heated by incident shock waves, and the infrared emission from the fundamental vibration-rotation band of NO at 5.3 microns was used to monitor the time-varying NO concentration. The decomposition of nitric oxide behind the shock was found to be modeled well by a fifteen-reaction system. A principal result of the study was the determination of the rate constant k1 for the reaction H + NO yields N + OH, which may be the rate-limiting step for NO removal in some combustion systems. Experimental values of k1 were obtained for each test through comparisons of measured and numerically predicted NO profiles. The data are fit closely by the expression k1 = 1.34 times 10 to the fourteenth power exp(-49 200/RT) cu cm/mole-sec. These data appear to be the first available for this rate constant.

Flower, W. L.↗
NASA NTRSDate not supplied

Enriching Heavy Noble Gases in Titan Atmosphere by Cryogenic Condensation

Titan is an extraordinary moon belonging to Saturn. It presents a dense atmosphere with a surface pressure approximately 1.45 times that of Earth’s. The relative abundance of noble gases and their isotopes can elucidate extant geochemical processes and inform past and future planetary evolution. The GCMS on the Hyugens probe sampled the dense atmosphere of Saturn’s Titan in 2005 and did not detect Kr or Xe at ppb concentrations. Several chemical pathways have been considered as mechanisms to account for the depletion of these heavy nobles. However, our understanding remains incomplete without in situ detection. Thus, we investigate spaceflight cryogenic enrichment for Kr and Xe. The thermodynamic processes would be capable of substantially amplifying these gases at femtomole concentrations, in anticipation of future atmospheric surveys on Titan.

condensation↗