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At least 91 records · Page 5

New proton emitter 188 At implies an interaction unprecedented in heavy nuclei

We report the discovery of a new atomic nucleus 188 At, which is the heaviest proton-emitting isotope known to date. The new activity was observed through the 107 Ag( 84 Sr, 3n) 188 At fusion-evaporation reaction using the focal-plane spectrometer of the gas-filled recoil separator in the Accelerator Laboratory of the University of Jyväskylä, Finland. To fully interpret the experimental data, we have expanded the non-adiabatic quasiparticle model to treat nuclei in the beyond-lead region. The description reproduced the measured decay rate and pointed towards emission from an extremely prolate-deformed state with a dominant s 1/2 proton component in the wave function. The Thomas-Ehrman shift can be enhanced in low angular momentum states, but such effects have not been observed in heavy nuclei. The single-proton separation energy of 188 At deviates from that extrapolated from the systematics, which can be interpreted as the first evidence of this effect in heavy nuclei.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Clues to the origin of sulfide minerals in CI chondrites

The dominant sulfide in CI carbonaceous chondrites is an Fe-deficient pyrrhotite containing about 1% Ni, Alais, Ivuna, and Orgueil also contain minor cubanite, CuFe2S3, and Alais minor pentlandite, (Fe,Ni)9S8. All pyrrhotites contain 39.4 + or - 0.1% S; Ni contents range from 0.7 to 1.3%. The phase diagrams reveal no temperature at which the observed pentlandite-pyrrhotite assemblage is at equilibrium. Similarly, the pyrrhotite composition alone are inconsistent with equilibrium formation from a gas of solar composition. In Xe from high-purity submilligram Orgueil pyrrhotite separates, the ratios Xe-129/Xe-132 are not significantly larger than those in trapped meteoritic Xe. The lack of positive evidence for extinct I-129 in pyrrhotite does not permit any inferences regarding cooling rates in the early solar nebula. It is concluded that sulfides in CI chondrites cannot be nebular condensates formed under equilibrium conditions. Argon isotopic abundances reveal the presence of significant spallation and trapped gas components in Orgueil pyrrhotite. The Orgueil exposure age is calculated to be at least about 10 m.y.

Kerridge, J. F.↗

Hydrogen Isotope Measurements of Organic Acids and Alcohols by Pyrolysis-GC-MS-TC-IRMS

One possible process responsible for methane generation on Mars is abiotic formation by Fischer-Tropsch-type (FTT) synthesis during serpentinization reactions. Measurement of carbon and hydrogen isotopes of intermediary organic compounds can help constrain the origin of this methane by tracing the geochemical pathway during formation. Of particular interest within the context of this work is the isotopic composition of organic intermediaries produced on the surfaces of mineral catalysts (i.e. magnetite) during hydrothermal experiments, and the ability to make meaningful and reproducible hydrogen isotope measurements. Reported here are results of experiments to characterize the hydrogen isotope composition of low molecular weight organic acids and alcohols. The presence of these organic compounds has been suggested by others as intermeadiary products made during mineral surface catalyzed reactions. This work compliments our previous study characterizing the carbon isotope composition of similar low molecular weight intermediary organic compounds (Socki, et al, American Geophysical Union Fall meeting, Abstr. #V51B-2189, Dec., 2010). Our hydrogen isotope measurements utilize a unique analytical technique combining Pyrolysis-Gas Chromatograph-Mass Spectrometry-High Temperature Conversion-Isotope Ratio Mass Spectrometry (Py-GC-MS-TC-IRMS). Our technique is unique in that it carries a split of the pyrolyzed GC-separated product to a Thermo DSQ-II? quadrupole mass spectrometer as a means of making qualitative and semi-quantitative compositional measurements of separated organic compounds, therefore both chemical and isotopic measurements can be carried out simultaneously on the same sample.

Socki, Richard A.↗

High power gas laser - Applications and future developments

Fast flow can be used to create the population inversion required for lasing action, or can be used to improve laser operation, for example by the removal of waste heat. It is pointed out that at the present time all lasers which are capable of continuous high-average power employ flow as an indispensable aspect of operation. High power laser systems are discussed, taking into account the gasdynamic laser, the HF supersonic diffusion laser, and electric discharge lasers. Aerodynamics and high power lasers are considered, giving attention to flow effects in high-power gas lasers, aerodynamic windows and beam manipulation, and the Venus machine. Applications of high-power laser technology reported are related to laser material working, the employment of the laser in controlled fusion machines, laser isotope separation and photochemistry, and laser power transmission.

Hertzberg, A.↗

A long-term change of the AR/KR/XE fractionation in the solar corpuscular radiation

Solar noble gases in an ilmenite separate from breccia 79035 (antiquity greater than 1 Ga) were analyzed by closed system stepped etching (CSSE). All five gases show the familiar two-component structure: first solar-wind (SW) gases are released, followed by gases from solar energetic particles (SEP). Element patterns in 79035 are similar to those of 71501 ilmenite. SW-He-Ne were partly lost, but SEP-He-Ne-Ar are retained (nearly) unfractionated. Constant Ar/Kr/Xe ratios indicate that ilmenites contain an unfractionated sample of the heavy SW-SEP noble gases. Ar/Kr/Xe ratios in the solar corpuscular radiation are, however, different from 'solar system' values, whereby the Kr/Xe difference in 79035 is about twice as large as in 71501. We propose that Xe is less fractionated than Kr and Ar, though its first ionization potential (FIP) is higher than the 'cutoff' at approximately 11.5 eV, above which all elements in SEP are usually assumed to be depleted by a roughly constant factor. SW-Ne may be isotopically slightly heavier in the ancient SW trapped by 79035, as proposed earlier. In this work we extend our previous CSSE studies of solar noble gases including Kr and Xe to a lunar sample irradiated at least 1 Ga ago (breccia 79035, ilmenite separate, 42-64 microns). This sample was particularly gently etched in the first steps. Surprisingly, the first three steps, each releasing less than or equal to 0.5% of the total 36-Ar, showed an SEP-like trapped component plus relatively large concentrations of cosmogenic gases. Steps 4ff contain much less cosmogenic and more solar gas with a SW-like isotope pattern. Thus, a very minor easily etchable phase that has completely lost its SW-gases must be responsible for steps 1-3. We will not discuss these steps here and refer to the actual step 4 as the 'initial' etching step.

Wieler, R.↗

Isotopic anomalies of noble gases in meteorites and their origins. VI Presolar components in the Murchison C2 chondrite

Rare gases were analyzed by stepped heating in five fractions of a chemically resistant residue from Murchison that had been separated according to grain size and resistance to HClO4. Nine gas components were recognized, of which three appear to be presolar: (1) Ne-E(H) released at 1000-1600 C and located in spinel; (2) Ne-E(L) released at less than 800 C and apparently located in a carbonaceous phase of grain size up to 10 microns; and (3) s-process Xe and Kr released at 1200-1600 C and located in a poorly characterized, possibly carbonaceous phase, distinct from the host phase of Ne-E(L).

Alaerts, L.↗

Krypton and xenon in lunar fines

Data from grain-size separates, stepwise-heated fractions, and bulk analyses of 20 samples of fines and breccias from five lunar sites are used to define three-isotope and ordinate intercept correlations in an attempt to resolve the lunar heavy rare gas system in a statistically valid approach. Tables of concentrations and isotope compositions are given.

Basford, J. R.↗

Online collection of LC effluent as droplets for automatic injection into ICP-MS

A sample introduction technique was developed to allow for online, dropwise injection of effluent into a mass spectrometer (MS). This allowed for the coupling of chromatography systems that were not driven by pumps without altering the set-up or separation performance. This capability combined the benefits of coupling separation and measurement while also enabling accurate chromatographic evaluation that would generally be performed offline. The incorporation of a flowing rinse into the system made dropwise resolution possible for any liquid capable of forming drops under ambient conditions. The technique was demonstrated utilizing gas pressurized extraction chromatography (GPEC) and inductively coupled plasma-time-of-flight mass spectrometry (ICP-TOFMS) to illustrate the qualitative applications for rapid separation development and procedure evaluation. This method's quantitative applications were evaluated using single and double isotope dilution mass spectrometry (IDMS) with an external mass bias correction to measure analytes across entire elutions including volumes as small as single drops. In conclusion, the total neodymium values afforded by both single and double IDMS were within the uncertainty of the calculated value for evaluation of full elution peaks and for most of the single drops analyzed that reached above 10k cps Nd-144.

GPEC↗

Effects of gas purity on backgrounds of collision reaction cell-equipped MC-ICP-MS

The advent of multi-collector inductively coupled plasma mass spectrometry (MC-ICP-MS) instruments equipped with collision reaction cells (CRCs) facilitates interference removal/mitigation via online gas phase separations. This approach has proven effective for high intensity ion beams measured on Faraday collectors; however, it has been observed that introduction of gas in the CRC can result in significant background signals relative to the more sensitive ion counters. These backgrounds hinder use of these instruments for low level concentration and isotopic ratio measurements when employing a reaction gas. Here, this work directly evaluates the effect of gas purity on backgrounds of CRC-MC-ICP-MS instruments. Introducing high-purity research grade O 2 (99.999%) into the CRC produces complex background spectra with intensities >10 4 cps observed at most masses across the measured mass range (7-300 m / z ). Some features of the observed spectra (i.e., positive mass defects) can be attributed to molecular compounds comprised of significant hydrogen. Additionally, some specific molecular species can be identified (i.e., MoO x H y + ) and appear to be derived from molybdenum rods comprising the CRC. Further purifying the gas reduces the intensity of these backgrounds by several orders of magnitude, to <10 2 cps in many cases, and reduces complexity of the resulting spectra. This reduction in background appears to be in part driven by removal of impurities (i.e., H 2 O) from the gas. This work demonstrates that additional purification of reaction gases prior to introduction into the CRC significantly reduces backgrounds detected, potentially expanding the utility of CRC-MC-ICP-MS for making low level measurements using inline gas phase ion separations.

Schlieder, Tyler D. [Pacific Northwest National La↗

Experimental Setup to Investigate Hydrogen Isotope Retention on Powder Samples as Slag/Dust Proxies for Advanced Fusion Reactors

Slag/dust formation is one of the critical issues regarding tritium retention in advanced fusion reactors. We upgraded an ultrahigh vacuum device, the sample exposure station (SES), to perform temperature-programmed desorption (TPD), also known as thermal desorption spectroscopy, to investigate deuterium (D) retention in powder samples that are utilized as proxies for slag/dust particles formed in fusion reactors. TPD analysis, calibrated for the desorption rate, was successfully performed on commercially available crystalline/amorphous boron (B) powder after D 2 neutral gas or D + ion exposure. We calibrated the B powder temperature measurement for TPD analysis utilizing a D 2 desorption peak from B-D bonding known for its desorption temperature ~700 K. We introduce a separation procedure of observed D TPD signals, convoluted for corresponding D retention pathways, that was necessary for TPD analysis. This is the first report on the retention of D 2 neutral gas to B, and this observation was enabled by utilizing the B powder sample, which has a larger surface area than films commonly used in laboratory experiments. In conclusion, the upgraded SES system will enable us to investigate hydrogen isotope behaviors for powder/dust samples of various elemental compositions, including metals.

Plasma-facing component debris↗

Carbon and Sulfur Isotopic Composition of Yellowknife Bay Sediments: Measurements by the Sample Analysis at Mars (SAM) Quadrupole Mass Spectrometer

Since landing at Gale Crater in Au-gust 2012, the Sample Analysis at Mars (SAM) instru-ment suite on the Mars Science Laboratory (MSL) “Curiosity” rover has analyzed solid samples from the martian regolith in three locations, beginning with a scoop of aeolian deposits from the Rocknest (RN) sand shadow. Curiosity subsequently traveled to Yellowknife Bay, where SAM analyzed samples from two separate holes drilled into the Sheepbed Mudstone, designated John Klein (JK) and Cumberland (CB). Evolved gas analysis (EGA) of all samples revealed the presence of H2O as well as O-, C- and S-bearing phas-es, in most cases at abundances below the detection limit of the CheMin instrument. In the absence of definitive mineralogical identification by CheMin, SAM EGA data can help provide clues to the mineralogy of volatile-bearing phases through examination of tem-peratures at which gases are evolved from solid sam-ples. In addition, the isotopic composition of these gas-es may be used to identify possible formation scenarios and relationships between phases. Here we report C and S isotope ratios for CO2 and SO2 evolved from the JK and CB mudstone samples as measured with SAM’s quadrupole mass spectrometer (QMS) and draw com-parisons to RN.

Franz, H. B.↗

Compound Specific Hydrogen Isotope Composition of Type II and III Kerogen Extracted by Pyrolysis-GC-MS-IRMS

The use of Hydrogen (H) isotopes in understanding oil and gas resource plays is in its infancy. Described here is a technique for H isotope analysis of organic compounds pyrolyzed from oil and gas shale-derived kerogen. Application of this technique will progress our understanding. This work complements that of Pernia et al. (2013, this meeting) by providing a novel method for the H isotope analysis of specific compounds in the characterization of kerogen extracted by analytically diverse techniques. Hydrogen isotope analyses were carried out entirely "on-line" utilizing a CDS 5000 Pyroprobe connected to a Thermo Trace GC Ultra interfaced with a Thermo MAT 253 IRMS. Also, a split of GC-separated products was sent to a DSQ II quadrupole MS to make semi-quantitative compositional measurements of the extracted compounds. Kerogen samples from five different basins (type II and III) were dehydrated (heated to 80 C overnight in vacuum) and analyzed for their H isotope compositions by Pyrolysis-GC-MS-TC-IRMS. This technique takes pyrolysis products separated via GC and reacts them in a high temperature conversion furnace (1450 C) which quantitatively forms H2, following a modified method of Burgoyne and Hayes, (1998, Anal. Chem., 70, 5136-5141). Samples ranging from approximately 0.5 to 1.0mg in size, were pyrolyzed at 800 C for 30s. Compounds were separated on a Poraplot Q GC column. Hydrogen isotope data from all kerogen samples typically show enrichment in D from low to high molecular weight compounds. Water (H2O) average deltaD = -215.2 (V-SMOW), ranging from -271.8 for the Marcellus Shale to -51.9 for the Polish Shale. Higher molecular weight compounds like toluene (C7H8) have an average deltaD of -89.7 0/00, ranging from -156.0 for the Barnett Shale to -50.0 for the Monterey Shale. We interpret these data as representative of potential H isotope exchange between hydrocarbons and sediment pore water during formation within each basin. Since hydrocarbon H isotopes readily exchange with water, these data may provide some useful information on gas-water or oil-water interaction in resource plays, and further as a possible indicator of paleo-environmental conditions. Alternatively, our data may be an indication of H isotope exchange with water and/or acid during the kerogen isolation process. Either of these interpretations will prove useful when deciphering H isotope data derived from kerogen analysis. More experiments are planned to discern these two or other possible scenarios.

Socki, Richard A.↗

Isotopic analyses of nitrogenous compounds from the Murchison meteorite: ammonia, amines, amino acids, and polar hydrocarbons

The combined volatile bases (ammonia, aliphatic amines, and possibly other bases), ammonia, amino acids, and polar hydrocarbons were prepared from the Murchison meteorite for isotopic analyses. The volatile bases were obtained by cryogenic transfer after acid-hydrolysis of a hot-water extract and analyzed by combined gas chromatography-mass spectrometry of pentafluoropropionyl derivatives. The aliphatic amines present in this preparation comprise a mixture that includes both primary and secondary isomers through C5 at a total concentration of > or = 100 nmoles g-1. As commonly observed for meteoritic organic compounds, almost all isomers through C5 are present, and the concentrations within homologous series decrease with increasing chain length. Ammonia was chromatographically separated from the other volatile bases and found at a concentration of 1.1-1.3 micromoles g-1 meteorite. The ammonia analyzed includes contributions from ammonium salts and the hydrolysis of extractable organic compounds, e.g., carboxamides. Stable isotope analyses showed the volatile bases to be substantially enriched in the heavier isotopes, relative to comparable terrestrial compounds delta D < or = +1221%; delta 13C = +22%; delta 15N = +93%). Ammonia, per se, was found to have a somewhat lower delta 15N value (+69%) than the total volatile bases; consequently, a higher delta 15N (>93%) can be inferred for the other bases, which include the amines. Solvent-extractable polar hydrocarbons obtained separately were found to be enriched in 15N (delta 15N = +104%). Total amino acids, prepared from a hydrolyzed hot-water extract by cation exchange chromatography, gave a delta 15N of +94%, a value in good agreement with that obtained previously. Nitrogen isotopic data are also given for amino acid fractions separated chromatographically. The delta 15N values of the Murchison soluble organic compounds analyzed to date fall within a rather narrow range (delta 15N = +94 +/- 8%), an observation consistent with their formation, or formation of their precursors, by interstellar chemistry.

Non-NASA Center↗

Developments and Challenges in the Design of the ITER DRGA

We report the ITER Diagnostic Residual Gas Analyzer (DRGA) will measure the distribution of gas species, i.e., deuterium (D), tritium (T), and impurities, in the divertor exhaust stream and in the plasma periphery, with time resolution relevant to fusion plasma–wall particle dynamics. The uniqueness of the DRGA, over previous implementations of plasma dynamics residual gas analysis, is an integrated approach, combining mass and low-temperature plasma-activated optical spectroscopy, in a differentially pumped analysis station. A further unique feature of the ITER divertor-specific DRGA is an ~8-m separation of the analysis station from the sampled pumping duct, while still maintaining a ~1-s response time for hydrogen isotopic concentrations. ITER DRGA final design activities are strongly benefiting from testing of prototypical DRGA components and methods on present fusion devices, most currently on JET and W7-X. DRGA systems are implemented on both these devices and include sensors (and pumping methods) that are directly relevant to the ITER DRGA design. The recent JET-DTE2 campaign has provided the first experience on operating the combined ITER DRGA sensors with D-T plasmas. While enhancing system design for ITER, this experience on operating devices has also revealed additional engineering challenges, which further guide the continuing final design project. Meanwhile, the recent determination that the ITER DRGA, with slight optimization, will resolve the helium isotopes well enough to support an ITER pre-DT, He-3-based heating scheme, has greatly increased ITER Research Program interest in the DRGA and its implementation well ahead of the DT phase.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Neon isotope studies of Fayetteville and Kapoeta meteorites and clues to ancient solar activity

Under the assumption that the solar-flare bombardment of the irradiated grains of gas-rich meteorites occurred about 4.5 b.y. ago on the parent body regoliths at 3 A.U., an estimate of the solar cosmic ray-produced Ne-21 is made by studying etched pyroxene minera separates from both light and dark portions of the gas-rich meteorites Fayetteville and Kapoeta. Excesses of solar cosmic ray Ne-21 were observed in dark portions of these meteorites, after accounting for their galactic cosmic ray Ne-21 production and solar flare Ne-21. In order to produce the estimated solar cosmic ray Ne-21 in the present samples, highly enhanced solar cosmic ray proton fluxes from the ancient sun are required.

Padia, J. T.↗

Dataset for Cruz-O'Byrne et al (2026): "Divergent biogeochemical responses in upland coastal forest soils to repeated flooding and shifts in water chemistry"

Hydrologic disturbances from accelerated sea-level rise and the increasing frequency and intensity of storms and tidal flooding are altering biogeochemical processes in upland coastal forests, transforming these ecosystems into wetlands. However, the initial effects of flooding on belowground biogeochemistry and the mechanisms driving greenhouse gas dynamics and soil organic matter stability during the early stages of this transition remain poorly understood. This dataset presents the results of a mesocosm experiment conducted in a controlled, highly instrumented laboratory environment, in which freshwater and brackish water pulses were applied to intact soil monoliths from a temperate upland coastal forest to examine how floodwater chemistry influences soil biogeochemistry and organo-mineral interactions. All data files are plain-text CSV (comma-separated value), and no special software is required to read them. Details about the content of each file are available in the document “Dataset_readme”. The dataset consists of the following data: • rcruzobyrne_moisture: Soil volumetric water content (VWC) • rcruzobyrne_GHG: Headspace greenhouse gas (GHG) concentration and fluxes • rcruzobyrne_methane_isotopes: Headspace methane isotope signature • rcruzobyrne_porewater: Porewater chemistry • rcruzobyrne_CDOM: Porewater colored dissolved organic matter (CDOM) • rcruzobyrne_FTIR: Soil Fourier-transform infrared (FTIR) spectroscopy Details of the experimental setup, data collection, and data analysis are provided in the manuscript by Cruz-O’Byrne et al (2026) Divergent biogeochemical responses in upland coastal forest soils to repeated flooding and shifts in water chemistry. Biogeochemistry. https://doi.org/10.1007/s10533-026-01340-0

EARTH SCIENCE > ATMOSPHERE > GREENHOUSE GAS↗

Carbon Isotope Characterization of Organic Intermediaries in Hydrothermal Hydrocarbon Synthesis by Pyrolysis-GC-MS-C-IRMS

We report results of experiments designed to characterize the carbon isotope composition of intermediate organic compounds produced as a result of mineral surface catalyzed reactions. The impetus for this work stems from recently reported detection of methane in the Martian atmosphere coupled with evidence showing extensive water-rock interaction during Martian history. Abiotic formation by Fischer-Tropsch-type (FTT) synthesis during serpentinization reactions may be one possible process responsible for methane generation on Mars, and measurement of carbon and hydrogen isotopes of intermediary organic compounds can help constrain the origin of this methane. Of particular interest within the context of this work is the isotopic composition of organic intermediaries produced on the surfaces of mineral catalysts (i.e. magnetite) during hydrothermal experiments, and the ability to make meaningful and reproducible isotope measurements. Our isotope measurements utilize a unique analytical technique combining Pyrolysis-Gas Chromatograph-Mass Spectrometry-Combustion-Isotope Ratio Mass Specrometry (Py-GC-MS-C-IRMS). Others have conducted similar pyrolysis-IRMS experiments on low molecular weight organic acids (Dias, et al, Organic Geochemistry, 33 [2002]). Our technique differs in that it carries a split of the pyrolyzed GC-separated product to a Thermo DSQ-II quadrupole mass spectrometer as a means of making qualitative and semi-quantitative compositional measurements of the organic compounds. A sample of carboxylic acid (mixture of C1 through C6) was pyrolyzed at 100 XC and passed through the GC-MS-C-IRMS (combusted at 940 XC). In order to test the reliability of our technique we compared the _13C composition of different molecular weight organic acids (from C1 through C6) extracted individually by the traditional sealed-tube cupric oxide combustion (940 XC) method with the _13C produced by our pyrolysis technique. Our data indicate that an average 4.3. +/-0.5. (V-PDB) apparent isotopic fractionation accompanies the pyrolysis extractions. We postulate that this isotope offset could be the result of incomplete thermal desorption during pyrolysis. We are continuing to investigate the reliability of this pyrolysis technique for correcting carbon isotope measurements of mineral surface catalyzed organic compounds.

Socki, Richard A.↗

Mesoscale Modeling of the Effects of Accelerated Burnup on UO2 Microstructural Evolution

Accelerating the nuclear fuel qualification process will rely on some combination of advanced modeling and simulation techniques with accelerated irradiation testing and separate effects experiments to enable the development of new fuel concepts in a shorter time frame. One of the key challenges to successfully leveraging accelerated irradiation tests will be understanding the artifacts that may be introduced with accelerated accumulation of dose and/or burnup. This work presents phase field (MARMOT) simulations of the evolution of representative 2D UO2 microstructures up to 40 MWd/kgU. Simulations were performed under both commercial light water reactor fuel conditions as well as those that would be expected for highly accelerated (~10x) burnup conditions similar to those used in the MiniFuel irradiations in Oak Ridge National Laboratory’s High Flux Isotope Reactor. The phase field model was coupled with a discrete nucleation algorithm to model re- structuring at high burnup. The effect of the different fission rates in both microstructures was investigated at two temperatures: 650?C and 800?C. The lower temperature simulations both showed an onset of restructuring at nearly 60 MWd/kgU. More extensive restructuring was obtained in the MiniFuel microstructure compared with that of the PWR fuel. At 800?C, no restructuring was obtained as a result of the thermally activated diffusion of Xe atoms and U vacancies to fission gas bubbles, which reduces the nucleation driving force. These results highlight the importance of using modeling and simulation tools to inform the environmental conditions during targeted accelerated irradiation tests to extract the most useful fuel performance data.

accelerated fuel qualification, Phase Field, Restr↗