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At least 55 records · Page 3
All sourcesNASA NTRSDOE OSTI
NASA NTRS1979

The elemental and isotopic abundances of H, C, N, O in comets

The elemental abundances of light elements in comets is discussed by considering gas and dust separately. It is noted that the icy conglomerate model of the nucleus (Whipple, 1957) has been confirmed, and that the dust-to-gas mass ratio has been estimated within a factor of two for two recent comets. It is found that the total amount of oxygen available is also nominally in solar abundance; this implies that the oxygen of the solar nebula has probably been quantitatively bound in compounds that have been completely condensed and accreted in cometary nuclei. In addition, the amount of hydrogen is clearly depleted by a factor of 2,000, suggesting that the only hydrogen present is that linked in molecular compounds of H, C, N and O.

Delsemme, A. H.↗
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↗
NASA NTRS1992

Solar-type xenon - Isotopic abundances in Pesyanoe

Elemental and isotopic abundances of Ar and Xe were measured in three grain-size separates in the dark phase of the enstatite achondrite Pesyanoe by stepwise heating, using a combination of pyrolysis and combustion steps. The data reveal a low-temperature gas fraction with Ar/Xe ratios close to the solar ratio and isotopically similar to solar-type Ar and Xe observed in lunar samples. The gas released at intermediate temperature steps shows that Ar and Xe are isotopically fractionated, compared to the low-temperature components. Pesyanoe does not have excess Ar-40 and fission Xe, which means its parent body was too small for ion reimplantation. It is concluded that solar-type Xe isotopic abundances can be inferred from the low-temperature component. A comparison of Pesyanoe and lunar data shows that isotopic signatures of solar-wind Xe, as sampled at two different points in solar system space and time, are identical within experimental error.

Kim, J. S.↗
NASA NTRS1979

Laboratory corroboration of the Pioneer Venus gas chromatograph analyses

Laboratory simulation and tests of the inlet sampling system and columns of the Pioneer Venus gas chromatograph show that the sensitivity to argon is not diminished after the column regeneration step, that argon isotopes are not separated, that oxygen and sulfur dioxide are not produced in the inlet sampling system from sulfur trioxide, and that sulfur trioxide is not formed from sulfur dioxide and oxygen. Comparisons of the volatile inventory of Venus and earth imply similar efficiencies of early outgassing but a lower efficiency for later outgassing in the case of Venus. The high oxidation state of the Venus atmosphere in the region of cloud formation may prohibit the generation of elemental sulfur particles.

Oyama, V. I.↗
DOE OSTI2023

Liquid solution centrifugation for safe, scalable, and efficient isotope separation

A general method of separating isotopes by centrifuging dissolved chemical compounds in a liquid is introduced. This technique can be applied to almost all elements and leads to large separation factors. The method has been demonstrated in several isotopic systems including Ca, Mo, O, and Li with single-stage selectivities of 1.046 to 1.067 per neutron mass difference (e.g., 1.43 in 40 Ca/ 48 Ca), which are beyond the capabilities of various conventional methods. Equations are derived to model the process, and the results agree with those of the experiments. The scalability of the technique has been demonstrated by a three-stage enrichment of 48 Ca with a total 40 Ca/ 48 Ca selectivity of 2.43, and the scalability is more broadly supported through analogies to gas centrifuge, whereby countercurrent centrifugation can further multiply the separation factor by 5 to 10 times per stage in a continuous process. Optimal centrifuge conditions and solutions can achieve both high-throughput and highly efficient isotope separation.

07 ISOTOPE AND RADIATION SOURCES↗
NASA NTRS1980

Solar wind sputtering effects in the atmospheres of Mars and Venus

It is found through an investigation, combining Monte Carlo simulations and analytical techniques, of the direct collisional interaction of an energetic particle flux with the neutral components of a planetary atmosphere, that solar wind sputtering could provide an important exospheric mass sink on both Mars and Venus under appropriate conditions. The computed rates of helium loss in the Venusian atmosphere and of carbon, nitrogen and oxygen in the Martian atmosphere imply that sputtering would have a significant effect on the noble gas budget of Venus and dominate the chemical and photochemical loss processes of Mars. Because of diffusive separation of lighter elements and isotopes, and because the gravitational binding energy is proportional to the mass, the erosion process preferentially removes the lighter components of the atmosphere. Solar wind sputtering could therefore compete with other erosion mechanisms in generating substantial fractionation effects.

Watson, C. C.↗
NASA NTRS1995

Carbon isotopic analysis of atmospheric methane by isotope-ratio-monitoring gas chromatography-mass spectrometry

Less than 15 min are required for the determination of delta C(sub PDB)-13 with a precision of 0.2 ppt(1 sigma, single measurement) in 5-mL samples of air containing CH4 at natural levels (1.7 ppm). An analytical system including a sample-introduction unit incorporating a preparative gas chromatograph (GC) column for separation of CH4 from N2, O2, and Ar is described. The 15-min procedure includes time for operation of that system, high-resolution chromatographic separation of the CH4, on-line combustion and purification of the products, and isotopic calibration. Analyses of standards demonstrate that systematic errors are absent and that there is no dependence of observed values of delta on sample size. For samples containing 100 ppm or more CH4, preconcentration is not required and the analysis time is less than 5 min. The system utilizes a commercially available, high-sensitivity isotope-ratio mass spectrometer. For optimal conditions of smaple handling and combustion, performance of the system is within a factor of 2 of the shot-noise limit. The potential exists therefore for analysis of samples as small as 15 pmol CH4 with a standard deviation of less than 1 ppt.

Merritt, Dawn A.↗
NASA NTRS2004

Modeling of Isotope Fractionation in Stratospheric CO2, N2O, CH4, and O3: Investigations of Stratospheric Chemistry and Transport, Stratosphere-Troposphere Exchange, and Their Influence on Global Isotope Budgets

We investigated the isotopic fractionation of CH4 and hydrogen (H2) in the stratosphere by incorporating isotope-specific rate coefficients into the Lawrence Livermore National Laboratory (LLNL) 2D model and comparing the model results with new observations from the NASA ER-2 aircraft (funded through a separate task under the Upper Atmosphere Research Program). The model results reveal that fractionation which occurs in the stratosphere has a significant influence on isotope compositions in the free troposphere, an important point which had previously been ignored, unrecognized or unquantified for many long-lived trace gases, including CH4 and H2 which we have focused our efforts on to date. Our analyses of the model results and new isotope observations have also been used to test how well the kinetic isotope effects are known, at least to within the uncertainties in model chemistry and transport. Overall, these results represent an important step forward in our understanding of isotope fractionation in the atmosphere and demonstrate that stratospheric isotope fractionation cannot be ignored in modeling studies which use isotope observations in the troposphere to infer the global budgets of CH4 (an important greenhouse gas) and of H2 (a gas whose atmospheric budget must be better quantified, particularly before a large human perturbation from fuel cell use is realized). Our analyses of model results and observations from the NASA ER-2 aircraft are briefly summarized separately below for CH4, H2, and H2O and for the contribution of these modeling studies to date to our understanding of isotope fractionation for N2O, CO2, and O3 as well.

Boering, Kristie A.↗
NASA NTRS1997

Extraterrestrial Helium (He@C60) Trapped in Fullerenes in the Sudbury Impact Structure

Fullerenes (C60 and C70) have recently been identified in a shock-produced breccia (Onaping Formation) associated with the 1.85-Ga Sudbury Impact Crater. The presence of parts-per-million levels of fullerenes in this impact structure raises interesting questions about the processes that led to the formation of fullerenes and the potential for delivery of intact organic material to the Earth by a large bolide (e.g., asteroid or comet). Two possible scenarios for the presence of fullerenes in the Sudbury impact deposits are that (1) fullerenes are synthesized within the impact plume from the C contained in the bolide; or (2) fullerenes are already present in the bolide and survived the impact event. The correlation of C and trapped noble gas atoms in meteorites is well established. Primitive meteorites contain several trapped noble gas components that have anomalous isotopic compositions, some of which may have a presolar origin. Several C-bearing phases, including SiC, graphite, and diamond, have been recognized as carriers of trapped noble gases. It has also been suggested that fullerenes (C60 and C70) might be a carrier of noble gas components in carbonaceous chondrites. Recently, fullerenes have been detected in separate samples in the Allende meteorite. Carbon-60 is large enough to enclose the noble gases He, Ne, Ar, Kr, and Xe, but it is too small to contain diatomic gases such as N2 or triatomic gases such as CO2. Recent experimental work has demonstrated that noble gases of a specific isotopic composition can be introduced into synthetic fullerenes at high temperatures and pressures; these encapsulated gases can then be released by the breaking of one or more C bonds during step-heating under vacuum. These thermal-release patterns for He encapsulated within the C60 molecule (He@C60) are similar to the patterns for acid residues of carbonaceous chondrites, suggesting that fullerenes could be an additional carrier of trapped noble gases in acid residues of meteorites. Analysis and Results: In order to characterize the noble gas compositions of the Sudbury fullerenes, we undertook a systematic study of acid-resistant residues throughout the C-rich layer (Black member) of the Onaping Formation. Samples were demineralized and extracted using standard techniques. The Onaping extracts were analyzed using several techniques, including UV-Vis adsorption, electro spray mass spectrometry, and laser desorption (linear and reflectron) time-of-flight (TOF) mass spectrometry (LDMS). The Sudbury fullerenes were then separated and purified using HPLC coupled with a photo diode array detector. The HPLC extracts containing the purified fullerenes were loaded into a metal tube furnace within a glove box under a N atmosphere in preparation for noble gas analyses. The 3-He and 4-He content of the fullerene extracts was measured using previously reported standard techniques . Discussion: Fullerenes (C60 and C70) in the Sudbury Impact Structure have been found to contain trapped He with a 3-He/4-He ratio greater than 5 x 10(exp -4). The 3-He/4-He ratio exceeds the accepted solar value by more than 30% and is more than 10x higher than the maximum reported mantle value. Terrestrial nuclear reactions or cosmic-my bombardment are not sufficient to generate such a high ratio. The 3-He/4-He ratios in the Sudbury fullerenes are similar to those determined for interplanetary dust particles. The greater-than-solar ratios of 3-He/4-He in the Sudbury fullerenes may indicate a presolar origin, although alternative mechanisms occurring in the ISM to explain these high ratios (e.g., spallation reactions, selective He implantation, etc.) cannot be entirely ruled out. We are currently attempting to isolate enough fullerene material to measure anomalous Ne (or Kr or Xe) contained within the C60 (e.g., the "pure" 22-Ne component) and thus determine whether the Sudbury fullerenes are indeed presolar in origin.

Becker, L.↗
NASA NTRS1972

Rare gas studies of the galactic cosmic ray irradiation history of lunar rocks.

Average irradiation depths and exposure ages of Tranquillity Base rocks are computed on the basis of eight analyses of the five noble gases in whole rock samples and lunar separates from lunar rocks, in conjunction with available literature data. Correlated variations in He-3/Ne-21 and Ar-38/Ne-21 reflect shielding differences. This correlation cannot be explained by diffusion losses, even though evidence for gas loss is obtained from mineral separate data. A qualitative shielding sequence is constructed which agrees reasonably well with the sequence based on Gd isotopic data.

Huneke, J. C.↗
NASA NTRS1994

Noble gases in presolar diamonds II: Component abundances reflect thermal processing

Using the isotopic compositions derived in Huss and Lewis, 1994a, abundances of the P3, HL, and P6 noble-gas components were determined for 15 diamonds separates from primitive chondrites of 8 chondrite classes. Within a meteorite class, the relative abundances of these components correlate with the petrologic subtype of the host meteorite, indicating that metamorphism is primarily responsible for the variations. Relative abundances of P3, HL, and P6 among diamond samples can be understood in terms of thermal processing of a single mixture of diamonds like those now found in CI and CM2 chondrites. With relatively gentle heating, primitive diamonds first lose their low-temperature P3 gases and a 'labile' fraction of the HL component. Mass loss associated with release of these components produces an increase in the HL and P6 content of the remaining diamond relative to unprocessed diamond. Higher temperatures initiate destruction of the main HL carrier, while the HL content of the surviving diamonds remains essentially constant. At the same time, the P6 carrier begins to preferentially lose light noble gases. Meteorites that have experienced metamorphic temperatures greater than or = 650 C have lost essentially all of their presolar diamond through chemical reactions with surrounding minerals. The P3 abundance seems to be a function only of the maximum temperature experienced by the diamonds and thus is independent of the nature of the surrounding environment. If all classes inherited the same mixture of primitive diamonds, then P3 abundances would tie together the metamorphic scales in different meteorite classes. However, if the P3 abundance indicates a higher temperature than do other thermometers applicable to the host meteorite, then the P3 abundance may contain information about heating prior to accretion. Diamonds in the least metamorphosed EH, CV, and CO chondrites seem to carry a record of pre-accretionary thermal processing.

Huss, Gary R.↗
NASA NTRS1993

A search for noble-gas evidence for presolar oxide grains

Early results from an ongoing search for isotopically distinctive noble gases as evidence for presolar oxide grains are presented. With some qualifications, we do not see such evidence in spinel rich acid residue fractions from the Allende meteorite. We remain hopeful that less abundant mineral separates may yet be fruitful. Presolar grains, micro-diamonds, silicon carbide, and graphite, were found in primitive meteorites. While the abundances of these three refractory C rich grains are low, a few hundred ppm, a few ppm, & less than 1 ppm, respectively in primitive meteorites, they are tagged with high concentrations of isotopically anomalous noble gas components, Xe-HL, KR & Xe-s and Ne-E(H), and Ne-E(L). These tags have served as tracers and allowed the development of techniques for their purification and eventual identification. One might expect similar amounts of refractory presolar oxides to have survived, but so far only three cases exist for their identification. The first two cases are individual corundum oxide grains. Huss et al. found one such grain from an Orgueil residue with an Al-26/Al-27 ratio of 8.9 x 10(exp -5), about 18 times higher than the canonical initial solar system value. The second corundum grain, from Murchison, was found by Nittler et al. to have unusual oxygen in addition to a similar Al-26/Al-27 ratio of 8.7 x 10(exp -4). The oxygen was depleted in O-18 by 22 percent and enriched in O-17 by a factor of 2. The third case is a measurement by Zinner et al. on an aggregate of fine grained spinels from a Murray residue with an O-17 enrichment and a possible O-18 depletion similar to the second grain, but much subdued. This is consistent with a few such presolar grains diluted by a much larger population of isotopically normal corundum grains and an even larger number of normal spinel grains.

Lewis, Roy S.↗
DOE OSTI2025

Preliminary Testing of a Continuous Cryopump for Primary Fusion Device Pumping and Direct Internal Recycling

Here, the concept of directly recirculating fusion machine exhaust gas, bypassing the tritium plant, to make fuel pellets was proposed in the 1990s and later termed direct internal recycling (DIR). In the DIR concept, the residual fusion fuel in the machine exhaust stream is separated from impurities locally and diverted directly to the fueling systems, bypassing isotopic separation and other processing equipment, and therefore significantly reducing the required size of the fuel processing plant, reducing plant inventory, and thus increasing the economic viability of fusion as an energy source. One concept for DIR consists of a series of cryogenic pumps to separate the impurities from the machine exhaust gas using different triple point temperatures and saturation curves of exhaust constituents. In this concept, the plasma exhaust is initially passed through an impurity trap operating at ~25–30 K to desublimate impurities such as hydrocarbons, argon, oxygen, and nitrogen. The resulting process stream will consist of DT fuel and helium. The process stream is then pumped by a continuous cryopump known as a “snail pump.” This pump is a steady-state continuous cryopump that desublimates all remaining exhaust gas constituents while allowing helium, a byproduct of the fusion reaction, to pass through. The helium is pumped to the tritium plant for processing while the desublimated material is continuously scraped off, heated up, and transported to the fueling system. This article will present the cryogenic DIR concept and outline the design and operation of the snail pump, along with results from preliminary testing. Tests to assess pumping and separation efficiency found that at D2 flows below 50.7 Pa ⋅ m3/s with 1% helium, the pump is capable of pumping and separating the gas with a resulting DIR fraction of >99%, with no helium entrained in the primary fuel exhaust stream. The main limitation is due to the thermal performance of the cryogenic circuits of the pump, which will be addressed in future testing.

Gebhart III, Trey E. [Oak Ridge National Laborator↗
DOE OSTI2025

Design Report on the MiniFuel Instrumented Test Apparatus for Understanding Radiation Effects

Most nuclear fuels irradiations at Oak Ridge National Laboratory (ORNL) over the past decade have been conducted using MiniFuel—a static capsule design employing subscale fuel specimens to collect separate-effects irradiated fuel performance data. Irradiation conditions for MiniFuel experiments are predicted pre-test using reactor physics, and thermal models are verified post-irradiation via SiC dilatometry and various spectrometry methods. Relevant fuel performance parameters are also observed post-irradiation in a hot cell, thereby providing a single data point for each parameter representing the cumulative effects of the irradiation conditions. Substantially more data can be harvested from a single test and within a shorter duration by instrumenting irradiation vehicles and measuring desired quantities in situ. This report presents the design and analysis of the MiniFuel INstrumented Irradiation Test Apparatus for Understanding Radiation Effects (MINITAURE)—an instrumented test rig based on the separate-effects MiniFuel concept that aims to capture fission gas release (FGR) and thermal conductivity degradation of fuel specimens during irradiation in the High Flux Isotope Reactor (HFIR). MINITAURE will be integrated with the Materials Irradiation Facility (MIF) located in the HFIR building outside the reactor containment. The MIF will act as the instrumentation and control center for the experiment, enabling real-time feedback from in situ sensors and control of irradiation temperatures via a gas delivery system. Two unique capsule designs were developed to capture each phenomenon: the thermal conductivity capsule, which uses a thermopile method to estimate fuel specimen thermal conductivity, and the fission gas release capsule, which will have continuous flowing gas communication to high-purity germanium detectors that are housed in the MIF for monitoring FGR. This report details the reactor physics and heat transfer modeling activities that were used to inform the experiment design and predict capsule performance. It also describes out-of-pile activities conducted to stand up this new capability and verify the measurement techniques. Modeling efforts to date have demonstrated the feasibility of the in situ measurement techniques and supported the development of the MINITAURE assembly configuration. Out-of-pile testing of the thermal conductivity measurement shows promise in capturing relative changes in thermal conductivity. However, significant errors exist in the measured absolute value, posing a need for further refinement.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2026

Investigation of the 244 Pu ⁢( 48 Ca,𝑥⁢𝑛) 292−𝑥 Fl reaction with the LBNL SHREC detector: Investigation of decay chains of isotopes of flerovium (𝑍=114)

The 244 Pu ⁢( 48 Ca,𝑥⁢𝑛)⁢ 292−𝑥 Fl reaction was investigated at Lawrence Berkeley National Laboratory’s 88 Inch Cyclotron using the Berkeley Gas-filled Separator (BGS), the newly installed Superheavy Recoil detector, along with an upgraded digital electronics and data acquisition system. Seven decay chains were observed starting with an evaporation residue, followed by a single 𝛼 decay and a spontaneous fission. The decay characteristics of these seven decay chains led to an assignment to 288 Fl , the product of the 4⁢𝑛 reaction channel. Two additional chains were (tentatively) assigned to the decay of the 3⁢𝑛 exit channel, 289 Fl . Cross sections for the 4⁢𝑛 and 3⁢𝑛 exit channels were 𝜎 prod =6.7⁢($^{36}_{25}$) pb and 𝜎 prod =1.6⁢($^{22}_{11}$) pb, respectively. Another decay chain, tentatively assigned to the 5⁢𝑛 exit channel through the 48 Ca + 244 Pu reaction or the 3⁢𝑛 exit channel of the 48 Ca + 242 Pu reaction, was also detected. Detailed information regarding the observed decay chains and their nuclear structure aspects is discussed, along with the performance of the BGS and the new detection system.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
NASA NTRS1972

Oxygen isotope cosmothermometer.

Variations in oxygen isotopic abundances of meteoritic minerals, chondrules, whole meteorites, and planets are discussed in terms of a model involving isotopic exchange between primordial dust and a cooling solar nebular gas. From the temperature-dependence of the isotopic fractionation factors, temperatures have been assigned to the processes of initial condensation, chondrule formation, and planetary accretion. Separated phases from carbonaceous chondrites fall into three isotopic groups representing widely differing conditions of formation: (1) low-iron olivine and pyroxene, and calcium-aluminum silicates condensed at temperatures above 1000 K; (2) high-iron olivine and pyroxene melted to form chondrules after prior cooling and exchange to temperatures of 530-620 K; and (3) hydrous silicates condensed at temperatures below 400 K.

Onuma, N.↗
NASA NTRS1984

Colloidally separated samples from Allende residues - Noble gases, carbon and an ESCA-study

Results are presented which strengthen the hypothesis of heterogeneity among the carbon- and nitrogen-bearing phases of the Allende meteorite. These data also highlight the possibility of performing physical separations yielding samples in which some of the noble gas- and carbon-bearing phases are extraordinarily predominant over others. The conclusion, based on mass and isotope balance arguments, that a significant portion of the carbonaceous matter in Allende is likely to be gas-poor or gas-free need not weaken the case for carbonaceous carriers for the major noble gas components. The concept that acid-soluble carbonaceous phases contain a multiplicity of components, each of which may have formed under a multiplicity of different physical-chemical conditions, is reemphasized by the results of the present study.

Ott, U.↗
NASA NTRS1981

Noble-gas-rich separates from the Allende meteorite

Predominantly carbonaceous HF/HCl-resistant residues from the Allende meteorite are studied. Samples are characterized by SEM/EDXA, X-ray diffraction, INAA, C, S, H, N, and noble gas analyses. Isotopic data for carbon show variations no greater than 5%, while isotopic data from noble gases confirm previously established systematics. Noble gas abundances correlate with those of C and N, and concomitant partial loss of C and normal trapped gas occur during treatments with oxidizing acids. HF/HCl demineralization of bulk meteorite results in similar fractional losses of C and trapped noble gases, which leads to the conclusion that various macromolecular carbonaceous substances serve as the main host phase for normal trapped noble gases and anomalous gases in acid-resistant residues, and as the carrier of the major part of trapped noble gases lost during HF/HCl demineralization. Limits on the possible abundances of dense mineralic host phases in the residues are obtained, and considerations of the nucleogenetic origin for CCF-XE indicate that carbonaceous host phases and various forms of organic matter in carbonaceous meteorites may have a presolar origin.

Ott, U.↗