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At least 541 records · Page 30

Hibonite-bearing microspherules - A new type of refractory inclusions with large isotopic anomalies

This paper presents petrographic description as well as results on the major- and trace-element chemistry and on Mg, Ca, and Ti isotopic compositions of three refractory inclusions, including 3413-1/31 inclusion from Lance and Murchison 7-228 and 7-753, the mineralogy of which is dominated by the oxide minerals spinel, hibonite, and perovskite. The microspherules examined seem to constitute a separate class of refractory inclusions, characterized by a distinct morphology and mineralogy; large excesses of Ca-48 and Ti-50, and Mg-26 depletions. It is suggested that this type of inclusions must have formed early, prior to the dilution of isotopic anomalies by mixing processes, and in an area characterized by excesses of Ca-48 and Ti-50, depletions of Mg-26, and a lack of Al-26.

Ireland, T. R.↗

Demonstration of a 228 Ra/ 228 Ac isotope generator

An isotope generator to produce 228 Ac from 228 Ra was developed using a cation exchange resin column eluted with an acetate-diethylenetriaminpentaacetic acid buffer. Here, the elution behavior of 228 Ac on the column was studied with solutions of various pHs to select the optimal conditions. Two identical isotope generators were eluted for 47 days with over 100 mL of eluant with no detectable 228 Ra breakthrough and high 228 Ac yields (∼95%). The separation requires only biocompatible reagents and is performed at pH 4.6, conditions suitable for radiopharmaceutical studies of Ac.

and nuclear chemistry↗

Round Robin Analysis of Uranium Isotopics on Cotton Swipes Measured Using Microextraction-Based Sampling Versus Conventional Bulk Analysis

A comparison of microextraction sampling methods to directly analyze uranium isotopics on cotton swipes was performed concurrently with traditional bulk-processing methods. For the microextraction sampling approach, two different detection platforms were evaluated, a quadrupole-based inductively coupled plasma mass spectrometer (ICP-MS) and the liquid sampling-atmospheric pressure glow discharge (LS-APGD) coupled to an Orbitrap mass spectrometer. Results presented from this innovative sampling approach (i.e., microextraction) are compared with a more traditional approach employed for analysis of cotton-based environmental swipes, namely bulk ashing/digestion, separation, and subsequent analysis by high-precision multi-collector ICP-MS. Overall, the microextraction approach proved to be a reliable and accurate means to determine isotopic ratios of uranium collected on cotton swipes. The ICP-MS-based detection had relative standard deviations of <0.65% for the major isotopic determinations, whereas the LS-APGD-Orbitrap method had relative standard deviations of <3%. The percent relative difference for the 235 U/ 238 U ratios, in comparison to the expected values, was <1% for ICP-MS and <4% for the microplasma-Orbitrap method. Additionally, the microextraction ICP-MS accurately (<2%) and precisely (<5%) determined the minor isotopic compositions (i.e., 234 U/ 238 U and 236 U/ 238 U).

ICP-MS↗

Atmosphere-entry behavior of a modular, disk-shaped, isotope heat source.

The authors have studied the entry and impact behavior of an isotope heat source for space nuclear power that disassembles into a number of modules which would enter the earth's atmosphere separately if a flight aborted. These modules are disk-shaped units, each with its own reentry heat shield and protective impact container. In normal operation, the disk modules are stacked inside the generator, but during a reentry abort they separate and fly as individual units of low ballistic coefficient. Flight tests at hypersonic speeds have confirmed that a stack of disks will separate and assume a flat-forward mode of flight. Free-fall tests of single disks have demonstrated a nominal impact velocity of 30 m/sec at sea level for a practical range of ballistic coefficients.

Vorreiter, J. W.↗

Mini-Brayton heat source assembly design study. Volume 2: Titan 3C mission

Major conclusions of the space shuttle heat source assembly study are reported that project a minimum weight design for a Titan 3 C synchronous orbit mission; requirements to recover the heat source in orbit are eliminated. This concept permits location of the heat source end enclosure supports and heat source assembly support housing in a low temperature region external to the insulation enclosure and considers titanium and beryllium alloys for these support elements. A high melting insulation blanket consisting of nickel foil coated with zirconia, or of gold foil separated with glass fiber layers, is selected to provide emergency cooling in the range 2000 to 2700 F to prevent the isotope heat source from reaching unsafe temperatures. A graphic view of the baseline heat source assembly is included.

Source record↗

A review of noble gas geochemistry in relation to early Earth history

One of the most fundamental noble gas constraints on early Earth history is derived from isotopic differences in (129)Xe/(130)Xe between various terrestrial materials. The short half life (17 m.y.) of extinct (129I, parent of (129)Xe, means that these differences must have been produced within the first 100 m.y. after terrestrial accretion. The identification of large anomalies in (129)Xe/(130)Xe in mid ocean ridge basalts (MORB), with respect to atmospheric xenon, suggests that the atmosphere and upper mantle have remained separate since that time. This alone is a very strong argument for early catastrophic degassing, which would be consistent with an early fractionation resulting in core formation. However, noble gas isotopic systematics of oceanic basalts show that the mantle cannot necessarily be regarded as a homogeneous system, since there are significant variations in (3)He/(4)He, (40)Ar/(36)Ar, and (129)Xe/(130)Xe. Therefore, the early degassing cannot be considered to have acted on the whole mantle. The specific mechanisms of degassing, in particular the thickness and growth of the early crust, is an important variable in understanding present day noble gas inventories. Another constraint can be obtained from rocks that are thought to be derived from near the lithosphere asthenosphere boundary: ultramafic xenoliths.

Kurz, M. D.↗

Stable hydrogen and carbon isotope ratios of extractable hydrocarbons in the Murchison meteorite

A fairly fool-proof method to ensure that the compounds isolated from meteorites are truly part of the meteorites and not an artifact introduced by exposure to the terrestrial environment, storage, or handling is presented. The stable carbon and hydrogen isotope ratios in several of the chemical compounds extracted from the Murchison meteorite were measured. The results obtained by studying the amino acids in this meteorite gave very unusual hydrogen and carbon isotope ratios. The technique was extended to the different classes of hydrocarbons and the hydrocarbons were isolated using a variety of separation techniques. The results and methods used in this investigation are described in this two page paper.

Krishnamurthy, R. V.↗

The Spatial Distribution of Organic Matter and Mineralogical Relationships in Carbonaceous Chondrites

Organic matter present within primitive carbonaceous meteorites represents the complex conglomeration of species formed in a variety of physically and temporally distinct environments including circumstellar space, the interstellar medium, the Solar Nebula & Jovian sub-nebulae and asteroids. In each case, multiple chemical pathways would have been available for the synthesis of organic molecules. Consequently these meteorites constitute a unique record of organic chemical evolution in the Universe and one of the biggest challenges in organic cosmochemistry has been in deciphering this record. While bulk chemical analysis has provided a detailed description of the range and diversity of organic species present in carbonaceous chondrites, there is virtually no hard experimental data as to how these species are spatially distributed and their relationship to the host mineral matrix, (with one exception). The distribution of organic phases is nevertheless critical to understanding parent body processes. The CM and CI chondrites all display evidence of low temperature (< 350K) interaction with aqueous fluids, which based on O isotope data, flowed along thermal gradients within the respective parent bodies. This pervasive aqueous alteration may have led to aqueous geochromatographic separation of organics and synthesis of new organics coupled to aqueous mineral alteration. To address such issues we have applied the technique of microprobe two-step laser desorption / photoionization mass spectrometry (L2MS) to map in situ the spatial distribution of a broad range of organic species at the micron scale in the freshly exposed matrices of the Bells, Tagish Lake and Murchison (CM2) carbonaceous chondrites.

Clemett, S. J.↗

The Use of Silver Chloride Injection in Remediation of Iodine-129 by In Situ Capture as Silver Iodide at the F-Area Seepage Basin - 20225

The Savannah River Site (SRS) produced tritium, plutonium, and special nuclear materials for national defense, medicine, and the space programs. As part of operations, the F-Area Seepage Basins operated until 1988 for the disposition of deionized acidic wastewater from the F Separations Facility. The wastewater contained dilute nitric acid and low concentrations of non-radioactive metals, and radionuclides, with the major isotopes being Cs-137, Sr-90, U-235, U-238, Pu-239, Tc-99, I-129, and tritium. The seepage basins were closed in 1988 and backfilled and capped by 1991. The groundwater emanating from beneath the closed and capped seepage basins is acidic and contains elevated levels of both chemical and radiological contaminants. Releases from the groundwater plumes sourced from the F-Area Seepage Basins have impacted the water quality of Fourmile Branch, which is a small tributary to the Savannah River, a regional water source. A large pump-and-treat system was constructed in 1997 and operated until 2003 in an attempt to capture the releases to Fourmile Branch. The system in F Area and a similar system in H Area were expensive (∼$1.3 M/month) to operate and produced large quantities of radioactive waste, with concentrations of I- 129 too high to be disposed of at the SRS. In 2004, SRS replaced pump-and-treat with a funnel and gate system that along with operation of a base injection system at the gates reduces the flux of contaminants to the wetlands adjacent to Fourmile Branch. The alkaline solution injected into the aquifer neutralizes the acidic plume and immobilizes many of the cationic constituents. However, base injection is not effective in managing the release of iodine-129, an anionic contaminant. To address iodine-129 SRS and the Savannah River National Laboratory developed an in situ technology that uses ultra-fine ground silver chloride (AgCl) as an injectable capture medium for the sequestration of iodine-129. The AgCl amendment has a very small particle size and is designed to be injected into the contaminated aquifer to capture iodine-129. Dissolved iodine-129 forms a stable and highly insoluble solid (silver iodide) upon contact with AgCl. Laboratory studies, a field scale pilot test (2009), and three deployments (2011, 2015 and 2019) of AgCl have been successfully performed at the F-Area Seepage Basins. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Separating $${^{39}\hbox {Ar}}$$ from $${^{40}\hbox {Ar}}$$ by cryogenic distillation with Aria for dark-matter searches

Abstract Aria is a plant hosting a $${350}\,\hbox {m}$$ 350 m cryogenic isotopic distillation column, the tallest ever built, which is being installed in a mine shaft at Carbosulcis S.p.A., Nuraxi-Figus (SU), Italy. Aria is one of the pillars of the argon dark-matter search experimental program, lead by the Global Argon Dark Matter Collaboration. It was designed to reduce the isotopic abundance of $${^{39}\hbox {Ar}}$$ 39 Ar in argon extracted from underground sources, called Underground Argon (UAr), which is used for dark-matter searches. Indeed, $${^{39}\hbox {Ar}}$$ 39 Ar is a $$\beta $$ β -emitter of cosmogenic origin, whose activity poses background and pile-up concerns in the detectors. In this paper, we discuss the requirements, design, construction, tests, and projected performance of the plant for the isotopic cryogenic distillation of argon. We also present the successful results of the isotopic cryogenic distillation of nitrogen with a prototype plant.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Extraction of Pm-147 from savannah river site nuclear material management programs

The Savannah River Site (SRS) processes used-nuclear fuel to recover uranium. There are many interesting fission products lost in the raffinate from this separation including 147 Pm. Here, the goal of this work was to recover 147 Pm from SRS waste solutions. A radiochemical separation method typically used for the determination of 147 Pm and 151 Sm was modified to purify significant quantities of 147 Pm from the H Canyon waste solutions. The developed scheme was tested on a small aliquot of waste solution from the processing of used fuel from the High Flux Isotope Reactor at Oak Ridge National Laboratory.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Gross and Net Soil Methane Flux and Ancillary Data, Edgewater, MD, USA, summer 2022

This data package contains measurements used to quantify methane cycling and environmental conditions in coastal forest soils during the 2022 growing season. It includes time‑series data of soil methane flux, soil respiration, soil temperature, and volumetric water content collected from soil monoliths transplanted along an inundation and salinity gradient. The package also provides one‑time measurements from a stable‑isotope pool‑dilution incubation, including gravimetric water content, methane headspace concentrations, and ¹³CH₄ enrichment over time. Data files are provided in comma‑separated values (CSV) format, with accompanying metadata and readme documentation in PDF and plain‑text formats. All files can be opened with standard software such as R, Python, or spreadsheet programs capable of handling CSV files. The metadata file describes variable definitions, units, processing steps, and the structure of each data table to support reuse and integration with other datasets.

13-C↗

Mini-99 Experiment Design and Target Assembly

Qualification of nuclear fuels requires an understanding of a myriad of fuel performance variables, which requires time-consuming irradiations in test reactors. Accelerating burnup accumulation to reduce the irradiation time has historically been accomplished by increasing the 235 U enrichment in integral fuel tests, which inherently couples the fuel’s temperature and fission heat generation. Separate effects irradiation testing of nuclear fuel, using the MiniFuel target in the Oak Ridge National Laboratory’s (ORNL’s) High Flux Isotope Reactor (HFIR), offers an approach for decoupling fuel temperature and fission rate by reducing the quantity of the fuel and relying primarily on gamma heating in the surrounding components to drive fuel temperatures. However, if the fission rate is high enough, the fuel temperature will still vary over time as the fission heating changes, primarily due to poor heat conduction between the fuel and the surrounding components. This work details the design, analysis, and fabrication of a MiniFuel target which utilizes sodium bonding to improve the heat rejection from the fuel specimen, enabling the testing of higher 235 U enrichments (~8wt.%) to further accelerate burnup accumulation without prohibitively large temperature variations throughout the course of the irradiation.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Accretion and primary differentiation of Mars

In collecting samples from Mars to address questions such as whether Mars accreted homogeneously or heterogeneously, how Mars segregated into a metallic core and silicate mantle, and whether Mars outgassed catastrophically coincident with accretion or more serenely on a longer timescale, we must be guided by our experience in addressing these questions for the Earth, Moon, and igneous meteorite parent bodies. A key measurement to be made on any sample returned from Mars is its oxygen isotopic composition. A single measurement will suffice to bind the SNC meteorites to Mars or demonstrate that they cannot be samples of that planet. A positive identification of Mars as the SNC parent planet will permit all that has been learned from the SNC meteorites to be applied to Mars with confidence. A negative result will perhaps be more exciting in forcing us to look for another object that has been geologically active in the recent past. If the oxygen isotopic composition of Earth and Mars are established to be distinct, accretion theory must provide for different compositions for two planets now separated by only 0.5 AU.

Drake, Michael J.↗

Assimilation of solids during ascent of magmas from the Bartoy Field of the Baikal Region, Siberia

Most investigators ascribe mare basalt magma genesis to partial melting at depths of approximately 130 to greater than 400 km within the cumulate pile deposited from a lunar magma ocean. Mare basalts share with mid-ocean ridge basalts the characteristic of relative depletion in LREE and other incompatible trace elements that arises from melting within 'used' mantle, from which crust-forming elements have already been separated. Some mare basalt types do not show the classical, La-Nd depleted mare basalt REE distributions; however, some types are isotopically heterogeneous. These differences have been ascribed to assimilation, mainly AFC-style, of KREEPy highland material overlying the source region. Might such assimilation occur during magma ascent through the KREEPy material? To gain information from a terrestrial setting on possible assimilation during ascent, we have studied a suite of Quaternary nepheline-hawalites and nepheline-mugearites from the Bartoy cinder cone complex of the Baikal Rift, Siberia. The Bartoy magmas originated from greater than 80 km deep, and erupted through thick Archean crust. We find evidence for assimilation of approximately 31 wt. percent xenocrysts of garnet, aluminous clinopyroxene, kaersutite, and olivine, all presumably from the basalt source region, but no appreciable assimilation of overlying crust, consistent with isotopic constraints. Magmatic superheat made available by rapid ascent and decomposition accounts adequately for the energy of assimilation; no accompanying fractional crystallization is required or evident.

Haas, Johnson R.↗

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.↗

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↗

On-line technique for measuring stable oxygen and hydrogen isotopes from microliter quantities of water

Detailed here is a method for extracting and analyzing oxygen and hydrogen isotopes from 10 microL-sized water samples. Based on the traditional CO2-H2O equilibration technique, the oxygen isotope exchange reaction is done exclusively in sealed 6-mm (o.d.) Pyrex tubes at 25 degrees C, with full isotope exchange completed in at least 28 h. Using the same water sample employed in the 18O equilibration, D/H extractions are done in separate sealed 6-mm (o.d.) Pyrex tubes by reaction with Zn at 450 degrees C to form H2(g). Provided that a correction factor is applied to 18O analyses, accuracy and precision for both 18O and D/H are comparable to standard techniques using much larger samples.

NASA Center JSC↗