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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

A new highly enriched 233 U reference material for improved simultaneous determination of uranium amount and isotope amount ratios in trace level samples

A highly-enriched 233 U reference material (>0.99987 n( 233 U)/n(U)) has been prepared and characterized for use as an isotope dilution mass spectrometry spike. An ion exchange separation was performed on 1 g of high purity 233 U to further reduce trace amounts of contaminant Pu in the material. The purified 233 U was then prepared as a master solution which was analyzed for molality of uranium by modified Davies and Gray titration. A portion of the master solution was quantitatively diluted and dispensed for reference material units. Selected units were analyzed for verification of uranium amount and to characterize uranium isotope amount ratios by multi-collector inductively couple plasma mass spectrometry. Furthermore, modelling of spike-corrected isotopic data show that the new spike will enable simultaneous measurements of uranium amount and isotope amount ratios with resulting uncertainties that are substantially less sensitive to over spiking than widely used 233 U certified reference materials.

233U↗
DOE OSTI2021

Certification of Uranium Isotope Amount Ratios in a Suite of Uranium Ore Concentrate Certified Reference Materials

Here, in this study, data from thirteen laboratories from around the world are presented for a successful certification of uranium isotope ratios in uranium ore concentrate (UOC) certified reference materials from the National Research Council Canada. Different mass spectrometric measurement principles (including SF-ICP-MS, quadruple ICP-MS, TIMS, MC-ICP-MS, SIMS and AMS) and measurement procedures were employed. In general, data from all sources exhibit good consistency with TIMS and MC-ICP-MS showing superior performance. The three candidate UOC CRMs (UCLO-1, UCHI-1 and UPER-1) have natural uranium isotope ratios with certified values of 0.5304(7) x 10 -4 , 0.5475(2) x 10 -4 and 0.5361(4) x 10 -4 for n( 234 U)/n( 238 U) and 0.007 2563(13), 0.007 2563(10) and 0.007 2542(11) for n( 235 U)/n( 238 U), respectively, with expanded uncertainty (k = 2) applicable to the last digit of the value given in the parentheses. Information values for n( 236 U)/n( 238 U) in these three CRMs, measured by AMS, are also provided: 10 x 10 -12 , 200 x 10 -12 and 22 x 10 -12 . The uncertainties of the proposed certified values of uranium isotope ratios in UOC CRMs are superior to available reference materials, and the values of n( 234 U)/n( 238 U) and n( 236 U)/n( 238 U) show significant variation among the three CRMs.

58 GEOSCIENCES↗
DOE OSTI2025

Plutonium isotope ratio measurements by total evaporation-thermal ionization mass spectrometry (TE-TIMS): an evaluation of uncertainties using traceable standards from the New Brunswick Laboratory

The accuracy and precision of isotope amount ratio measurements using thermal ionization mass spectrometry (TIMS) instrumentation are described, and the measurement of Pu materials is emphasized. The mass fractionation observed for Am, Ga, Pu, and U for isotope amount ratio measurements using the total evaporation (TE) technique is compared with theoretical estimates to demonstrate the advantage of the TE methodology and to investigate systematic biases in the major isotope amount ratios of U and Pu certified reference material (CRM) standards from the U.S. provider of CRMs. The quality of the Pu isotopic data generated by TIMS instruments in an analytical laboratory is demonstrated by the application of the double ratio technique to estimate the 241 Pu half-life. Analytical data on traceable Pu CRMs from the New Brunswick Laboratory (NBL), generated as part of routine measurements supporting various programs, are used for this half-life estimation. Although the 241 Pu abundances in CRMs of 136, 137, 138, and 126-A are approximately 200–2000× smaller than those in the 241 Pu material used in the previous Institute for Reference Materials and Measurements (IRMM) evaluation of the 241 Pu half-life, the half-life value estimated in this work shows excellent agreement with the currently accepted value from the IRMM. This agreement also demonstrates the pedigree of the Pu isotopic standards from the NBL and the quality of the isotope amount ratio measurements using TIMS instrumentation. For both the major and minor Pu isotope amount ratios, this report describes the relative importance of the factors affecting the uncertainty of TIMS measurements, which are considered the gold standard in isotope ratio measurements (LA-UR-24-29199).

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2025

A new HALEU isotopic certified reference material

Candidate certified reference material (CRM) U196 was prepared by gravimetrically mixing and dissolving NNSA NRMP CRM 112-A (natural uranium metal) and CRM 116-A (highly enriched 93.2% 235 U metal) to achieve a high-assay low-enriched uranium (HALEU) isotopic abundance reference material. CRM U196 will be certified for the 233 U/ 238 U, 234 U/ 238 U, 235 U/ 238 U, and 236 U/ 238 U ratios. Gravimetrically determined uranium isotope amount ratios and values derived from the isotope data were calculated from the buoyancy corrected mass data and from certified values for the metal CRMs used to create the solution. The 235 U isotope amount fraction (·100) and expanded uncertainty is 19.5846 ± 0.0028. For attribute verification, total evaporation and modified total evaporation isotope ratio measurements were performed. In conclusion, the reference material is to be distributed as a unit containing 5 mg uranium as dry uranyl nitrate.

High-assay low-enriched uranium↗
DOE OSTI2021

New reference materials for trace-levels of actinide elements in plutonium

In this report two plutonium oxides were prepared as unique reference materials for measurement of actinide elements present as trace constituents. Each reference material unit is approximately 200 mg of PuO 2 powder in a quartz glass bottle. Characterized attributes of the oxides included mass fractions of plutonium, americium, neptunium, and uranium. Isotope-amount ratios were also determined for plutonium and uranium, but neptunium and americium were observed to be monoisotopic 237 Np and 241 Am. Measurements for characterization and verification of the attributes show that plutonium and trace actinides are homogeneous with the exception of limited heterogeneity for uranium, primarily observed for the 238 U isotope. Model purification ages calculated from measured americium and uranium attribute values are consistent with material histories and indicate that these impurities are predominantly due to the decay of plutonium isotopes.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2025

Bayesian Statistical Analysis for Mass Spectrometric Data Processing

• Thermal ionization mass spectrometry (TIMS) is a “gold standard’ technique for actinide isotope amount ratio and assay measurements. • Ubiquitously used in: • Nuclear Nonproliferation • Nuclear Safeguards • Nuclear Forensics • Basic Science • Savannah River National Laboratory (SRNL) installed a new Thermo Scientific TRITON Plus TIMS in early 2024.

McLarty, Ellis C. [Savannah River National Laborat↗
DOE OSTI2025

Bayesian Statistical Analysis for Mass Spectrometric Data Processing

Thermal ionization mass spectrometry (TIMS) is a “gold standard’ technique for actinide isotope amount ratio and assay measurements. • Ubiquitously used in: • Nuclear Nonproliferation • Nuclear Safeguards • Nuclear Forensics • Basic Science • Savannah River National Laboratory (SRNL) installed a new Thermo Scientific TRITON Plus TIMS in early 2024.

McLarty, Ellis C. [Savannah River National Laborat↗
DOE OSTI2022

The NEON Daily Isotopic Composition of Environmental Exchanges Dataset

The National Ecological Observatory Network (NEON) provides open-access measurements of stable isotope ratios in atmospheric water vapor (δ 2 H, δ 18 O) and carbon dioxide (δ 13 C) at different tower heights, as well as aggregated biweekly precipitation samples (δ 2 H, δ 18 O) across the United States. These measurements were used to create the NEON Daily Isotopic Composition of Environmental Exchanges (NEON-DICEE) dataset estimating precipitation (P; δ 2 H, δ 18 O), evapotranspiration (ET; δ 2 H, δ 18 O), and net ecosystem exchange (NEE; δ 13 C) isotope ratios. Statistically downscaled precipitation datasets were generated to be consistent with the estimated covariance between isotope ratios and precipitation amounts at daily time scales. Isotope ratios in ET and NEE fluxes were estimated using a mixing-model approach with calibrated NEON tower measurements. NEON-DICEE is publicly available on HydroShare and can be reproduced or modified to fit user specific applications or include additional NEON data records as they become available. The NEON-DICEE dataset can facilitate understanding of terrestrial ecosystem processes through their incorporation into environmental investigations that require daily δ 2 H, δ 18 O, and δ 13 C flux data.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

BIRDIE beryllium-10 and -7 measurements from 2022 summer deep convection rain at ARM SGP

Water samples were manually collected from 11 SGP ARM sites in the early summer of 2022 to measure cosmogenic isotopes of beryllium. The water samples were brought back to the Center for Accelerator Mass Spectrometry (CAMS) at LLNL and analysed for beryllium-10 and beryllium-7 as well as for chlorine-37, chlorine-36, and tritium. A total of six storm events were measured over three weeks. At least five of those storms included overshooting cloud events. Available data include precipitation amount, beryllium-10 concentration, beryllium-7 concentration, and 10/7Be ratio. Spatial and temporal variability in the cosmogenic isotopes was relatively high but could not directly be linked to precipitation amount. Analysis is on-going to explain the measured variability and to see if it can be linked to cloud top height and overshooting depth.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS1986

Spectroscopic observations of the planets

The first phase of a program to determine D/H in the atmospheres of all of the major planets and Titan was completed. D/H on Titan and Uranus is significantly higher than on Jupiter and Saturn. Titan has the highest value, consistent with the possibility for hydrogen escape. These measurements were all made in terms of CH3D/CH4. They suggest that at least two reservoirs for deuterium exist in the outer solar system - a large one in hydrogen and a much smaller one in hydrogen-containing compounds that have not isotopically equilibrated with the hydrogen. This result also demonstrates that a large fraction of the carbon in the outer solar nebula was in the form of methane and it supports the nucleation model for the formation of the outer planets. Other studies included an investigation of the phosphine abundance over the Great Red Spot (GRS) of Jupiter, pre-Voyager determination of the amount of acetylene on Uranus, and the carbon isotope ratio in Halley's Comet. UV spectra of the GRS obtained with the IUE show no evidence of the enhancement of phosphine that would be expected if the red color of this object is caused by P4.

Owen, T.↗
DOE OSTI2022

RAPID UNSEPARATED RARE EARTH ELEMENT ANALYSES BY ISOTOPE DILUTION MULTICOLLECTOR INDUCTIVELY COUPLED MASS SPECTROMETRY (ID-MC-ICP-MS)

We present a method for analyzing rare earth elements (REEs) by isotope dilution without separation of individual elements. Utilizing a Nu Plasma 2 multicollector inductively coupled plasma mass spectrometer (MC-ICP-MS) equipped with an Aridus II desolvation nebulizer, sample introduction tuning parameters (torch position, gas flows) were investigated and used to minimize oxide formation (e.g., NdO/Nd <0.05%) and remove the need to analyze the REEs as separated “cuts.” Ratios for spike/sample isotopes in mixed synthetic standards containing varying amounts of Ce, Nd, Sm, Eu, Gd, Dy, Er, and Yb were measured accurately within 1% of IUPAC values. La and Lu in the standards were more than 2% off from expected values due to more demanding interference corrections. A USGS BCR-2 rock standard was also processed with flux fusion, iron coprecipitation and a single column pass bulk separation followed by analysis. The concentrations for Ce, Nd, Sm, Eu, Dy, Er, and Yb fell within 2% of consensus values. A United States Geological Survey (USGS) BIR-1A rock standard was also processed in triplicate by hydrofluoric and nitric acid digestion, yielding rare earth concentrations within 3% of consensus values with 0.3% relative standard deviation (n=3). This demonstrates the ability to produce high quality REE patterns of comparable quality to traditional methods involving labor and time intensive REE separation, with sample preparation and analytical times that are comparable to analyses against isotope dilution by single-collector ICP-MS.

Shen, Steve D.↗
NASA NTRS2012

Compound-Specific Isotopic Analysis of Meteoritic Amino Acids as a Tool for Evaluating Potential Formation Pathways

Measurements of stable hydrogen, carbon, and nitrogen isotopic ratios (delta D, delta C-13, delta N-15) of organic compounds can reveal information about their origin and formation pathways. Several formation mechanisms and environments have been postulated for the amino acids detected in carbonaceous chondrites. As each proposed mechanism utilizes different precursor molecules, the isotopic signatures of the resulting amino acids may point towards the most likely of these proposed pathways. The technique of gas chromatography coupled with mass spectrometry and isotope ratio mass spectrometry provides compound-specific structural and isotopic information from a single splitless injection, enhancing the amount of information gained from small amounts of precious samples such as carbonaceous chondrites. We have applied this technique to measure the compound-specific C, N, and H isotopic ratios of amino acids from seven CM and CR carbonaceous chondrites. We are using these measurements to evaluate predictions of expected isotopic enrichments from potential formation pathways and environments, leading to a better understanding of the origin of these compounds.

Elsila, Jamie E.↗
NASA NTRS1992

Past and present water budget of Venus

Attention is given to a detailed analysis of Pioneer Venus large-probe neutral mass spectrometer data which confirm an earlier report that the abundance of Venus deuterium relative to hydrogen is two orders of magnitude larger than that of terrestrial deuterium. The D/H ratio in the bulk atmosphere of Venus today is found to be between 0.014 and 0.02. The argument that present-day HDO can be in a steady state with exogenous (cometary) sources is based on an underestimate of the hydrogen abundance and an overestimate of current escape rates. The large isotope ratio requires that Venus once had above-surface water amounting to at least a few tenths of a percent of a terrestrial ocean and has since lost almost all of the associated hydrogen.

Donahue, T. M.↗
DOE OSTI2021

Measurement of the 230 Th( p ,2n)Pa229 and 230 Th( p ,3n)Pa228 reaction cross sections from 14.1 to 16.9 MeV

Actinium-225 is of interest for medical isotope production and there is on-going research into methods of producing Ac 225 , either directly or via the decay of its parent isotopes ( Th 229 , Pa 229 , and Ra 225 ). One method that has been suggested is the Th 230 ( p , 2 n ) Pa 229 reaction. However, there is no available cross-section data for this reaction in the literature. Purpose: Measure the Th 230 ( p , 2 n ) and Th 230 ( p , 3 n ) reaction cross sections in the energy range where the ( p , 2 n ) reaction is predicted to peak to determine the feasibility of Ac 225 production via the Th 230 ( p , 2 n ) reaction. Methods: Targets naturally enriched in Th 230 were irradiated at the Center for Accelerator Mass Spectrometry at Lawrence Livermore National Laboratory with energies ranging from 14.1 to 16.9 MeV. Furthermore, chemical processing was used to separate the protactinium activation products, followed by γ -ray spectroscopy to measure the activities of Pa 228 , 229 , 230 , 232 produced in the irradiation. Results: We find that excitation functions are reported for the first time in the literature for the Th 230 ( p , 2 n ) and Th 230 ( p , 3 n ) reactions in this energy range. The peak measured value of the Th 230 ( p , 2 n ) reaction was found to be 182 ± 12 mb at 14.4 ± 0.1 MeV. The Th 232 ( p , n ) Pa 232 reaction was used to verify the experimental conditions, the measured values are reported and are comparable to the existing literature values. From the γ -ray spectrometry data, the half-life of Pa 229 was measured as 1.5 ± 0.1 days, which is within the error of the half-life reported in the evaluated nuclear data as well as in the recent measurements, and the half-life of Pa 228 was measured as 19.5 ± 0.4 hours. Conclusions: Overall, the Th 230 ( p , 2 n ) Pa 229 reaction could reasonably be used for Ac 225 isotope production, although significant amounts of relatively isotopically pure Th 230 would be needed for significant production because the low alpha-decay branching ratio of Pa 229 and long half-life of Th 229 inhibit the in-growth of significant amounts of Ac 225 .

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
NASA NTRS2009

Ethane's 12C/13C Ratio in Titan: Implications for Methane Replenishment

As the .main destination of carbon in the destruction of methane in the atmosphere of Titan, ethane provides information about the carbon isotopic composition of the reservoir from which methane is replenished. If the amount of methane entering the atmosphere is presently equal to the amount converted to ethane, the 12C/13C ratio in ethane should be close to the ratio in the reservoir. We have measured the 12C/13C ratio in ethane both with Cassini CIRS(exp 1) and from the ground and find that it is very close to the telluric standard and outer planet values (89), consistent with a primordial origin for the methane reservoir. The lower 12C/13C ratio measured for methane by Huygens GCMS (82.3) can be explained if the conversion of CH4 to CH3 (and C2H6) favors 12C over 13C with a carbon kinetic isotope effect of 1.08. The time required for the atmospheric methane to reach equilibrium, i.e., for replenishment to equal destruction, is approximately 5 methane atmospheric lifetimes.

Jennings, Donald E.↗
DOE OSTI2023

Plutonium Signatures in Molten-Salt Reactor Off-Gas Tank and Safeguards Considerations

Fluid-fueled molten-salt reactors (MSRs) are actively being developed by several companies, with plans to deploy them internationally. The current IAEA inspection tools are largely incompatible with the unique design features of liquid fuel MSRs (e.g., the complex fuel chemistry, circulating fuel inventory, bulk accountancy, and high radiation environment). For these reasons, safeguards for MSRs are seen as challenging and require the development of new techniques. This paper proposes one such technique through the observation of the reactor’s off-gas. Any reactor design using low-enriched uranium will build up plutonium as the fuel undergoes burnup. Plutonium has different fission product yields than uranium. Therefore, a shift in fission product production is expected with fuel evolution. The passive removal of certain gaseous fission products to the off-gas tank of an MSR provides a valuable opportunity for analysis without significant modifications to the design of the system. Uniquely, due to the gaseous nature of the isotopes, beta particle emissions are available for observation. The ratios of these fission product isotopes can, thus, be traced back to the relative amount and types of fissile isotopes in the core. This proposed technique represents an effective safeguards tool for bulk accountancy which, while avoiding being onerous, could be used in concert with other techniques to meet the IAEA’s timeliness goals for the detection of a diversion.

Dunkle, Nicholas (ORCID:000000027323011X)↗
DOE OSTI2025

Demonstration of a Novel Radiochemical Mix Diagnostic for Fusion Implosions at the National Ignition Facility

Mixing of the ablator material into the fuel of an inertial confinement fusion implosion reduces compression and enhances radiative losses, preventing ignition. Here, we describe a novel use of charged-particle radiochemistry to measure the ablator mix in contact with the fusion hot spot. The capsule uses a graded Be-Cr layer to increase the confinement of the hot spot. 52 Mn and 51 Cr isotopes are collected from the implosion and counted, and the ratio is related to the amount of Cr mixed into the hot spot. Thus, a new diagnostic to determine the degradation due to mix on fusion implosions has been developed.

MacLaren, S. A. [Lawrence Livermore National Labor↗
NASA NTRS1976

Earth tides, volcanos and climatic change

The effect of variations in tidal stresses on the earth caused by the sun and moon on volcanic activity and climate is investigated. A statistically significant correlation is found between the derivatives of the envelopes of peak tidal stresses at high northern latitudes and the mean temperature of the Northern Hemisphere as reflected in oxygen isotope ratios in the Greenland ice cap. It is suggested that variations in tidal stresses cause changes in the amount of stratospheric dust produced by volcanic activity, which affects the thickness of the stratospheric dust veil and the atmospheric radiation balance. For a simple model, periodic variations in tidal stress account for 13% of the variance in the ice-core temperature record.

Roosen, R. G.↗