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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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All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

CO 2 electroreduction favors carbon isotope 12 C over 13 C and facilitates isotope separation

We discovered that CO 2 electroreduction strongly favors the conversion of the dominant isotope of carbon ( 12 C) and discriminates against the less abundant, stable carbon 13 C isotope. Both absorption of CO 2 in the alkaline electrolyte and CO 2 electrochemical reduction favor the lighter isotopologue. As a result, the stream of unreacted CO 2 leaving the electrolyzer has an increased 13 C content, and the depletion of 13 C in the product is several times greater than that of photosynthesis. Using a natural abundance feed, we demonstrate enriching of the 13 C fraction to ~1.3% (i.e., +18%) in a single-pass reactor and propose a scalable and economically attractive process to yield isotopes of a commercial purity. Our finding opens pathways to both cheaper and less energy-intensive production of stable isotopes ( 13 C, 15 N) essential to the healthcare and chemistry research, and to an economically viable, disruptive application of electrolysis technologies developed in the context of sustainability transition.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Neutron Coincidence Measurements of Uranium-233 Oxide

Renewed international interest in thorium-fueled advanced reactors has challenged the safeguards community to address future proliferation concerns. Thorium-based technology presents many benefits but does not eliminate the proliferation risks associated with producing and processing fissile material. A byproduct of thorium-fueled reactors is uranium-233, which is classified as a direct-use material. As a result, the development of new or improved methods to characterize and measure materials containing 233U must mirror the pace of development of reactors and facilities that produce such material. Research is underway to assess, develop, and test approaches for safeguarding nuclear materials within the thorium fuel cycle. Neutron signatures from the nondestructive assay (NDA) of materials containing 233U are being quantified to inform the potential characterization of these materials. Using a traditional neutron coincidence counter and a series of well-documented 233U oxide samples, initial measurements have been made to assess the feasibility of 233U characterization and discrimination from other uranium isotopes, primarily 235U, using a combination of measurement techniques and analysis methods. Data acquisition is performed in list mode, allowing for a variety of analyses to be performed on the raw data that is not available using traditional shift register technology. Measurements were performed in passive and active configurations to quantify the strength of signal and to validate simulations in support of this work. This paper presents and discusses the results of the initial measurements of 233U oxide performed at Oak Ridge National Laboratory.

Lockhart, Madeline↗
DOE OSTI2022

Low 13 C- 13 C abundances in abiotic ethane

Distinguishing biotic compounds from abiotic ones is important in resource geology, biogeochemistry, and the search for life in the universe. Stable isotopes have traditionally been used to discriminate the origins of organic materials, with particular focus on hydrocarbons. However, despite extensive efforts, unequivocal distinction of abiotic hydrocarbons remains challenging. Recent development of clumped-isotope analysis provides more robust information because it is independent of the stable isotopic composition of the starting material. Here, we report data from a 13 C- 13 C clumped-isotope analysis of ethane and demonstrate that the abiotically-synthesized ethane shows distinctively low 13 C- 13 C abundances compared to thermogenic ethane. A collision frequency model predicts the observed low 13 C- 13 C abundances (anti-clumping) in ethane produced from methyl radical recombination. In contrast, thermogenic ethane presumably exhibits near stochastic 13 C- 13 C distribution inherited from the biological precursor, which undergoes C-C bond cleavage/recombination during metabolism. Further, we find an exceptionally high 13 C- 13 C signature in ethane remaining after microbial oxidation. In summary, the approach distinguishes between thermogenic, microbially altered, and abiotic hydrocarbons. The 13 C- 13 C signature can provide an important step forward for discrimination of the origin of organic molecules on Earth and in extra-terrestrial environments.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1976

The isotopic composition of hydrogen and helium in low-energy cosmic rays

The isotopes H-2 and He-3 have been identified in low-energy cosmic rays during solar-quiet periods from 1973 January to 1974 October. These observations, made with the electron/isotope spectrometer on IMP-7, cover the energy intervals 5-29 MeV per nucleon for H-2 and 7-50 MeV per nucleon for He-3. The energy spectra of H-1, H-2, and He-3 fall rapidly with decreasing energy, giving H-2/H-1 and He-3/H-1 ratios which are essentially independent of energy as expected from current theories of the solar modulation of galactic cosmic rays. The measured He-4 spectrum, however, is essentially flat below 40 MeV per nucleon, suggesting that there may be contributions from a local, nonsolar source of He-4. Comparisons of the H-1, H-2, and He-3 observations with calculated spectra at 1 AU imply a mean interstellar path length of 7 plus or minus 2 g/sq cm. However, present low-energy measurements of H and He isotopes at 1 AU do not discriminate between possible cosmic-ray source spectra.

Mewaldt, R. A.↗
NASA NTRS1994

Acquisition and processing of data for isotope-ratio-monitoring mass spectrometry

Methods are described for continuous monitoring of signals required for precise analyses of 13C, 18O, and 15N in gas streams containing varying quantities of CO2 and N2. The quantitative resolution (i.e. maximum performance in the absence of random errors) of these methods is adequate for determination of isotope ratios with an uncertainty of one part in 10(5); the precision actually obtained is often better than one part in 10(4). This report describes data-processing operations including definition of beginning and ending points of chromatographic peaks and quantitation of background levels, allowance for effects of chromatographic separation of isotopically substituted species, integration of signals related to specific masses, correction for effects of mass discrimination, recognition of drifts in mass spectrometer performance, and calculation of isotopic delta values. Characteristics of a system allowing off-line revision of parameters used in data reduction are described and an algorithm for identification of background levels in complex chromatograms is outlined. Effects of imperfect chromatographic resolution are demonstrated and discussed and an approach to deconvolution of signals from coeluting substances described.

NASA Discipline Exobiology↗
DOE OSTI2022

Iron isotope evidence of an impact origin for main-group pallasites

Despite decades of work, the origin of pallasite meteorites has remained enigmatic. Long thought to be samples of the core-mantle boundary of differentiated asteroids, more recent studies have suggested a range of mechanisms for pallasite formation. These include olivine-metal mixing during a planetesimal collision and the intrusion of over-pressured core liquids into a planetesimal mantle. Establishing if the olivine and metal that comprise pallasites were once equilibrated at high temperature remains key to discriminating between these hypotheses. We determined the iron isotope compositions of olivine and metal in eleven main-group pallasites and found, in all cases, that olivine is isotopically lighter than metal. To interpret these data, we constrained the olivine-metal equilibrium Fe isotope fractionation with ab initio calculations and high temperature experiments. These independent approaches show that olivine preferentially incorporates the heavy isotopes of iron relative to metal. Our results demonstrate that pallasitic olivine and metal never achieved isotopic equilibrium with respect to iron. This precludes extended cooling at high temperature and is best reconciled with an impact origin for the main-group pallasites.

58 GEOSCIENCES↗
DOE OSTI2023

R “SHINY” GUI DEVELOPMENT FOR URANIUM ISOTOPIC ANALYSIS WITH MATRIX-ASSISTED IONIZATION MASS SPECTROMETRY

The international nuclear safeguards community continues to seek rapid, accurate, and precise characterization capabilities for the in-field measurement of uranium isotopic compositions in nuclear facilities. Mass spectrometry (MS) is considered the “gold standard” for analysis of relatively long-lived actinides such as uranium (U) and plutonium; however, conventional MS analysis often requires time consuming sample preparation and complex analytical methodologies that are difficult to perform in-field or in-facility. Matrix assisted ionization (MAI) is a novel ambient ionization MS technique (i.e., MAI-MS) that potentially addresses these challenges due to the relative simplicity of the ionization phenomenon and ruggedness of ambient MS instrumentation. Savannah River National Laboratory (SRNL, USA) has demonstrated this technique for nanogram-level 235U/238U isotope ratio measurements within seconds, with percent-level analytical uncertainties capable of discriminating depleted, natural, and low-enriched uranium. Current experimental work on developing MAI methods for uranium isotopic analysis has been enabled by parallel development of a comprehensive MAI-MS data analysis suite at SRNL. Development of this bespoke data analysis software was necessary because commercially available ambient MS software is poorly suited for uranium isotope ratio measurement. The effort leverages the power of R, a popular open-source programming language, and Shiny, an R package providing tools for graphical user interface (GUI) and web interface coding. This software allows researchers without any programming experience to harness and utilize R’s considerable data analysis/visualization power.

LaBone, Elizabeth D.↗
DOE OSTI2020

Design and construction of a new detector to measure ultra-low radioactive-isotope contamination of argon

Large liquid argon detectors offer one of the best avenues for the detection of galactic weakly interacting massive particles (WIMPs) via their scattering on atomic nuclei. The liquid argon target allows exquisite discrimination between nuclear and electron recoil signals via pulse-shape discrimination of the scintillation signals. Atmospheric argon (AAr), however, has a naturally occurring radioactive isotope, 39Ar, a ß emitter of cosmogenic origin. For large detectors, the atmospheric 39Ar activity poses pile-up concerns. The use of argon extracted from underground wells, deprived of 39Ar, is key to the physics potential of these experiments. The DarkSide-20k dark matter search experiment will operate a dual-phase time projection chamber with 50 tonnes of radio-pure underground argon (UAr), that was shown to be depleted of 39Ar with respect to AAr by a factor larger than 1400. Assessing the 39Ar content of the UAr during extraction is crucial for the success of DarkSide-20k, as well as for future experiments of the Global Argon Dark Matter Collaboration (GADMC). This will be carried out by the DArT in ArDM experiment, a small chamber made with extremely radio-pure materials that will be placed at the centre of the ArDM detector, in the Canfranc Underground Laboratory (LSC) in Spain. The ArDM LAr volume acts as an active veto for background radioactivity, mostly ?-rays from the ArDM detector materials and the surrounding rock. This article describes the DArT in ArDM project, including the chamber design and construction, and reviews the background required to achieve the expected performance of the detector.

Noble liquid detectors, Dark Matter detectors, Cry↗
DOE OSTI2025

The stable carbon isotope fractionation of methanogenesis products at complete carbon consumption

The stable carbon isotope signature (δ 13 C) of methane (CH 4 ) is used to discriminate between biological, thermogenic, and abiotic sources. Methanogens, or methane producing archaea, inhabit a broad range of chemical conditions. Many of these environments are replete in dissolved inorganic carbon (DIC), causing isotopically depleted δ 13 C biogenic CH 4 . However, some extreme environments inhabited by methanogens, such as serpentinising systems, exhibit low carbon dioxide (CO 2 ) availability, replete H 2 , and isotopically enriched δ 13 C CH 4 that is outside the known biogenic range. We measured the δ 13 C of CO 2 , biomass, lipids, and CH 4 during hydrogenotrophic methanogenesis under hydrogen replete conditions with a limited carbon pool to investigate carbon isotope dynamics at complete DIC consumption. As theory predicts, we found that the final, accumulated methane δ 13 C values closely reflect the δ 13 C of the initial DIC supply, and that methane is more 13 C enriched than biomass and lipids. This provides the first experimental evidence that methanogens can achieve complete carbon consumption and thus can produce accumulated CH 4 products that isotopically reflect the initial CO 2 . These data show that the range of possible δ 13 C values from biogenic methane needs to be expanded for natural environments impacted by extreme carbon limitation.

biomass↗
NASA NTRS1987

Isotopic characterisation of kerogen-like material in the Murchison carbonaceous chondrite

Data on isotopic composition of C, H, and N in insoluble organic fraction from the Murchison CM chondrite were used to discriminate between different theories for the origin of prebiotic organic material in the early solar system. Considerable isotopic variability was found among the samples and attributed to kerogen-like organic fraction. Three to four different isotopic components, two of them of polycyclic aromatic nature, were tentatively identified. Aliphatic moieties in the kerogen-like material, most of the polycyclic aromatic network, and extractable amino acids were found to carry a highly D-enriched component believed to have originated in an interstellar molecular cloud. A least part of the polycyclic aromatic fraction may also represent interstellar material.

Kerridge, John F.↗
NASA NTRS1992

Trapped xenon in ordinary chondrites

A trapped component of heavy noble gates representing a distinct solar system (presumably asteroid belt) reservoir is known to be concentrated in carbonaceous carriers of chondritic meteorites. The isotopic signature of trapped Xe in separates of the H4 chondrite Forest Vale (FV) was determined by combusting its carrier phases at 600 C in oxygen, discriminating against in situ produced nucleogenic components which are released above 600 C. The isotopic abundances of FV combustion-Xe (FVC-Xe) are compared to signatures of bulk trapped Xe in chondritic meteorites. We conclude that FVC-Xe represents the predominant trapped component in ordinary chondrites (OC) for which we adopt the term OC-Xe. Its isotopic signature differs from Xe in ureilites, in 'average carbonaceous chondrites', in earth's atmosphere, and in the solar wind. Additional minor Xe components were identified in type 3 chondrites and in the metal phase of chondrites. We discuss relationships among solar system Xe reservoirs and show that OC-Xe signature is consistent with a mixture of HL-Xe with slightly mass fractionated solar-type Xe.

Lavielle, Bernard↗
DOE OSTI2020

Analytical Determination of Radioactive Strontium and Cesium by Thermal Ionization Mass Spectrometry

Thermal ionization mass spectrometry (TIMS) has been evaluated for the detection of the radioactive isotopes of strontium and cesium. The instrument was investigated for the analysis of isotopic ratios of 89Sr to 90Sr and 135Cs to 137Cs in the presence of atomic isobars (Y and Zr for Sr analysis and Ba for Cs analysis). Signicant discrimination using TIMS was found for both Sr and Cs through evaluation using stable isotopes. Fusion procedures with different flux were evaluated for preparation of sample matrices. Chemical separations were developed and used after fusion to isolate the Sr and Cs from a prepared background matrix (i.e., Montana Soil). A graded approach, increasing in stable background isotopes, was performed to monitor the chemistry and instrument response. A thermal neutron irradiation was performed to produce a sample that contained the radioisotopes of Sr and Cs. Even though the irradiated sample was not a certified standard it does provide accurate expectation values via published, well understood cumulative fission yield data. The results presented in this work correlate extremely well with the published data. Furthermore, a significant decrease in uncertainty (by a factor of 5 { 10) was found for the isotopic ratios measured with TIMS compared to the published values.

TIMS, environmental contamination, radiostrontium,↗
DOE OSTI2021

Search for double-β decay of 76 Ge to excited states of 76 Se with the Majorana Demonstrator

The M AJORANA DEMONSTRATOR is a neutrinoless double-β decay search consisting of a low-background modular array of high-purity germanium detectors, ~2/3 of which are enriched to 88% in 76 Ge. The experiment is also searching for double-beta decay of 76 Ge to excited states (e.s.) in 76 Se. 76 Ge can decay into three daughter states of 76 Se, with clear event signatures consisting of a ββ-decay followed by the prompt emission of one or two γ rays. This results with high probability in multi-detector coincidences. In this work, the granularity of the DEMONSTRATOR detector array enables powerful discrimination of this event signature from backgrounds. Using 41.9 kg yr of isotopic exposure, the DEMONSTRATOR has set world leading limits for each e.s. decay of 76 Ge, with 90% CL lower half-life limits in the range of (0.75–4.0) × 10 24 yr. In particular, for the 2ν transition to the first 0 + e.s. of 76 Se, a lower half-life limit of 7.5 × 10 23 yr at 90% CL was achieved.

59 ≤ A ≤ 89↗
DOE OSTI2020

Results of the MAJORANA DEMONSTRATOR’s Search for Double-Beta Decay of 76 Ge to Excited States of 76 Se

The MAJORANA DEMONSTRATOR is searching for double-beta decay of 76 Ge to excited states (E.S.) in 76Se using a modular array of high purity Germanium detectors. 76 Ge can decay into three E.S.s of 76 Se. The E.S. decays have a clear event signature consisting of a ββ-decay with the prompt emission of one or two γ-rays, resulting in with high probability in a multi-site event. The granularity of the DEMONSTRATOR detector array enables powerful discrimination of this event signature from backgrounds. Using 21.3 kg-y of isotopic exposure, the DEMONSTRATOR has set world leading limits for each E.S. decay, with 90% CL lower half-life limits in the range of (0.56 – 2.1) • 10 24 y. In particular, for the 2v transition to the first 0 + E.S. of 76 Se, a lower half-life limit of 0.68 • 10 24 at 90% CL was achieved.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2026

Position-Specific Carbon Isotope Fingerprinting of Fluorinated Organics and Degradation Products

Fluorinated organic compounds are of growing environmental and forensic relevance due to their widespread use in pharmaceuticals, agrochemicals, and consumer products, their environmental persistence, and potential ecological and human health impacts. Elucidating their sources and transformation pathways is therefore a major focus of current research. Stable carbon isotope analysis provides a powerful approach for tracing molecular origins and linking parent compounds to degradation products. Recent isotope measurements have largely relied on mass-spectrometry techniques, which provide only an average isotope ratio across a compound. In this work, we employ a novel nuclear magnetic resonance (NMR) spectroscopy tool to determine position-specific carbon isotope ratios ( 13 C/ 12 C) in organofluorine compounds and their degradation products. This approach enables isotope measurements without combustion or extensive purification and, crucially, resolves ratios at individual carbon positions rather than bulk averages. The resulting intramolecular isotope fingerprints are unique to a molecule’s source. Applied to selected pharmaceuticals and pesticides, these fingerprints allow discrimination of chemically identical compounds. Moreover, we show that the 13 C/ 12 C signature at the fluorinated carbon persists through degradation, demonstrated for lansoprazole and fipronil. The 19 F NMR data produced for the 13 C/ 12 C analyses are also well suited for impurity profiling, providing an additional dimension for fingerprinting fluorinated organics. These findings suggest that position-specific isotope analysis can serve as part of a broader suite of tools for source characterization of organofluorine compounds and their breakdown derivatives, with potential applications in product validation, forensics, and linking these compounds to their breakdown products.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

A stilbene–strontium iodide based radioxenon detection system for monitoring nuclear explosions

Atmospheric measurement of noble gases has been extensively used for monitoring clandestine nuclear weapon explosions for many years. The ratios of four xenon isotopes of interest ( 131 mXe, 133 mXe, 133 Xe, and 135 Xe) help in discriminating regular reactor operations from nuclear tests. A new coincidence-based detection system using stilbene and strontium iodide [SrI 2 (Eu)] for electron and photon detection respectively was developed at Oregon State University to address some of the challenges of the radioxenon systems deployed in the field such as memory effect, and poor energy resolution. Silicon photomultipliers (SiPMs) were used for sensing optical photons from all scintillation media. Real-time coincidence identification was achieved using the eight-channel digital pulse processor. The detection system was evaluated using lab check sources and Oregon State TRIGA reactor irradiated radioxenon samples. A 48-hour background coincidence spectrum was collected yielding a coincidence count rate and background rejection rate of 0.0174 ± 0.0003 counts per second (cps) and 98.9% respectively. The minimum detectable concentration (MDC) of the system was evaluated to be 0.11 ± 0.01, 0.13 ± 0.02, 0.20 ± 0.02, and 0.73 ± 0.08 for 131 mXe, 133 mXe, 133 Xe, and 135 Xe respectively. The memory effect of the detection system was found to be 0.069 ± 0.015%, which is almost a 70-fold reduction compared to traditional plastic scintillators. Here, the detection elements, custom-designed electronics, and the detector response to radioxenon are detailed in this work.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2020

DUAL-PARTICLE DOSEMETER BASED ON ORGANIC SCINTILLATOR

Abstract Traditionally available handheld dosemeters are generally sensitive to only one type of radiation: neutrons or photons. Some dosemeters also rely on very specific attenuation correlations between response and dose, are not scalable in size and multiple dosemeters are required to characterise mixed-particle fields. The research presented here serves as a proof-of-concept for a method to simultaneously measure dose rates from neutrons and photons using a particle discriminating organic scintillation detector without the need for spectral deconvolution. The method was compared with traditional instruments and to simulation. Isotopic photon dose rates measured with this method were within 4% of simulated truth, whereas fission spectrum neutron dose rates were measured within 21%. Measurements of dose rates from both particles agree with simulated truth better than traditional instruments. This new method allows for measurement of dose equivalent from both neutrons and photons with a single instrument and no reliance on spectral deconvolution.

Miller, C. A.↗
DOE OSTI2025

Elemental and Isotopic Yields from T Coronae Borealis: Predictions and Uncertainties

T Coronae Borealis (T CrB) is a symbiotic recurrent nova system expected to undergo its next outburst within the next 2 yr. Recent hydrodynamic simulations have predicted the nucleosynthetic yields for both carbon–oxygen (CO) and oxygen–neon (ONe) white-dwarf models, but without accounting for thermonuclear reaction rate uncertainties. We perform detailed Monte Carlo postprocessing nucleosynthesis calculations based on updated thermonuclear reaction rates and uncertainties from the 2025 evaluation. We quantify the resulting abundance uncertainties and identify the key nuclear reactions that dominate them. Our results show that both the CO and ONe nova models robustly produce characteristic CNO isotopes. More pronounced abundance differences emerge for elements with A ≥ 20. Sulfur is the most robust observational discriminator between the CO and ONe nova models, with a model-to-model difference of a factor of ≈30 and minimal sensitivity to reaction rate uncertainties. Neon, silicon, and phosphorus exhibit even larger abundance differences (factors of ≈150–250), providing strong diagnostic potential. While their predicted yields are subject to larger uncertainties, these remain smaller than the model-to-model differences, allowing these elements to serve as useful, though less precise, tracers of white-dwarf composition. Chlorine, argon, and potassium also differ between models, but the 1σ-abundance ranges for the CO and ONe models overlap, reducing their present usefulness as composition tracers. We find that only nine nuclear reactions dominate the abundance uncertainties of the most diagnostically important isotopes, and their influence is largely independent of the underlying white-dwarf composition. These results provide guidance for future experimental efforts and for interpreting ejecta compositions in the next eruption of T CrB.

Chemical Abundances↗