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At least 73 records · Page 4
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Chemical abrasion: the mechanics of zircon dissolution

Chemical abrasion is a technique that combines thermal annealing and partial dissolution in hydrofluoric acid (HF) to selectively remove radiation-damaged portions of zircon crystals prior to U–Pb isotopic analysis, and it is applied ubiquitously to zircon prior to U–Pb isotope dilution thermal ionization mass spectrometry (ID-TIMS). The mechanics of zircon dissolution in HF and the impact of different leaching conditions on the zircon structure, however, are poorly resolved. We present a microstructural investigation that integrates microscale X-ray computed tomography (µCT), scanning electron microscopy, and Raman spectroscopy to evaluate zircon dissolution in HF. We show that µCT is an effective tool for imaging metamictization and complex dissolution networks in three dimensions. Acid frequently reaches crystal interiors via fractures spatially associated with radiation damage zoning and inclusions to dissolve soluble high-U zones, some inclusions, and material around fractures, leaving behind a more crystalline zircon residue. Other acid paths to crystal cores include the dissolution of surface-reaching inclusions and the percolation of acid across zones with high defect densities. In highly crystalline samples dissolution is crystallographically controlled with dissolution proceeding almost exclusively along the c axis. Increasing the leaching temperature from 180 to 210 °C results in deeper etching textures, wider acid paths, more complex internal dissolution networks, and greater volume losses. How a grain dissolves strongly depends on its initial radiation damage content and defect distribution as well as the size and position of inclusions. As such, the effectiveness of any chemical abrasion protocol for ID-TIMS U–Pb geochronology is likely sample-dependent. We also briefly discuss the implications of our findings for deep-time (U-Th)/He thermochronology.

58 GEOSCIENCES↗
DOE OSTI2024

$\overline{TKE}$ Parameterization and $\bar{v}$ Uncertainty Analysis for CGMF

Previous work was performed on tuning CGMF parameters for 235 U, 238 U, and Plutonium isotopes. Now work is being done to tune minor uranium isotopes. However, uranium isotopes like 232 U and 236 U have almost no experimental data. We are applying cross-isotope models to extrapolate and tune CGMF on isotopes that lack experimental data. There exist several internal CGMF physics quantities that affect the output of CGMF—multi-chance fission probability, excitation energy sharing, spin-cutoff factor, spin scaling, and fragment total kinetic energy to name a few. The mean fragment total kinetic energy, $\overline{TKE}$, is particularly interesting because of its strong anti-correlation with $\bar{v}$. We are most interested in the mean fragment total kinetic energy before neutron emissions. $\overline{TKE}$ is assumed to be pre-neutron emission unless otherwise stated. Currently in CGMF, the $\overline{TKE}$ model for 233,234,235,238 U are tuned independently to reproduce ν for the associated isotopes. In this report, we will tune a cross-isotope $\overline{TKE}$ model to experimental $\overline{TKE}$ data for 232,233,234,235,236,238 U. Because of the unreliable and sparse nature of $\overline{TKE}$ experimental data, future work will use more reliable experimental $\bar{v}$ data to infer the $\overline{TKE}$ model (and likely other internal CGMF parameters) for uranium isotopes. Such work has been performed previously using a sensitivity analysis and Kalman filter methods.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2021

Enhancing isotope mixing in U-10Mo downblend castings with electromagnetic stirring

Uranium alloyed with 10 wt percent molybdenum (U-10Mo) is the proposed fuel for use in the United States’ high-performance research reactors. The U-10Mo fuel is fabricated by a two-step casting process that downblends highly enriched uranium with depleted uranium (DU) and/or natural uranium (NU) and subsequently alloys the resulting high-assay low-enriched uranium (HALEU) with Mo. Currently, a two-step casting process is needed to meet the ingots’ U-235 enrichment homogeneity specifications. This work demonstrates the ability to provide more homogeneous U-235 distributions during downblend casting by using zirconia for crucibles rather than graphite. When graphite is used as a crucible, the electromagnetic field produced by the induction heater couples directly with the graphite. Zirconia is nonconducting in this study, and therefore does not couple with the field. The induction field couples directly with the metal, and causes electromagnetic stirring (EMS) in the molten metal pool. Eight downblend casting experiments were carried out in this work. Four were performed with zirconia crucibles and four with graphite crucibles. The U-235 enrichment was measured at nine discrete points in each casting using laser ablation multi-collector inductively coupled mass spectrometry (LA-MC-ICP-MS). The enrichment homogeneity was approximately eight times better in zirconia crucible castings than in graphite crucible castings as measured by the plate enrichment range and enrichment coefficient of variation. The results show a single casting step could be used to meet USHPRR enrichment specifications if electromagnetic stirring is present during casting. A related investigation was carried out to determine whether it is appropriate to measure enrichment on as-cast ingots or whether heat treated specimens should be used to accurately characterize enrichment. The results show that the as-cast microstructure plays a significant role in enrichment homogeneity. It is recommended that all enrichment measurements be done after the homogenization heat treatment typical of U-10Mo processing.

36 MATERIALS SCIENCE↗
NASA NTRS2006

Concordant Rb-Sr and Sm-Nd Ages for NWA 1460: A 340 Ma Old Basaltic Shergottite Related to Lherzolitic Shergottites

Preliminary Rb-Sr and Sm-Nd ages reported by [1] for the NWA 1460 basaltic shergottite are refined to 336+/-14 Ma and 345+/-21 Ma, respectively. These concordant ages are interpreted as dating a lava flow on the Martian surface. The initial Sr and Nd isotopic compositions of NWA 1460 suggest it is an earlier melting product of a Martian mantle source region similar to those of the lherzolitic shergottites and basaltic shergottite EETA79001, lithology B. We also examine the suggestion that generally "young" ages for other Martian meteorites should be reinterpreted in light of Pb-207/Pb-206 - Pb-204/Pb-206 isotopic systematics [2]. Published U-Pb isotopic data for nakhlites are consistent with ages of approx.1.36 Ga. The UPb isotopic systematics of some Martian shergottites and lherzolites that have been suggested to be approx.4 Ga old [2] are complex. We nevertheless suggest the data are consistent with crystallization ages of approx.173 Ma when variations in the composition of in situ initial Pb as well as extraneous Pb components are considered.

Nyquist, L. E.↗
DOE OSTI2025

Diversion Path Analysis: A Proposed Methodology to Develop an MC&A Approach for Liquid-Fueled Molten Salt Reactors

Nuclear material control and accounting (MC&A) is a critical element of both the US Nuclear Regulatory Commission (NRC) and US Department of Energy (DOE)’s domestic safeguards and security requirements. NRC licensees are required, under Title 10 of the Code of Federal Regulations (10 CFR) Part 74 to establish and maintain an MC&A program that captures and records the quantities and locations of special nuclear material (SNM) at the facility. Along with physical protection, MC&A is a key element of domestic nuclear material safeguards that enables the NRC to ensure that SNM is controlled and accounted for. SNM, per 10 CFR Part 74, refers to plutonium, 233 U, and uranium enriched in the isotope 233 U or 235 U, but does not include source material. Periodic physical inventories, coupled with material balance evaluations, are effective and demonstrated tools to account for and detect theft or diversion of SNM in facilities containing SNM in bulk material form (i.e., not in discrete, countable items). Historically in the United States, these types of facilities have included fuel fabrication, conversion, and enrichment facilities. In comparison, reactors have relied on item counting of assemblies and control of SNM while in containment (e.g., a sealed reactor pressure vessel) because, to date, reactor fuel has been in item form. In liquid-fueled molten salt reactors (MSRs), unlike traditional light water reactors (LWRs) or bulk facilities, bulk SNM quantities can change significantly during operation as a result of depletion and transmutation. This introduces challenges to the use of traditional periodic physical inventories and material balance evaluations to detect theft or diversion of SNM in reactors that use SNM in bulk material form. Liquid-fueled (i.e., salt-fueled) MSR facilities are MSRs that use SNM within a salt eutectic as the fuel. The SNM is in a bulk material form any time it is outside of fresh or spent fuel storage containers. Some examples of when SNM will be in bulk form in the facility are during addition of fuel to the reactor system, while fuel is circulating in operation, and while fuel is in a drain tank. Periodic physical inventories and material balance evaluations can likely be effectively applied to many portions of an MSR facility, including all areas where depletion and transmutation are not significantly changing the quantities of SNM within the control area. Within an MSR facility, this would include fresh fuel receipt and loading, waste streams that may contain SNM, irradiated fuel storage outside of the reactor core, and any irradiated fuel processing that may happen after SNM has been removed from the reactor. All of these process steps could rely on measurements of SNM quantities compared with documented inventories. Any discrepancies from predicted (i.e., book) inventories and measured inventories could be quantified as inventory differences, consistent with traditional MC&A guidance from the NRC (e.g., in NUREG-1065 Revision 2, NUREG-2159 Revision 1, and RG 5.29 Revision 2). Within the reactor system, additions and removals to the book inventory include depletion of the SNM (e.g., fission of 235 U), which complicates the use of physical inventories. SNM control, however, can also likely be effectively applied to detect theft of SNM throughout a liquid-fueled MSR facility. To complement these approaches, prior technical reports have identified that a diversion path analysis may be a useful, risk-informed, and performance-based tool to determine suitable elements of an MC&A approach for the reactor system within a liquid-fueled MSR facility.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2022

The need for speed – Burnup determination of spent nuclear fuel

Here we present the application of a novel analytical approach for high-speed evaluation of burn-up in spent nuclear fuel. This automated online separation–direct analysis method, which simultaneously measures the isotopic compositions and concentrations of Nd, Pu, and U using isotope dilution-inductively coupled plasma mass spectrometry, enables the determination of burnup in as little as 4.5 h per sample with expanded uncertainties as low as 1.2% using as little as 1µg of fuel. We compare the determined burn-up values, sample requirements, and analysis times with an ultra-high precision, in-house developed, methodology which employs multiple analytical techniques to measure the isotopic compositions and concentrations of Nd, Pu, and U yielding burn-up values with expanded uncertainties as low as 0.49% at the 95% confidence level, the lowest reported to date.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2022

U–Pb Geochronology and Stable Isotope Geochemistry of Terrestrial Carbonates, Lower Cretaceous Cedar Mountain Formation, Utah: Implications for Synchronicity of Terrestrial and Marine Carbon Isotope Excursions

The terrestrial Lower Cretaceous Cedar Mountain Formation, Utah, is a critical archive of paleoclimate, tectonics, and vertebrate ecology and evolution. Early Cretaceous carbon cycle perturbations associated with ocean anoxia have been interpreted from this succession, as expressed in stable carbon isotopes. However, refining the timing of the observed stable isotope excursions remains a key challenge in understanding how marine anoxia affects the Earth system, and is ultimately recorded in the terrestrial realm. The geochronology and geochemistry of a terrestrial carbonate near the base of this succession, which potentially records the Ap7 global carbon isotope excursion, is studied here. Petrographic and geochemical analyses are used to test plausible mechanisms for U incorporation into the calcite lattice in this sample. Using these methods, the hypothesis that the incorporation of U was at or close to the timing of carbonate precipitation is evaluated. U–Pb geochronology of calcite indicates a plausible Early Cretaceous age. However, comparison of the new U–Pb ages of calcite with detrital zircon maximum depositional ages immediately beneath the studied sample indicates a disparity in the apparent sedimentation rates if both types of geochronologic information are interpreted as reflecting the timing of sediment deposition. The totality of data supports an early, and high-temperature, diagenetic timing of U incorporation, with potential for minor leaching of U in subsequent fluid–rock interaction. The most likely mechanism for U transport and immobilization in these samples is hydrothermal fluid–rock interaction. Therefore, the radiometric ages, and corresponding stable isotope composition of U-bearing carbonate domains in this sample, indicate early subsurface fluid–rock interactions and not a record of atmosphere–soil geochemical reactions.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Analysis of FRAM Measurements to Establish Methodology Uncertainty

Qualification measurements were performed at Oak Ridge National Laboratory (ORNL) on a variety of measurement standards. These measurements will be used to qualify the Fixed-Energy, Response Function Analysis with Multiple Efficiency (FRAM) code with a high purity germanium (HPGe) detector for use at ORNL. Measured items include uranium isotopic standards, U 3 O 8 line sources, and a uranium tetrafluoride source. The 235 U enrichment was estimated using the FRAM isotopic analysis software for each source and compared with the declared isotopic values.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
NASA NTRS2019

Mechanisms and Consequences of Intra-Crystalline Enrichment of Ancient Radiogenic Pb in Detrital Hadean Zircons from the Jack Hills, Western Australia

The recent discovery of Pb* (radiogenic lead) -enriched domains (PEDs) in zircon using high-resolution scanning ion imaging, atom probe tomography and transmission electron microscopy indicates that the U-Pb isotopic system in zircon can be affected not only by Pb* loss but also by intra-crystalline Pb* enrichment. However, the formation mechanism of PEDs and the consequences for in-situ U-Pb dating remain elusive. To further understand these issues, scanning ion imaging and U-Pb dating were carried out on 51 Hadean detrital zircon grains from the Jack Hills, Western Australia. Of these, 8 grains were found to contain micrometer-scale PEDs with elevated Pb-207 and Pb-206 in the ion images. Isotope profiles across these PEDs confirm that they represent unsupported Pb* resulting from intra-grain mobilization and local enrichment of Pb* during ancient overprinting events. The PEDs are rare in most grains, with only 1 – 3 Pb* hotspots present in any ~70 μm × 70 μm imaged area, and are located either in dark-CL, high-U growth zones, or associated with bright-CL, low-Th recrystallized domains, suggesting that they were likely formed by local-scale processes. The PEDs located in dark-CL, high-U growth zones likely resulted from Pb* trapped in local, interconnected pathways produced by radiation damage during thermal overprinting events. Those associated with bright-CL, low-Th domains are interpreted as Pb* concentrated in nanoscale pores formed during fluid-present recrystallization of non-metamict zircon. Our interpretations therefore imply that intra-crystalline enrichment of Pb* in zircon can occur at various scales and through diverse mechanisms. Age calculations based on the ion images demonstrate that incorporation of PEDs in conventional in-situ SIMS spots produces spuriously old ages that are either reversely discordant or concordant, depending on the time of Pb* mobilization and the analytical precision. The implication is that careful investigation of intra-grain distribution of U-Th-Pb isotopes is required in order to better understand the U-Pb isotopic system and to obtain reliable crystallization ages for ancient zircons affected by complex Pb* mobilization and redistribution.

Unsupported radiogenic lead↗
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 OSTI2020

Influence of physical and chemical hydrology on bioremediation of a U-contaminated aquifer informed by reactive transport modeling incorporating 238 U/ 235 U ratios

Microbially-catalyzed reductive immobilization of aqueous uranium (U) as a solid phase has been proposed as a U remediation technique. Both laboratory and field experiments have demonstrated that this reduction reaction alters the 238 U/ 235 U ratio, producing a 238 U-enriched U(IV) solid. In contrast, other major U reactive transport processes fractionate these isotopes much less. This suggests the potential to quantify the extent of bioreduction occurring in groundwater containing U using the 238 U/ 235 U ratio, which would substantially improve upon current practices largely relying on U concentration measurements alone. Current reactive transport models for uranium dynamics include only concentration measurements, which are strongly influenced by highly coupled reactive transformation and aqueous transport processes. The complex physical and chemical behavior of U potentially compromises such quantitative analysis of U storage and release. Here we report the first numerical reactive transport model which explicitly incorporates variations in the 238 U/ 235 U ratio of U and demonstrates improved interpretation of the principal chemical reactions and groundwater transport processes affecting the subsurface mobility and distribution of this widespread contaminant. Recent U bioreduction studies performed in a contaminated aquifer in Rifle, Colorado, USA applied Rayleigh distillation models to interpret U stable isotope fractionation observed as a result of acetate amendment. These simplified models were unable to resolve the spatiotemporal pattern of U isotope fractionation recorded in the aqueous solutes. Here, we employ the multi-component, isotope-enabled CrunchTope reactive transport software to interpret these measured U isotope ratios, and demonstrate accurate reproduction of observed trends in both geochemistry and 238 U/ 235 U ratios for two consecutive years of field experiments. Overall, our results indicate that accurately modeling both the U concentration and isotope ratio distributions greatly constrains the parameter space of the model. We find that the transport properties of U in the Rifle aquifer are governed by the presence of low-permeability regions, which the isotopes are uniquely sensitive to. When U reduction is spatially constrained by these low-permeability regions, the shift in the 238 U/ 235 U ratio becomes more muted. Accurate modeling of observed U isotope ratios thus provides a powerful means to better understand bioremediation, and the current study serves to advance the application of this novel method.

238U/235U↗
DOE OSTI2025

U-Pu and Ba-Cs isotopic measurements on Trinitite by laser ablation sampling on the Neoma MC-ICP-MS

In this study we present the results of combined U-Pu and Ba-Cs isotope measurements obtained by laser ablation (LA) sampling of two glassy debris fragments (‘Trinitite’) from the world's first atomic bomb detonation conducted in New Mexico on July 16, 1945. Our primary goal in conducting these measurements was to understand whether examination of the U-Pu and Ba-Cs systematics by direct sampling (e.g. without any chemical separation or purification prior to isotope ratio measurement) could yield meaningful information that would differentiate the Trinitite fragments from glassy material lacking a nuclear fission signature. These measurements were conducted on a ThermoFisher Scientific Neoma multi collector – inductively coupled plasma – mass spectrometer (MC-ICP-MS), which is a relatively new MC-ICP-MS platform, so we also examine the behavior of these isotope systems in standards sampled in solution and via LA. Unsurprisingly, the measurements made on purified solutions of the U, Pu, and Ba isotopic standards produce high precision isotope ratios. Furthermore, this extends to the U-Pu measurements made by LA sampling, with the expected degradation in precision and accuracy related to matrix effects and signal intensity fluctuation. However, the Ba-Cs data acquired by LA is of low precision across all of the matrices examined and bears evidence of complex mass fractionation that will require further investigation to resolve. In total, our results indicate that the observed U-Pu isotope data are of sufficient quality to accurately constrain the U and Pu isotopic composition of glass containing sub-ppm levels of these elements which in turn could be used to differentiate glass containing anthropogenic fission products from natural glass whereas the Ba-Cs LA data cannot be used for this purpose until further methodological refinement is performed.

Ba-Cs↗
DOE OSTI2024

IDB Loader

SAND2024-08428O The IDB Loader is a database designed to hold gamma spectra. IDB is a web-accessible database of reference gamma spectra for measuring uranium (U) and plutonium (Pu) isotopic composition. The database, developed by the International Atomic Energy Agency (IAEA), provides access to well-characterized groups of gamma spectra curated by international experts in gamma spectroscopy. It was created to promote sustainability and maintenance of software used to determine the isotopic abundances of U and Pu. The IDB Loader works by uploading one set of spectral data into an existing IDB. The Data Loader package includes documentation describing the IDB's table, the format of the spectral data, and a description of the loader program. The IDB is currently hosted by the IAEA at: https://nds.iaea.org/idb Sandia National Laboratories is a multimission laboratory managed and operated by National Technology & Engineering Solutions of Sandia, LLC, a wholly owned subsidiary of Honeywell International Inc., for the U.S. Department of Energy’s National Nuclear Security Administration under contract DE-NA0003525.

Schwartz, Steven↗
NASA NTRS1971

Mini gas-core propulsion concept

A propulsion concept is presented that can achieve specific impulses of 1000 to 2000 seconds for thrust levels on the order of 100 pounds (445 N) and maintain a small (1.22 m) reactor diameter for a total power-plant weight of approximately 10,000 kg. The concept combines a small (0.61 m) diameter spherical gas core centrally located, followed by a moderator (BeO-15 cm), surrounded by a driver fuel region and contained in a pressure vessel (ID of 1.22 m). Best results (i.e., highest ratio of cavity power to total power) occur with U-233 isotope as the fuel in both the cavity and the driver, although U-235 can also be used. Concept may also have application in the testing of a gas-core reactor and MHD devices and in high temperature-pressure materials research.

Hyland, R. E.↗
NASA NTRS1971

Mini gas-core propulsion concept.

A propulsion concept is presented that can achieve specific impulses of 1000 to 2000 seconds for thrust levels on the order of 100 pounds (445 N) and maintain a small (1.22 m) reactor diameter for a total power-plant weight of approximately 10,000 kg. The concept combines a small (0.61 m) diameter spherical gas core centrally located, followed by a moderator (BeO-15 cm), surrounded by a driver fuel region and contained in a pressure vessel (ID of 1.22 m). Best results (i.e., highest ratio of cavity power to total power) occur with U-233 isotope as the fuel in both the cavity and the driver, although U-235 can also be used. Concept may also have application in the testing of a gas-core reactor and MHD devices and in high temperature-pressure materials research.

Hyland, R. E.↗
DOE OSTI2025

Comprehensive Measurement of the Reactor Antineutrino Spectrum and Flux at Daya Bay

This Letter reports the precise measurement of the reactor antineutrino spectrum and flux based on the full dataset of 4.7 ×10 6 inverse-beta-decay candidates collected at Daya Bay near detectors. Expressed in terms of the inverse-beta-decay yield per fission, the antineutrino spectra from all reactor fissile isotopes and the specific 235 U and 239 Pu isotopes are measured with 1.3%, 3%, and 8% uncertainties, respectively, near the 3 MeV spectrum peak in reconstructed energy, reaching the best precision in the world. The total antineutrino flux and isotopic 235 U and 239 Pu fluxes are precisely measured to be 5.84 ± 0.07, 6.16 ± 0.12, and 4.16 ± 0.21 in units of 10 −43 cm 2 /fission. These measurements are compared with the Huber-Mueller model, the reevaluated conversion model based on the Kurchatov Institute measurement, and the latest summation model (SM2023). Furthermore, the Daya Bay flux shows good consistency with the Kurchatov Institute and SM2023 models but disagrees with the Huber-Mueller model. The Daya Bay spectrum, however, disagrees with all model predictions.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2023

Investigation of potential polyatomic interferences on uranium isotope ratio measurements for the LS-APGD-Orbitrap MS system

The determination of actinide (e.g., U and Pu) content and isotopics is of importance to the nuclear forensics and safeguards communities. However, in the analysis of environmental samples, such as those collected by the International Atomic Energy Agency, uranium measurements can be complicated by isobaric interferences from polyatomic variants of heavy elements (e.g., Pb). This leads to complex, time-consuming sample manipulations (i.e., separations) before determining isotope ratios. An alternative strategy to sample pretreatment is to use high-resolution mass spectrometric platforms during the analysis to fully resolve the uranium isotopes from potential polyatomic interferences, negating the need for prior chemical separation. The liquid sampling - atmospheric pressure glow discharge (LS-APGD) coupled with an Orbitrap mass spectrometer provides a high-resolution (>70,000 m/Δm at m/z 200) inorganic mass spectrometry platform. Further, as a demonstration of the power of this instrumental platform, and indeed, the high-resolution approach in general, uranium isotope ratios were determined in the presence of elemental impurities (e.g., Pb, Pt, Ta, W) commonly encountered with environmental sample swipe analysis, without any prior treatment. Even at elemental impurity concentrations of 1000–5000× relative to uranium, no interference was observed with the 235 U or 238 U signal. In addition, the 235 U/ 238 U isotope ratio for the samples with the concomitants present are within 2 standard deviations of the values obtained without their addition, indicating that these impurities do not impact the determined uranium isotope ratio. These findings represent a significant first step in leveraging the high resolution of the LS-APGD-Orbitrap-MS to overcome isobaric and molecular interferences instead of relying on chemical separations.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗