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At least 217 records · Page 12

Episodic mantle differentiation - Nd and Sr isotopic evidence

A study of Nd and Sr isotopic composition of clinopyroxenes separated from two hydrous and four anhydrous ultramafic nodules is presented. Correlation of Nd-143/Nd-144 with Sm/Nd suggests that a second partial melting occurred about 560 m.y. ago resulting in LREE enrichment of a part of the anhydrous mantle. The isotopic data for anhydrous nodules show that oceanic type mantle underlies at some continental areas. It is concluded that the separation of subcontinental mantle regions from an initially chondritic reservoir may occur in discrete episodes, and that different histories of depletion and/or enrichment will produce isotopically distinct mantle reservoirs.

Stosch, H. G.↗

Re-Os Systematics and HSE Distribution in Metal from Ochansk (H4) Chondrite

Previous studies of the Re-Os systematics of chondrites have documented considerable variation in the Re/Os ratios of whole rock samples. For some whole rock chondrites, Re-Os systematics display large deviations from the primitive isochron that are considerably larger than deviations in other isotope systems. Possible interpretation of these facts is that the Re-Os system in chondrites is particularly sensitive to post-formation alteration processes, thus providing a useful tool to examine such processes. Significant variations that have been detected in highly siderophile element (HSE) patterns for ordinary chondrites support this conclusion. We report Re-Os isotope data for metal separates from the Ochansk H4 chondrite coupled with abundance data for Ru, Pd, Ir, and Pt, determined in the same samples by isotope dilution. We chose this meteorite mainly because it is an observed fall with minimal signs of weathering, and its low metamorphic grade (H4) and shock stage (S3).

Smoliar, M. I.↗

Oxygen isotopes implanted in the LDEF spacecraft

Secondary ion mass spectrometry was used to study oxygen implanted in the surface of copper from the Long Duration Exposure Facility (LDEF). Oxidation that occurred in orbit shows a characteristic oxygen isotope composition, depleted in O-18. The measured depletion is comparable to the predicted depletion (45 percent) based on a model of the gravitational separation of the oxygen isotopes. The anomalous oxygen was contained within 10nm of the surface. Tray E10 was calculated to have received 5.14 x 10(exp 21) atoms of oxygen cm(sup -2) during the LDEF mission and so there is sufficient anomalous implanted oxygen present in the surface to obtain a reliable isotopic profile.

Saxton, J. M.↗

Production, Purification and Characterization of Radioisotopes (Final Report)

This collaborative proposal between the University of Alabama at Birmingham (UAB, PI Suzanne Lapi), and Los Alamos National Laboratory (LANL, collaborator Michael Fassbender) aims to develop novel techniques for isotope production. This proposal takes advantage of complementary techniques available at the UAB cyclotron facility and LANL isotope production facility (IPF) and involved UAB faculty, postdocs, graduate students and undergraduates as well as LANL scientists and staff. This project involved the development of separation techniques for radioisotope production at UAB, using radiotracer analogues produced using the TR24 cyclotron, which would directly translate to separations of the desired isotopes produced at LANL via neutron spallation. Extended visits to LANL by UAB students involved in this initiative were originally envision but were hampered due to COVID restrictions.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Control of iodine and tellurium for use in domestic molybdenum-99 production efforts

Three initial proof-of-concept experiments were performed to test the removal of I and Te from solutions containing Mo for potential abatement during chemical processing to purify 99 Mo. All three proof-of-concept experiments produced results indicating that further optimization could provide methods for I and/or Te abatement from multiple matrices. Decamp and Happel (2013) describe the use of CL resin from Eichrom Technologies loaded with Ag + combined with Amberlite XAD-4 in the chromatographic separation of irradiated fission products in 1 M HNO 3 to separate iodine species where iodide and iodate react with Ag + and I2 adheres to the Amberlite resin. The method worked well under processing conditions in a medical isotope facility although many separation methods use higher concentrations of HNO 3 which could adversely impact the Ag + loading. The experiment performed here used a roughly 2 mL column of CL resin loaded with Ag + and Amberlite XAD-4 to separate µg quantities of I, Te, and Mo in 3 M HNO 3 .

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Radioisotope production at the Spallation Neutron Source: Design concept of experimental target station

Completion of the Proton Power Upgrade Project for the Spallation Neutron Source (SNS) accelerator at Oak Ridge National Laboratory opens an opportunity to utilize reserve beam power of more than 100 kW for applications beyond neutron production. One of these applications is the production of critical radionuclides. To demonstrate the feasibility of using the reserve beam power to produce radioisotope at SNS, a design concept of a small-scale experimental target station in the Linac Dump area has been developed. This experimental facility will provide isotope yield benchmarking data using protons in the GeV range. It will also enable additional research and development in isotope handling and radiochemical separation. The target station consists of a target module enclosed in a vessel and concrete shielding. Particle transport calculations and thermo-mechanical simulations are used to determine beam parameters, decay time, isotope yield, shielding dimensions, and target design parameters. Calculations verified that the irradiated capsule can be handled manually using hands-off tools and transported to a hot cell in a shielded container for post-irradiation characterizations.

Lee, Yong Joong [ORNL] (ORCID:0000000298381723)↗

Development of Solid Isotope Harvesting Methods in Preparation for FRIB (Final Report)

In a collaborative effort between Hunter College (HC), Lawrence Livermore National Laboratory (LLNL), and Michigan State University (MSU), we aimed to investigate the recovery of 88 Zr produced as the secondary beam at the National Superconducting Cyclotron Laboratory (NSCL) from solid collectors via solid isotope harvesting. We developed separation schemes to isolate Zr from sub-gram-scale collectors composed of various materials including carbon, aluminum, copper, tungsten, and gold. The solid harvesting endstation was constructed and then used as part of a dedicated beamtime at the NSCL using 88 Zr beam. After irradiation, the 88 Zr was radiochemically separated from each of the collector materials and the recovery efficiencies from each was assessed. The results of this work provide a path forward for harvesting hydrolysable metals at FRIB as a complementary approach to aqueous isotope harvesting.

07 ISOTOPE AND RADIATION SOURCES↗

Production of Cf-252 and other transplutonium isotopes at Oak Ridge National Laboratory

In 1957 Glenn T. Seaborg conceived and advocated for the construction of the High Flux Isotope Reactor (HFIR) and the Transuranium Processing Plant (since then renamed the Radiochemical Engineering Development Center, or REDC) at Oak Ridge National Laboratory. There, heavily shielded hot cells, glove boxes, and laboratories allow recovery of transuranium elements produced in substantial quantities. Seaborg’s vision of HFIR and REDC producing milligram quantities of berkelium, californium, and einsteinium has been fulfilled beginning in 1966 through May 2019 with 78 production campaigns yielding a cumulative totals of 1.2 g of 249 Bk, 10.2 g of 252 Cf, 39 mg of 253 Es, and 15 pg of 257 Fm. Notably, 252 Cf is a neutron source used in many industrial applications including oil exploration; process control systems for the cement industry, coal analysis, and power production; sources to start nuclear reactors and perform nondestructive materials analyses; homeland security and national defense detection devices; and medical research. Isotopes made available through transplutonium production at HFIR/REDC have enabled scientists to study the nuclear properties and reactions, chemical properties, optical properties, and solid-state properties of transplutonium elements. Long-lived isotopes have served as targets in heavy ion accelerators to produce heavier elements leading to the discovery of 104 Rf, 105 Db, 106 Sg, 113 Nh, 114 Fl, 115 Mc, 116 Lv, 117 Ts, and 118 Og. This paper reviews the evolution of the processing flowsheets to produce, separate, and purify transplutonium isotopes, which have evolved over 50 years of operation at HFIR and REDC, and summarizes directions of future work to improve the efficiency of the production operations.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Age and isotopic relationships among the angrites Lewis Cliff 86010 and Angra dos Reis

The paper presents results of a wide-ranging isotopic investigation of the the Antarctic angrite LEW-86010 (LEW), and reassesses the type angrite Angra dos Reis (ADOR) in order to obtain precise radiometric ages and initial Sr isotopic compositions, and to search for the erstwhile presence of the short-lived nuclei Sm-146 and Al-26 via their daughter products. The isotopic compositions of Sm, U, Ca, and Ti were measured to allow a detailed appraisal to be made of the relations between, and the geneology of, these two angrites. LEW proves to be severely contaminated with modern terrestrial Pb, which is shown to result from terrestrial weathering. Concordant Pb-Pb model ages of pyroxene separates are obtained; uranium isotopic compositions are normal within error. Overall, striking age and isotopic similarities between LEW and ADOR were found, suggesting almost simultaneous production on the same asteroid, even though recent experimental studies imply that the two are not comagmatic.

Lugmair, G. W.↗

The isotopes of neon in the galactic cosmic rays

The paper examines the results obtained by the University of Chicago instrument on board the IMP 7 satellite used to measure the abundances of Ne-20 and Ne-22 in the galactic cosmic rays during 1973-1977, over the general energy range of 60-230 MeV per nucleon. It is reported that the instrument shows a mass resolution of 0.7 amu(sigma) which was confirmed by calibrating a backup instrument at the LBL Bevalac with separated beams of neon isotopes. Through the use of standard solar modulation and cosmic-ray propagation models, the cosmic-ray source ratio inferred is Ne-22/Ne-20 = 0.38 = or -0.07 which is significantly greater than the present solar system ratio. It is concluded that propagation effects or cross-section uncertainties cannot account for such a large abundance of Ne-22, and thus this measurement provides evidence that the cosmic rays come from a source region where the Ne-22 abundance is substantially greater than in solar system material.

Garcia-Munoz, M.↗

Practical considerations for amino acid isotope analysis

Over the last few decades, isotopic analysis of amino acids at the compound- and position-specific levels has been rapidly advancing across diverse fields. As these techniques progress, evaluation of isotopic fractionation associated with sample workup is essential. This critical review of analytical methods through the lens of isotope geochemistry provides a benchmark for researchers across disciplines seeking to make compound- and position-specific amino acid isotope measurements. We focus on preparation, acid hydrolysis, clean-up, derivatization, separation, and C, H, N, and S isotope measurement. Despite substantial customizability across these steps, the following general recommendations should maximize recovery while minimizing isotopic fractionation. Samples should be freeze-dried and stored anoxically at ≤ –20 °C prior to conventional acid hydrolysis (6N HCl, 110 °C, 20–24 h, anoxic), which suffices for many residues. Both gas and liquid chromatographic (GC and LC, respectively) techniques are well-established and separate about 15 amino acids; LC bypasses the need for derivatization, while GC provides higher sensitivity. Furthermore, when derivatization is needed, n-acetyl and alkoxycarbonyl esters provide the most reproducible C isotope ratios. For compound-specific analyses, online GC–IRMS and LC–IRMS systems offer the easiest workflow, but EA–IRMS enables potential multi-element isotope analysis. Emerging techniques like high-resolution mass spectrometry are also promising for multi-element analysis and recover position-specific isotopic information. Looking forward to the next decade of innovation, isotope geochemists and ecologists can improve amino acid isotope analysis by focusing on streamlining multi-element analysis and standardizing calibration practices across laboratories.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Photonuclear Production of Radioxenon for Air Samples

Radioxenon plays an important role in ensuring compliance with the Comprehensive Nuclear-Test-Ban Treaty due to its ability to be transported through the atmosphere, as well as the fact that the half-lives of its isotopes provide a window long enough to be detected but not long enough that it could become background radiation. This allows it to be correlated with specific events that indicate the testing of nuclear weapons. Idaho National Laboratory supports this mission by providing spiked air samples for monitoring stations to enable instrument calibration and ensure measurement accuracy. We tested a photonuclear method of producing one of the main isotopes of radioxenon, Xe-135. We also tested the separation of Xe-135 from the parent isotope Xe-136 using the method of kinematic recoil. Aluminum coils were placed in quartz ampoules filled with enriched Xe-136 and were irradiated by a bremsstrahlung beam with an endpoint energy of 21 MeV. The results showed that we were not only successful in producing Xe-135 but also that the Xe-135 was deposited into the coil allowing it to be removed from the Xe-136 gas. The coil and the Xe-135 can then be chemically separated. At the time of counting the coil, it was calculated that there was about 18 Bq of activity from Xe-135 remaining in the coil. Future work includes determining the optimal material and geometry of the catcher to maximize the amount of Xe-135 captured.

07 ISOTOPE AND RADIATION SOURCES↗

The age of ferroan anorthosite 60025 - Oldest crust on a young moon?

Sm-Nd isotopic data for mineral separates from the ferroan anorthosite 60025, which define a precise isochron of 4.44 + or - 0.02 Ga age, are discussed. This age is about 110 Myr younger than the formation of the first large solid objects in the solar nebula. If the moon is as old as the oldest meteorite, the relatively young age determined for 60025 implies that the magma ocean did not form synchronously with lunar formation or that the magma ocean required over 100 Myr to reach the stage of ferroan anorthosite crystallization. It is proposed that the accumulated body of radiogenic isotope data for lunar rocks permit the moon to be as young as 4.44-4.51 Ga. This is consistent with the idea that the materials that make up the moon were derived from the earth.

Carlson, Richard W.↗

Oxygen isotope studies of ordinary chondrites

Several stages in the evolution of ordinary chondritic meteorites are recorded in the oxygen isotopic composition of the meteorites and their separable components (chondrules, fragments, clasts, and matrix). The whole-rock isotopic compositions reflect the iron-group of the meteorite (H, L, or LL). Isotopic uniformity of H3 to H6 and L3 to L6 are consistent with closed-system metamorphism within each parent body. LL3 chondrites differ slightly from LL4 to LL6, implying a small degree of open-system aqueous alteration and carbon reduction. On the scale of individual chondrules, the meteorites are isotopically heterogeneous, allowing recognition of the solar-nebular processes of chondrule formation. Chondrules for all classes of ordinary chondrites are derived from a common population, which was separate from the population of chondrules in carbonaceous or enstatite chondrites. Chondrules define an isotopic mixing line dominated by exchange between (O - 16)-rich and (O - 16)-poor reservoirs. The oxygen isotopic compositions of chondrites serve as 'fingerprints' for identification of genetic association with other meteorite types (achondrites and iron) and for recognition of source materials in meteoritic breccias.

Clayton, Robert N.↗

Primitive Xe in the atmospheres of Earth and mars

Published data on Xe isotope compositions in primitive carbonaceous meteorites are examined using multidimensional correlation analysis. Distribution of the Xe data in multidimensional data space, except for (129)Xe, can be characterized by a single component, whose isotope composition is identical to 'H plus L minus Xe'. Additional small contributions to the data variations, less than 1 percent of total variations, can be attributed to 'S minus Xe' as well as atmospheric contamination. Isotopic composition of primitive Xe common to the Earth's atmosphere and carbonaceous meteorites are determined with the same assumption as adopted by Pepin and Phinney: primitive Xe is precisely related to fission-free Xe in the Earth's atmosphere by mass fractionation. The determined isotopic composition of primitive Xe is closer to Solar-type Xe, rather than U-Xe (and the primitive Xe estimated from chondrite-achondrite correlation. Hence, the present published data on Xe isotope compositions in meteorites do not seem to require any special component for the primitive Xe common to the Earth's atmosphere and carbonaceous meteorites. Thus Earth's accreting planetesimals would have trapped Xe from the surrounding nebula gases where Xe isotope composition is identical to Solar-type Xe. The trapped Xe was subsequently subject to isotopic fractionation due to gravitational separation as planetesimals grew. Finally fissiogenic Xe from (244)Pu was added to form the present Xe isotope composition of the Earth's atmosphere. The amount of fissiogenic (136)Xe is estimated to be 2.6 percent of the total amount of (136)Xe in the atmosphere, which is about a half of that estimated by Pepin and Phinney (4.65 percent).

Igarashi, G.↗

An approach to separating Pu, U, and Ti from high-purity graphite for isotopic analysis by MC-ICP-MS

Information about elemental and isotopic systematics of ultra-trace level actinides (e.g. U and Pu) and main group elements (e.g. Ti) present within nuclear grade graphite is vital to the nuclear community for improved reactor operation and security. In support of this, extensive effort has been placed on improving analysis methods (i.e., inductively coupled plasma-mass spectrometry). However, significantly less effort has been devoted to the optimization of chemical separation methods. Within the separation community, commercially available Eichrom™ resins are often employed, as their elution characteristics for various elements have been well studied, but the direct optimization of actinides and trace metal separations from a single sample have not been widely investigated. Here, methods using various Eichrom pre-packed cartridges were explored to achieve separation of ultra-trace levels of U, Pu, and Ti from a variety of graphite samples. Once the validity of the combined separation scheme was established using certified reference materials, the method was applied to historic, unirradiated and irradiated, graphite samples. For all samples investigated, precise isotope ratio measurements for the titanium isotope systems were made.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Age determination of a 75 Se gamma radiography source for nuclear forensics

Here, two methods were used to evaluate the age of 75 Se sealed source material. Both methods utilized gamma spectroscopy to determine the quantity of parent 75 Se present, but they differed in the technique used to determine the quantity of daughter 75 As. In one method, 75 As was quantified using inductively coupled plasma-mass spectrometry (ICP-MS) after using chromatographic techniques to separate the parent and daughter isotopes. In the other method, total As was measured using optical emission spectroscopy (OES), which did not require separation prior to measurement. The OES method was faster and gave slightly lower uncertainties, but required more daughter material to be present because of higher concentration requirements, making it unsuitable for young material. Both methods are hampered by the monoisotopic nature of As, but still gave reasonable model ages that were in agreement with each other.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗