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At least 271 records · Page 15

Potential Operating Orbits for the SAFE-400

Safety must be ensured during all phases of space fission system design, development, fabrication, launch, operation, and shutdown. One potential space fission system application is fission electric propulsion (FEP), in which fission energy is converted into electricity and used to power high efficiency (Isp is greater than 3000s) electric thrusters. For these types of systems it is important to determine which operational scenarios ensure safety while allowing maximum mission performance and flexibility. Space fission systems are essentially non-radioactive at launch, prior to extended operation at high power. Once high power operation begins, system radiological inventory steadily increases as fission products build up. For a given fission product isotope, the maximum radiological inventory is typically achieved once the system has operated for a length of time equivalent to several half-lives. After that time, the isotope decays at the same rate it is produced, and no further inventory builds in. For an FEP mission beginning in Earth orbit, altitude and orbital lifetime increase as the propulsion system operates. Two simultaneous effects of fission propulsion system operation are thus (1) increasing fission product inventory and (2) increasing orbital lifetime. Phrased differently, as fission products build up, more time is required for the fission products to naturally convert back into non-radioactive isotopes. Simultaneously, as fission products build up, orbital lifetime increases, providing more time for the fission products to naturally convert back into non-radioactive isotopes. Operational constraints required to ensure safety can thus be quantified.

Houts, Mike↗

Search for extinct natural radioactivity of Pb205 via thallium-isotope anomalies in chondrites and lunar soil.

Thallium and Pb204 contents were determined by stable-isotope-dilution analysis in 16 chondrites, one achondrite, and Apollo 11 and 12 lunar fines. Meteoritic thallium contents vary over a large range, 0.02 to 100 ppb, corresponding to the fact that thallium is a highly fractionated volatile element. Lunar thallium contents are less than 5 ppb. The Tl205/Tl203 ratio was determined in most of the samples, with precision ranging from 0.03% to several percent depending mainly on the amount of thallium present. No variations from the terrestrial ratio were observed. The chondritic isochron slope for Pb205 (13.8-m.y. half-life) is less than or equal to 0.00009 (99% confidence level), corresponding to an interval of at least 60 m.y. and possibly exceeding 120 m.y. between the termination of s-process nucleosynthesis and the lead-thallium fractionations.

Huey, J. M.↗

Lunar and Planetary Science XXXV: Isotopes in Meteorites

The session"Isotopes in Meteorites" consisted of the following presentations:The Common Property of Isotopic Anomalies in Meteorites; Revised Production Rates for 22Na and 54Mn in Meteorites Using Cross Sections Measured for Neutron-induced Reactions; Modeling of 14C and 10Be Production Rates in Meteorites and Lunar Samples; Investigating Xenon Isotopic Fractionation During Rayleigh-type Distillation; The Mean Life Squared Relationship for Abundances of Extinct Radioactivities; and Magnesium Isotopic Fractionation of Forsterite During Evaporation from Different Crystallographic Surfaces.

Source record↗

The coordination properties and ionic radius of actinium: A 120-year-old enigma

Actinium is an elusive element with untamed properties and represents a peculiar case in the periodic table, as its isotopes are all radioactive, the longest-lived one having only a 22-year half-life, and the availability of actinium isotopes remains very low (microgram level, at best), hindering research on its compounds. Despite being a natural element discovered more than 120 years ago, and despite an increasing interest in using one of its isotopes ( 225 Ac) for highly efficient cancer therapies, the chemistry of actinium is still largely unknown relative to other elements. Since Ac is the first element of the actinide series, it is accepted that its ion, Ac 3+ , is the most voluminous trivalent cation of the periodic table. However, the structural data available on Ac 3+ compounds are scarce and have mainly been collected in the 1940-1960's, when actinide chemistry was still in its infancy, and have not been put in perspective with the advances in the chemistry of other elements, making it difficult to accurately evaluate its actual size and coordination chemistry. Here, we review progress made on the chemistry of lanthanides and actinides and reevaluate the structural data published on Ac 3+ since the era of the Manhattan Project. The data are combined across different spectroscopic and characterization methods and presented in the context of periodic trends. When considering crystallographic data, solution chemistry results, and the nuclear properties of actinium isotopes, it appears that some structural parameters ascribed to the Ac 3+ ion may have been overestimated. This review can guide researchers interested in actinide sciences and those who are pursuing the development of actinium-based radiotherapies, from isotope production to clinical trials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Gamma-ray spectra analyses of molten salts in spent nuclear fuels pyroprocessing facilities for mass measurement

To evaluate radioactive tracer dilution and gamma spectroscopy as a safeguards technique for monitoring the mass of liquid salt in molten salt systems, the gamma spectroscopy data of salt samples from the pyroprocessing facilities in Idaho National Laboratory were acquired and analyzed. The primary focus is the uncertainty analysis of the gamma radioactivity of 154 Eu isotope in the molten salts. The facilities include an electrorefiner for pyroprocessing spent oxide fuels (SOF-ER) and Mark-IV ER for processing the metallic fuels from Experimental Breeder Reactor-II (EBR-II). The relative gamma radioactivity uncertainty was consistently at 3% for 137 Cs for both Mark-IV ER and SOF-ER salts. However, for 154 Eu, it was 8% for SOF-ER salt and 7% for Mark-IV ER salt. Here, the main reason for the higher uncertainty for 154 Eu is believed to be the lower counting statistics in gamma spectroscopy. To improve the gamma radioactivity uncertainty of isotope 154 Eu, a longer data acquisition time (12 h instead of 4 h) and a higher count rate gamma detector for gamma spectroscopy were tested and it was found that the uncertainty for 154 Eu was significantly improved from 7% or 8–3%.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Cosmic-ray isotopic composition

The 'age' of the cosmic rays and the origin of cosmic ray source matter are discussed. General approaches to the interpretation of the abundances of secondary radioactive nuclides are reviewed using Be-10 as an illustration. The present state of Be-10 based cosmic ray age determinations are summarized, briefly mentioning some recent results based on the isotope Al-26. The effects of nonhomogeneous propagation models on the interpretation of the radioactive isotope observations are mentioned. The cosmic ray source isotopic composition is discussed, emphasizing the neon composition. Mass histogram findings on the abundance of various elements in cosmic rays are described and possible reasons for some abundance enhancements are considered.

Wiedenbeck, M. E.↗

Isotopic discrimination of natural and anthropogenic perchlorate sources in groundwater in a semi-arid region of northeastern Oregon (USA)

Perchlorate (ClO 4 - ) has synthetic and natural sources. Synthetic ClO 4 - is released to the environment from its use as an oxidant in military and aerospace applications, and from its presence in a variety of common commercial products, such as safety flares, chlorate herbicides, and fireworks. Natural sources of ClO 4 - in the environment include imported nitrate fertilizers derived from salt deposits in the Atacama Desert of Chile and indigenous natural ClO 4 - that accumulates in unsaturated soils and groundwaters in other arid and semi-arid environments, largely from atmospheric deposition. The stable isotope ratios of chlorine ( 37 Cl/ 35 Cl) and oxygen ( 18 O/ 16 O, 17 O/ 16 O) and the isotopic abundance of radioactive 36 Cl in ClO 4 - can be used to discriminate these different sources. Perchlorate was previously detected at relatively high concentrations (3.8–34.7 μg/L) in groundwater from many wells in the Boardman-Umatilla area near the Columbia River in northeastern Oregon, which is a semi-arid, highly agricultural, heavily irrigated area that includes several past and current military installations. Eight representative groundwater wells were sampled throughout this region and isotopic characteristics of ClO 4 - collected from each well were measured along with other chemical and isotopic parameters including tritium and other groundwater age indicators. We report isotopic data indicate that indigenous natural ClO 4 - was present in groundwater from all sampled wells and was the predominant source in five of the wells. Synthetic ClO 4 - was present in the three remaining wells with natural ClO 4 - , and a minor fraction of Atacama-fertilizer-derived ClO4- was indicated in one of the wells. Data from this study expand the geographic area of the USA in which indigenous natural ClO 4 - has been detected to include the semi-arid northwest. This study also illustrates the role of irrigation recharge as a mechanism for producing relatively high concentrations of indigenous natural ClO 4 - in groundwater by flushing accumulated salts from the unsaturated zone.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Target development using the method of High-Intensity Vibrational Powder Plating (HIVIPP) at the Center for Accelerator Target Science (CATS) at Argonne National Laboratory (ANL)

One of the primary goals of the Center for Accelerator Target Science (CATS) is to provide targets and foils in support of the ATLAS User Facility and the Low-Energy community at large. While a wide array of target production techniques are available at CATS, new methods that must be explored invariably arise. One such technique, the High-Intensity Vibrational Powder Plating (HIVIPP), was first reported in 1997 by Isao Sugai. It was developed to produce targets and stripper foils that were difficult to make by standard methods. At Argonne National Laboratory (ANL), we have successfully constructed and tested a simple system for this purpose. We have produced targets of carbon and titanium on various metal backings using the HIVIPP method. We are currently in the exciting phase of exploring the production of other elements, including isotopically enriched and radioactive material. This work is in progress and will be further detailed with specific examples.

47 OTHER INSTRUMENTATION↗

Three Dimensional Characterization of the Mundrabilla Meteorite

The differentiated meteorite, Mundrabilla, exhibits a rare structure of primary kamacite/taenite, and at least 25 volume % of sulfide (troilite and daubreelite). The structure has been investigated in three dimensions using the technique of gamma-ray computed tomography (CT) with a radioactive (60)Co isotope as the source of the flux. Using CT, a 50 kg slab with dimensions 12.6 x 8.2 x approx. 70 cm has been sectioned at 1 mm intervals over 50 cm length, and the three dimensional structure is at present being evaluated. These data revealed, in addition to the metallic and troilite-rich phases, the presence and distribution of graphite-rich cones (up to 5 cm long), and small (1-2 mm), low density particles. The graphite cones are readily visible on the surfaces of many of the sections of Mundrabilla, while the smaller phases have a density (determined from CT) of approximately 2.9 g/cc, and are assumed to be silicate inclusions. CT spatial resolution is not adequate to elucidate the shapes of these particles. One can only state that they show no directionality and are equiaxed.

Gillies, Donald C.↗

Development of Stirling Convertors for Radioisotope and Fission Power Systems

NASA has been developing free-piston Stirling-cycle power convertors over the past 22 years for use in nuclear power systems that would provide electricity for space science missions to dark, dusty, or distant destinations where solar power is not practical. These nuclear power systems would generate heat from either the radioactive decay of isotopes or fission nuclear reactors. That heat would be converted to usable electricity using highly efficient Stirling convertors for a wide range of power needs needing 10s of watts to 50 kWe. NASA’s Radioisotope Power Systems (RPS) Program is maturing advanced thermoelectric and dynamic conversion technologies that would increase the system efficiency beyond what is currently possible using heritage systems to enable a larger number of robotic missions or higher power missions to solar system bodies of interest. The Dynamic Radioisotope Power Systems (DRPS) Project has matured prototype Stirling convertors to sufficiently increase the technology readiness level for infusion into flight development. Flexure and gas-bearing free-piston Stirling convertors were developed under contract by commercial partners and delivered to enable government evaluation. Gas-bearing designs have met performance and robustness requirements and were selected for flight development. This paper provides the status of SRSC test campaign and maturity level.

Dynamic↗

Development of Stirling Convertors for Radioisotope and Fission Power Systems

NASA has been developing free-piston Stirling-cycle power convertors over the past 22 years for use in nuclear power systems that would provide electricity for space science missions to dark, dusty, or distant destinations where solar power is not practical. These nuclear power systems would generate heat from either the radioactive decay of isotopes or fission nuclear reactors. That heat would be converted to usable electricity using highly efficient Stirling convertors for a wide range of power needs needing 10s of watts to 50 kWe. NASA’s Radioisotope Power Systems (RPS) Program is maturing advanced thermoelectric and dynamic conversion technologies that would increase the system efficiency beyond what is currently possible using heritage systems to enable a larger number of robotic missions or higher power missions to solar system bodies of interest. The Dynamic Radioisotope Power Systems (DRPS) Project has matured prototype Stirling convertors to sufficiently increase the technology readiness level for infusion into flight development. Flexure and gas-bearing free-piston Stirling convertors were developed under contract by commercial partners and delivered to enable government evaluation. Gas-bearing designs have met performance and robustness requirements and were selected for flight development. This paper provides the status of SRSC test campaign and maturity level.

Dynamic↗

Asymptotic Giant Branch stars as a source of short-lived radioactive nuclei in the solar nebula

We carried out a theoretical evaluation of the contribution of Asymptotic Giant Branch (AGB) stars to some short-lived (10(exp 6) less than or equal to Tau-bar less than or equal to 2 x 10(exp 7) yr) isotopes in the Interstellar Medium (ISM) and in the early solar system using stellar model calculations for thermally pulsing evolutionary phases of low-mass stars. The yields of s-process nuclei in the convective He-shell for different neutron exposures tau(sub 0) were obtained, and AGB stars were shown to produce several radioactive nuclei (especially Pd-107, Pb-205, Fe-60, Zr-93, Tc-99, Cs-135, and Hf-182) in diferent amounts. Assuming either contamination of the solar nebula from a single AGB star or models for continuous injection and mixing from many stars into the ISM, we calculate the ratios of radioactive to stable nuclei at the epoch of the Sun's formation. The dilution factor between the AGB ejecta and the early solar system matter is obtained by matching the observed Pd-107/Pd-108 and depends on the value of tau(sub 0). It is found that small masses M(sub He) of He-shell material (10(exp -4)-10(exp -7) solar mass) enriched in s-process nuclei are sufficient to contaminate 1 solar mass of the ISM to produce the Pd-107 found in the early solar system. Predictions are made for all of the other radioactive isotopes. The optimal model to explain several observed radioactive species at different states of the proto-solar nebula involves a single AGB star with a low neutron exposure (tau(sub 0) = 0.03 mbarn(sup -1)) which contaminated the cloud with a dilution factor of M(sub He)/solar mass approximately 1.5 x 10(exp -4). This will also contribute newly synthesized stable s-process nuclei in the amount of approximately 10(exp -4) of their abundances already present in the proto-solar cloud. Variations in the degree of homogenization (approximately 30%) of the injected material may account for some of the small general isotopic anomalies found in meteorites. It is also found that Fe-60 is produced in small but significant quantities that may be sufficient to explain the observations if the time elapsed delta from the contamination of the ISM to the formation of protoplanetary bodies is not higher than delta = 5 x 10(exp 6) yr. If delta is longer, up to 10 x 10(exp 6) yr, this would require the single AGB star to experience enhanced neutron densities (n(sub n) approximately 3 x 10(exp 9)n/cu cm) in the s-processing zone in order to compensate for the branching at Fe-59. The alternative model of long-term continuous ejection of matter from many AGB stars does not appear to match the observations. We also estimate the Al-26 production from the H-shell and find that the Al-26 abundance in the early solar system may be readily explained in a self-consistent manner. Moreover, Al-26 from AGB stars may contribute substantially to the galactic Al-26 gamma-source, while no significant gamma-flux from Co-60 (deriving from Fe-60 decay) is to be expected.

Wasserburg, G. J.↗

Experimental studies of the two-step scheme with an intense radioactive 132 Sn beam for next-generation production of very neutron-rich nuclei

The study of nuclei in the yet-unexplored, very neutron-rich, mid- to heavy-mass region of the nuclear chart, comprising perhaps half of all nuclei predicted to exist, is leading to new and/or upgraded facilities, as well as to research into the underlying production processes. In the present study, the usefulness of the two-step scheme, an alternate method to produce very neutron-rich nuclei, by a combination of an isotope-separation online (ISOL) system as a first step, and in-beam fragmentation of re-accelerated radioactive isotopes (RIs) as a second step, was investigated with a 132 Sn beam. In this work, very neutron-rich RIs around the neutron-rich neutron number N = 82 region were produced from the 278-MeV/nucleon 132 Sn beam impinging on a 5.97-mm Be target, and their production cross sections were measured. Yields were then estimated for the two-step scheme with the 132 Sn beam relative to the ones by a one-step scheme, in-flight fission of a 238 U beam, for 1-MW proton and 238 U beams at respective RI-beam facilities. This comparison suggests that the two-step scheme with the 132 Sn beam provides yields >40-times higher than those with the one-step scheme for the very neutron-rich N = 82 region. Moreover, by using various RI beams over the nuclear chart from ISOL, certain kinds of very neutron-rich RIs around the supernova r-process path can be produced with greater yields than by the one-step approach.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Radioactive halos and ion microprobe measurement of Pb isotope ratios

This investigation was to obtain, if possible, the Pb isotope ratios of both lunar and meteoritic troilite grains by utilizing ion microprobe techniques. Such direct in situ measurement of Pb isotope ratios would eliminate contamination problems inherent in wet chemistry separation procedures, and conceivably determine whether lunar troilite grains were of meteoritic origin. For comparison purposes two samples of meteoritic troilite were selected (one from Canyon Diablo) for analysis along with two very small lunar troilite grains (approximately 50-100 microns). It was concluded that the ion microprobe as presently operating, does not permit the in situ measurement of Pb isotope ratios in lunar or meteoritic troilite. On the basis of these experiments no conclusions could be drawn as to the origin of the lunar troilite grains.

Gentry, R. V.↗

Inline gamma-spectrometry of fission product elements after rapid high-pressure ion chromatographic separation

Analysis of irradiated material shortly after irradiation can be non-trivial due to highly radioactive activation and fission isotopes increasing dead time in gamma-ray detection systems, often requiring a “cooling-period” between receipt of a sample and the subsequent analysis. A direct separation–detection method has been developed combining ion chromatography and inductively coupled mass spectrometry for rapid, low-level analysis of fission products; it cannot, however, detect certain short-lived species below the detection limit of the system. In this paper we report the implementation of an inline gamma-ray detector, which was added post-separation, pre-analysis, to test the quality and utility of elementally-isolated gamma-ray spectroscopy.

Inline gamma-ray detection↗

Resolution of a discrepancy in the γ-ray emission probability from the β decay of 137 Ce g

We have deduced the emission probability of the 447-keV γ ray from the ε + β + decay of Ce g 137 (9.0 h) relative to that of the 254-keV γ ray from the Ce m 137 (34.4 h) decay in transient equilibrium. The time-dependent factor in transient equilibrium was applied following the Bateman equation for a radioactive decay chain. The isotope was produced via the La 139 ( p , 3 n ) Ce m , g 137 reaction by bombarding nat La with a proton beam from the 88-in. cyclotron at Lawrence Berkeley National Laboratory. γ -ray intensities were measured using an HPGe detector. The emission probability for the 447-keV γ ray deduced in this work is 1.21(3) (that is 1.21 ± 0.03) per hundred parent decays, which differs significantly from an earlier published value of 2.24(10). We identify the source of this discrepancy to be an incorrect use of the time-dependent factor. Additionally, we have deduced the emission probability of the 504-keV γ ray from the decay of Y g 85 (2.68 h) relative to that of the 232-keV γ ray from the Sr m 85 (1.127 h) decay in transient equilibrium. The isotope was produced via the Sr 86 ( p , 2 n ) Y g 85 reaction by bombarding SrCO 3 86 with a proton beam at the same facility. Overall, the study confirms the assumption of the time-dependent correction for recommending the emission probability of the 504-keV γ ray in the literature. Our work highlights the importance of explicit description by authors of any time-dependent correction they have made when reporting γ -ray intensities for nuclides in transient equilibrium. The need and significance of accurate and precise decay data of Ce g 137 and Y g 85 in basic science and medicine is briefly outlined.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗