Actinide Abundances Research Articles

Impact of actinide-induced crystal defects on REE-bearing titanite reactivity

Titanite is a widespread accessory silicate which, in some deposits, hosts rare earth elements (REEs) at levels where it can be considered an important carrier. As titanite also accommodates Th and U at concentrations up to 2000 ppm, evidence of metamitctization, a process where radioactive decay of the actinides progressively damages the crystalline structure, is often observed. The current study aims to investigate how the extent of metamictization within a natural titanite specimen may impact its reactivity, principally in the context of REE recovery. Detailed structural characterization revealed the presence of crystalline domains coexisting with sectors having a dominant amorphous component. Compositionally, the density of irradiation-induced defects, leading to amorphization, shows a strong positive correlation not only with the abundance of actinides, but also with the REE concentration. Heat treatment of titanite performed at temperatures ranging from 400 to 800 °C indicates that, while the compositional zonation is maintained, thermal annealing of the defects results in progressive recovery of the crystalline structure. After treatment in sulfuric acid at 200 °C, the habit of reacted titanite grains is highly irregular, indicating distinct decomposition rates for specific sectors, where the more refractory regions coincide with the REE-depleted crystalline domains. A more detailed visualization of the impact of crystal properties on titanite reactivity, obtained by exposing polished grains to a 50% NaOH solution at 50 °C, reveals that, for pristine titanite, the extent of etching observed on crystal surfaces is controlled by the density of the actinide-induced defects, mainly concentrated in the REEs- and Th-enriched amorphous domains. On the other hand, for grains that were initially heat-treated, the etching features are much weaker, emphasizing that thermal annealing renders the crystals less reactive. From these observations, selective REE recovery, where only the more accessible amorphous titanite domains need to be decomposed, seems possible as long as the ore pre-treatment does not involve a high-temperature stage.

Characterizing r-Process Sites through Actinide Production

Of the variations in the elemental abundance patterns of stars enhanced with r-process elements, the variation in the relative actinide-to-lanthanide ratio is among the most significant. We investigate the source of these actinide differences in order to determine whether these variations are due to natural differences in astrophysical sites, or due to the uncertain nuclear properties that are accessed in r-process sites. We find that variations between relative stellar actinide abundances is most likely astrophysical in nature, owing to how neutron-rich the ejecta from an r-process event may be. Furthermore, if an r-process site is capable of generating variations in the neutron-richness of its ejected material, then only one type of r-process site is needed to explain all levels of observed relative actinide enhancements.

Actinide-rich and Actinide-poor r-process-enhanced Metal-poor Stars Do Not Require Separate r-process Progenitors

Abstract The astrophysical production site of the heaviest elements in the universe remains a mystery. Incorporating heavy-element signatures of metal-poor, r-process-enhanced stars into theoretical studies of r-process production can offer crucial constraints on the origin of heavy elements. In this study, we introduce and apply the “actinide-dilution with matching” model to a variety of stellar groups, ranging from actinide-deficient to actinide-enhanced, to empirically characterize r-process ejecta mass as a function of electron fraction. We find that actinide-boost stars do not indicate the need for a unique and separate r-process progenitor. Rather, small variations of neutron richness within the same type of r-process event can account for all observed levels of actinide enhancements. The very low-Y e , fission-cycling ejecta of an r-process event need only constitute 10%–30% of the total ejecta mass to accommodate most actinide abundances of metal-poor stars. We find that our empirical Y e distributions of ejecta are similar to those inferred from studies of GW170817 mass ejecta ratios, which is consistent with neutron-star mergers being a source of the heavy elements in metal-poor, r-process-enhanced stars.

Early Solar System r-process Abundances Limit Collapsar Origin

Abstract Heavy elements produced exclusively through rapid neutron capture (the “r-process”) originate from violent cosmic explosions. While neutron star mergers are the primary candidates, another plausible production site are “collapsars”—collapsing massive stars that form a black hole with an accretion disk. Here we show that collapsars are too rare to be the prime origin of r-process elements in the solar system. By comparing numerical simulations with the early solar system abundances of actinides produced exclusively through the r-process, we exclude higher than 20% contribution from collapsars with 90% confidence. We additionally limit r-process ejecta masses from collapsars to less than 10% of the ejecta mass from neutron star mergers, about 10−2 M ⊙.

Probing the Production of Actinides under Different r-process Conditions

Abstract Several extremely metal-poor stars are known to have an enhanced thorium abundance. These actinide-boost stars have likely inherited material from an r-process that operated under different conditions than the r-process that is reflected in most other metal-poor stars with no actinide enhancement. In this article, we explore the sensitivity of actinide production in r-process calculations to the hydrodynamical conditions as well as the nuclear physics. We find that the initial electron fraction Y e is the most important factor determining the actinide yields and that the abundance ratios between long-lived actinides and lanthanides like europium can vary for different conditions in our calculations. In our setup, conditions with high entropies systematically lead to lower actinide abundances relative to other r-process elements. Furthermore, actinide-enhanced ejecta can also be distinguished from the “regular” composition in other ways, most notably in the second r-process peak abundances.

A nearby neutron-star merger explains the actinide abundances in the early Solar System.

A growing body of evidence indicates that binary neutron-star mergers are the primary origin of heavy elements produced exclusively through rapid neutron capture1-4 (the 'r-process'). As neutron-star mergers occur infrequently, their deposition of radioactive isotopes into the pre-solar nebula could have been dominated by a few nearby events. Although short-lived r-process isotopes-with half-lives shorter than 100 million years-are no longer present in the Solar System, their abundances in the early Solar System are known because their daughter products were preserved in high-temperature condensates found in meteorites5. Here we report that abundances of short-lived r-process isotopes in the early Solar System point to their origin in neutron-star mergers, and indicate substantial deposition by a single nearby merger event. By comparing numerical simulations with the early Solar System abundance ratios of actinides produced exclusively through the r-process, we constrain the rate of occurrence of their Galactic production sites to within about 1-100 per million years. This is consistent with observational estimates of neutron-star merger rates6-8, but rules out supernovae and stellar sources. We further find that there was probably a single nearby merger that produced much of the curium and a substantial fraction of the plutonium present in the early Solar System. Such an event may have occurred about 300 parsecs away from the pre-solar nebula, approximately 80 million years before the formation of the Solar System.

An Integrated Apatite Geochronology and Geochemistry Tool for Sedimentary Provenance Analysis

AbstractSediment provenance studies utilizing detrital geochronology are often limited by source‐rock non‐uniqueness with respect to mineral age. Thus, the development of integrated techniques which permit identification of source rock age and lithology are highly desirable. In this case study from the southern Massif Central, France, we target modern‐river sediment from the river Tarn to assess the utility of combined U‐Pb and multiple trace‐element geochemical analysis of detrital apatite as a provenance tool. The study area was chosen because the sediment source areas chiefly comprise a relatively simple mix of medium‐ to low‐grade Variscan metasediments and late Variscan granitoids, which should yield detrital apatite readily distinguishable by age, trace‐element chemistry, or both. Based on comparison with previously published apatite trace‐element data from metasedimentary rocks and granitoids, pelitic apatite in the river Tarn detritus is primarily distinguished by high Sr/Mn, light rare‐earth element depletion (LREE) and low actinide contents, whereas granitic apatite is characterized by much lower Sr/Mn, and high LREE and actinide abundances. These source rock determinations are highly consistent with apatite trace‐element data from Tarn tributaries that drain either predominantly metapelitic or granitoid catchments. U‐Pb analysis of detrital rutile was also undertaken on those catchments for comparative purposes. As pelitic and granitic apatite can be readily distinguished, samples that have experienced downstream sediment mixing can then be comprehensively characterized. Using this method we identify a source lithology for nearly every analyzed apatite grain in the river sediment, even though 59% of the analyzed grains do not yield reliable U‐Pb ages.

Diagenetic sequestration of rare earths and actinides in phosphatic oil shale from the lacustrine Green River Formation (Eocene), Utah, USA: an SEM and LA-ICP-MS study

The upper Green River Formation of the eastern Uinta Basin of Utah comprises variably organic-rich mudrock deposited in a stratified, alkaline lake that fluctuated in size and in hydrology from open to evaporitic. Beds of oil shale, representing periods of deep lake, suboxic-anoxic deposition include examples with anomalously high phosphate and toxic trace-metal levels, as determined by whole rock X-ray diffraction, scanning electron microscopy (SEM), and both solution and laser-ablation (LA) inductively coupled plasma-mass spectrometry (ICP-MS). The SEM identifies an early, pre-compaction, diagenetic succession of euhedral rhombic dolomite and high-Mg-calcite, nodular pyrite, blocky low-Mg calcite, and microcrystalline carbonate fluorapatite (CFA). LA-ICP-MS indicates the CFA intervals have distinct lower and upper margins where P content rises from ~0.079 to ~3.2% across 2–3 cm of section. Enrichments of rare earth elements (REEs) and actinides (Th, U) show a complex correlation with the phosphatic margins. Light REEs average a tenfold enrichment at the outer margins with progressively heavier REEs exhibiting up to 20-fold enrichment toward the inner margin (Lu from 0.15 to 2.63 ppm). Actinide abundances also increase tenfold (U from ~5 to ~80 ppm) toward the inner margin. There is greatest similarity between Th and the Ho distributions and between U and Lu. This is a similar distribution to what elsewhere has been found in fossil bone and teeth. The microcrystalline CFA is interpreted to have precipitated (or recrystallized from a precursor phosphate) when the rate of dissolved P being generated from organic-matter breakdown exceeded P diffusion rates into the water column, allowing for P supersaturation. As the crystallites grew, diffusion of REE and actinide ions and complexes from surrounding porewaters into the concreting phosphate occurred only until pores were occluded and permeability dropped. As with fossil bone, at the outer margin of the phosphate interval, this allowed for fractionation and preferential substitution of Ca cations in the CFA lattice by light REEs of similar ionic radius. Heavier REEs and actinides of smaller ionic radius diffused further into margin of the phosphate interval.

Nuclear robustness of therprocess in neutron-star mergers

We have performed r-process calculations for matter ejected dynamically in neutron star mergers based on a complete set of trajectories from a three-dimensional relativistic smoothed particle hydrodynamic simulation. Our calculations consider an extended nuclear network, including spontaneous, $\beta$- and neutron-induced fission and adopting fission yield distributions from the ABLA code. We have studied the sensitivity of the r-process abundances to nuclear masses by using different models. Most of the trajectories, corresponding to 90% of the ejected mass, follow a relatively slow expansion allowing for all neutrons to be captured. The resulting abundances are very similar to each other and reproduce the general features of the observed r-process abundance (the second and third peaks, the rare-earth peak and the lead peak) for all mass models as they are mainly determined by the fission yields. We find distinct differences in the abundance yields at and just above the third peak, which can be traced back to different predictions of neutron separation energies for r-process nuclei around neutron number $N=130$. The remaining trajectories, which contribute 10% by mass to the total integrated abundances, follow such a fast expansion that the r process does not use all the neutrons. This also leads to a larger variation of abundances among trajectories as fission does not dominate the r-process dynamics. The total integrated abundances are dominated by contributions from the slow abundances and hence reproduce the general features of the observed r-process abundances. We find that at timescales of weeks relevant for kilonova light curve calculations, the abundance of actinides is larger than the one of lanthanides. Hence actinides can be even more important than lanthanides to determine the photon opacities under kilonova conditions. (Abridged)

A low initial abundance of 247Cm in the early solar system and implications for r-process nucleosynthesis

The short-lived nuclide 247Cm is produced by r-process nucleosynthesis. When the presolar nebula formed, 247Cm became isolated from r-process production and its abundance diminished as a result of radioactive decay. Given its short half-life of only ∼ 16 million years, 247Cm is presently extinct, but its former presence should be detectable as small variations in 235U/ 238U in primitive meteoritic material, provided Cm was chemically fractionated from U at the time these solid objects formed. The magnitude of U isotopic anomalies in meteorites can thus be used to elucidate the timing and character of the last r-process nucleosynthetic event for input into models describing the formation and evolution of the early solar system. Here we report coupled U isotopic determinations and Nd/U proxy measurements for Cm/U in a series of acid-etched leachates and mineral assemblages extracted from meteorites containing primitive phases expected to show strong Cm–U fractionations. Using multiple-collector ICPMS, we are able to determine 235U/ 238U with 2 σ analytical uncertainties of ± 1 epsilon (1 epsilon = 1 part in 10,000) on sample sizes consisting of < 3 ng of 238U and < 20 pg of 235U. A double-spiking procedure using a mixed 236U– 233U spike was employed to allow instrumental mass fractionation to be reliably corrected internally and at high precision. Uranium isotopic results for almost 40 different phases show no resolvable deviations in 235U/ 238U from the chondritic value, at the ∼ 1–2 epsilon level. These data supplement our previous observations for a suite of bulk meteorite samples [C.H. Stirling, A.N. Halliday, D. Porcelli, In search of live 247Cm in the early solar system, Geochim. Cosmochim. Acta 69 (2005) 1059–1071] and provide evidence for a solar system initial 247Cm/ 235U of < 8 × 10 − 5 . Such a low value is difficult to explain without a long time-scale of ∼ 2.3 × 10 8 years between the last actinide producing r-process event and the formation of the solar system. As such it is difficult to reconcile with a model of actinide production in the same r-process forming event as 182Hf with a half-life of 8.9 My [G.J. Wasserburg, M. Busso, R. Gallino, Abundances of actinides and short-lived nonactinides in the interstellar medium: Diverse supernova sources for the r-processes, Astrophys. J. 466 (1996) L109–L113]. The alternative models of 182Hf production via a neutron-rich fast s-process, occurring, for example, in the helium burning shell in a 25 solar mass star during explosive nucleosynthesis [G.J. Wasserburg, M. Busso, R. Gallino, Abundances of actinides and short-lived nonactinides in the interstellar medium: Diverse supernova sources for the r-processes, Astrophys. J. 466 (1996) L109–L113], or via a distinct r-process event that is separate from actinide production [G.J. Wasserburg, M. Busso, R. Gallino, K.M. Nollet, Short-lived nuclei in the early solar system: Possible AGB sources, Nucl. Phys. A (in press)], may provide a viable explanation. However, further studies are also required to assess the veracity of Cm–U systematics, which are critically dependent on the suitability of using Nd and the light rare earth elements (LREEs) as a chemical proxy for Cm.

Reactivity and neutron emission measurements of highly burnt PWR fuel rod samples

Fuel rods with burnup values beyond 50 GWd/t are characterised by relatively large amounts of fission products and a high abundance of major and minor actinides. Of particular interest is the change in the reactivity of the fuel as a function of burnup and the capability of modern codes to predict this change. In addition, the neutron emission from burnt fuel has important implications for the design of transport and storage facilities. Measurements have been made of the reactivity effects and the neutron emission rates of highly burnt uranium oxide and mixed oxide fuel rod samples coming from a pressurised water reactor (PWR). The reactivity measurements have been made in a PWR lattice in the PROTEUS zero-energy reactor moderated in turn with: water, a water and heavy water mixture and water containing boron. A combined transport flask and sample changer was used to insert the 400 mm long burnt fuel rod segments into the reactor. Both control rod compensation and reactor period methods were used to determine the reactivities of the samples. For the range of burnup values investigated, an interesting exponential relationship has been found between the neutron emission rate and the measured reactivity.

Actinides and the sources of cosmic rays

The abundances of the actinide elements in the cosmic rays can provide critical constraints on the major sites of their acceleration. Using recent calculations of the r-process yields in core-collapse supernovae (SNe), we have determined the actinide abundances averaged over various assumed time intervals for their supernovae generation and their cosmic-ray acceleration. Using standard Galactic chemical evolution models, we have also determined the expected actinide abundances in the present interstellar medium. From these two components, we have calculated the U/Th and other actinide abundances expected in the SN-active cores of superbubbles, as a function of their ages and mean metallicity. We calculate the expected actinide abundances in cosmic-rays accelerated by Galactic SNe. We find that the current measurements of actinide/Pt-group and preliminary estimates of the UPuCM/Th ratio in cosmic rays are all consistent with the expected values if superbubble cores have mean metallicities of around three times solar. Future measurements of the abundance ratios will help to solve these questions. First results of experiments performed on the MIR space station (ECCO) and with balloon flights (TIGER) are promising.

Actinides in the Source of Cosmic Rays and the Present Interstellar Medium

The abundances of the actinide elements in the cosmic rays can provide critical constraints on the major sites of their acceleration. Using recent calculations of the r-process yields in core collapse supernovae, we have determined the actinide abundances averaged over various assumed time intervals for their supernova generation and their cosmic-ray acceleration. Using standard Galactic chemical evolution models, we have also determined the expected actinide abundances in the present interstellar medium. From these two components, we have calculated the U/Th and other actinide abundances expected in the supernova-active cores of superbubbles, as a function of their ages and mean metallicity resulting from dilution with interstellar cloud debris. Then, using observations of the fractions of Galactic supernovae that occur in superbubbles and in the rest of the interstellar medium, we calculate the expected actinide abundances in cosmic rays accelerated by Galactic supernovae. We find that the current measurements of actinide/Pt-group and preliminary estimates of the UPuCm/Th ratio in cosmic rays are all consistent with the expected values if superbubble cores have mean metallicities of around 3 times solar. Such metallicities are quite comparable to the superbubble core metallicities inferred from other cosmic-ray observations. Future, more precise measurements of these ratios with experiments such as ECCO are needed to provide a better measure of the mean source metallicity sampled by the local Galactic cosmic rays. Measurements of the cosmic- ray actinide abundances have been favorably compared with the protosolar ratio, inferred from present solar system abundances, to infer that the cosmic rays are accelerated from the general interstellar medium. We suggest, however, that such an inference is not valid because the expected actinide abundances in the present interstellar medium are very different from the protosolar values, which sampled the interstellar medium 4.5 Gyr ago and included an additional fresh ejecta component from a neighboring supernova.

Abundance of actinides in cosmic radiation

Ultra heavy (UH) cosmic rays of Z⩾65 are produced either by s- or r-process of nucleosynthesis. Since these two processes occur under different astrophysical environments, the relative abundances of UH ions could be an important parameter in finding their source and origin. Data analysis is carried out on four detector stacks exposed in space by UH cosmic ray experiment on board LDEF. Scanning and analysis of ∼0.21 m 2 detector area resulted in finding of 72 UH ions (68⩽ Z⩽96) including two actinides (88⩽ Z⩽100). The ratio of actinides to that of sub-actinides is found to be ∼0.034±0.024, which is well within the observational limits of other experiments. Results suggest possible sources, which predominantly ejects r-process synthesized material.

Thorium and Uranium Chronometers Applied to CS 31082‐001

We use the classical r-process model to explore the implications of the recently reported first observation of U in the extremely metal-poor, r-process element–enriched halo star CS 31082-001 for U and Th cosmochronometry. Using updated nuclear physics input and performing a new, conservative, analysis of the remaining uncertainties in the classical r-process model, we confirm that U (together with Th) abundance observations in metal-poor stars are a promising tool for dating r-process events in the early Galaxy, independent of assumptions on Galactic chemical evolution. We show that nuclear physics uncertainties limit the present accuracy of estimated U/Th ages to about 2 Gyr. Critical nuclear data that are required to lower this uncertainty include � -delayed fission branchings and reliable predictions of the onset of deformation in the vicinity of the N ¼ 184 shell closure around 244 Tl, as both directly affect predicted U/Th ratios in r-process models. In this paper we apply, for the first time, the new HFBCS-1 mass model within the framework of the classical r-process model. We find that the predicted U and Th abundances are incompatible with the solar U and Th abundances and trace this back to a different prediction of the onset of deformation around 244 Tl. In the case of CS 31082-001, we find it likely that the zero-age U and Th abundances were enhanced by about a factor of 2.5 compared to both (1) a theoretical extrapolation from the observed stable elements using the classical r-process model and (2) the zero-age abundances of Th and U in other r-process–enhanced, metalpoor halo stars. Although presently ad hoc, this ‘‘ actinide boost ’’ assumption solves the apparent problem of the relative age difference compared with other metal-poor halo stars and, at the same time, the problem of the inconsistency of ages based on U/(stable nucleus), Th/(stable nucleus) and U/Th ratios. There clearly exist differences, among some r-process–enhanced, metal-poor stars, in the level of the elemental abundances of actinides beyond the third r-process peak. Whether CS 31082-001 is a relatively rare case or commonplace awaits the identification of larger numbers of r-process–enhanced, metal-poor stars in which both U and Th can be measured. Using the U/Th ratio, we obtain a best age estimate for the r-process elements in CS 31082001 of 15:5 � 3:2 Gyr. Future observations of Pb and Bi and a better determination of the r-process contribution to solar Pb are needed to put the age estimates for this and other stars on a more solid basis. For our most likely scenario, we provide predictions of the expected upper and lower limits on the abundances of the elements Pb and Bi in CS 31082-001. Subject headings: Galaxy: abundances — Galaxy: evolution — nuclear reactions, nucleosynthesis, abundances — stars: abundances — stars: Population II

The relative abundance of actinides in the cosmic radiation

Abstract The DIAS-ESTEC Ultra Heavy Cosmic Ray Experiment (UHCRE) on the Long Duration Exposure Facility (LDEF) collected approximately 3000 cosmic-ray nuclei with Z>65 in the energy region E>1.5 GeV/nucleon during a six year exposure in Earth orbit. The entire accessible collecting area of the solid-state nuclear-track detector (SSNTD) array has been scanned for actinides, yielding a sample of thirty from an exposure of ≈150 m 2 sr yr. The observed charge spectrum is presented. The current best value for the cosmic-ray actinide relative abundance, (Z>88)/(74≤Z≤87), is given. This value is considered in the context of the predictions of source/propagation models.

Hf–W internal isochrons for ordinary chondrites and the initial [formula omitted] of the solar system

Three ordinary chondrites, Forest Vale (H4), Ste. Marguerite (H4) and Richardton (H5) have been studied with 182 Hf– 182 W system ( t 1/2=9 million years [m.y.]) in order to provide constraints on the initial 182 Hf/ 180 Hf for the chondritic parent body and the solar system. All three samples display positive correlations between 182 W/ 184 W and 180 Hf/ 184 W , providing confirmation that live 182 Hf was present in these samples. The best-fit lines define comparable slopes, passing through, or close to, the data for the bulk carbonaceous chondrites Allende and Murchison. At the current level of resolution this indicates a common and well-mixed chondritic reservoir in terms of the Hf–W isotope system. Forest Vale yields the most precise results with an apparent initial 182 Hf/ 180 Hf of (1.87±0.16)×10 −4 and an initial 182 W/ 184 W of 0.864710±15. If the Pb–Pb phosphate age of Forest Vale (∼5 m.y. younger than the Pb–Pb age of Allende CAI) is a formation age, the bulk solar system initial 182 Hf/ 180 Hf is estimated to be (2.75±0.24)×10 −4, comparable to previous estimates based on the differences in W isotopic compositions between iron meteorites and the mean of carbonaceous chondrites. The solar system 182 W/ 184 W initial of 0.86457±4 ( ε W=−4.99±0.46) is similar to the least radiogenic W reported for iron meteorites, suggesting an extremely early origin of their parent bodies and the segregation of metallic cores from planetesimals. The solar system 182 Hf/ 180 Hf initial obtained in this study is high relative to the initial abundances of other short-lived nuclides, including those with longer half-lives such as 129 I ( t 1/2=16 m.y.). However, this result is explicable with the model of Wasserburg et al. (Wasserburg, G.J., Busso, M., Gallino, R., 1996. Abundances of actinides and short-lived nonactinides in the interstellar medium: diverse supernova sources for the r-processes. Astrophys. J. 466, L109–113) who have proposed that 182 Hf is synthesized in the same r-process supernovae events that produced the actinides over most of galactic history.

Leaching of Spent Fuel in Cladding Segments and After Removal From Cladding

AbstractIn the early 1980s, tests of the leaching behavior of spent light water reactor fuel were conducted in Sweden by SKB and in the USA by the NNWSI Project. Both organizations used fuels with similar burnup, leaching solutions with similar chemical compositions, and conducted the tests at ambient hot cell temperature. Most of the test results were closely similar. The exception was in the recovery of actinide elements at the end of leaching cycles. In the NNWSI tests, the test vessels were stripped with nitric acid at the end of the leaching cycle. When the actinide inventories recovered in the original leaching cycle plus vessel rinse solutions were added to the amount recovered from the acid stripping, the relative abundances of uranium, plutonium, and other actinides were approximately the same as their inventories in the fuel samples. In the SKB tests, the materials recovered from stripping the leaching vessels were low in amount and interpreted to be fine fuel fragments. Only a few percent of the plutonium inventory that would correspond to the uranium recovered in solution was accounted for in the solution samples. To investigate the reasons for this difference in recovery of the actinides, a new test was undertaken using a fuel sample that had been leached for several years using the SKB methods. The fuel was removed from the cladding after a total of a bit more than two years of leaching inside the cladding. The bare fuel was then leached for several cycles using a geometry that simulated the NNWSI tests and a test procedure that was similar to that used in the NNWSI tests. The cladding from which the fuel was removed was also leached in a separate vessel in parallel with the bare fuel leaching. This paper presents the results of the test series and discusses the effects of specimen geometry on the mobility of actinides during leaching. During leaching of spent fuel inside the original cladding, a secondary phase containing Pu seems to form. This phase appears to be less easily dissolved than spent fuel itself.

Abundances of Actinides and Short-lived Nonactinides in the Interstellar Medium: Diverse Supernova Sources for the [ITAL]r[/ITAL]-Processes

Abundances of ^(244)Pu, ^(235)U, ^(238)U, and ^(232)Th in the early solar system are about those expected for uniform production over most of galactic history. The inferred abundance of 182Hf is also compatible with this model. We here associate production of ^(182)Hf with the same r-process SN sources that produce actinides (SNACS). This requires that r-process nucleosynthesis in SNACS took place rather uniformly over the age of the galaxy until ~10^7 yr prior to solar system formation. The low abundance of ^(107)Pd and ^(129)I in the early solar system indicates that SNACS cannot produce these nuclei at the high yields expected from standard r-process models. We propose that there are distinctive SN sources for different r-process nuclei with a sharp distinction in different SN contributions below and above A ~ 140. Abundances in stars with very low metallicities will vary depending on the type of SN contributing to the local region of star formation. A time scale of ~10^7 yr is much shorter than the 108 yr time usually associated with processes in the galaxy and with the last time of r-process injection accounting for ^(129)I, but may be compatible with the rate of SN occurrence. The hypothesis of a nearby SN polluting the protosolar nebula is critically discussed.

Response to Comment by W.A. Myers and P.K. Kuroda on “Actinide abundances in ordinary chondrites”

One aspect of our recent paper (HAGEE et al., 1990) on actinide abundances in ordinary chondrites is estimation of the amount of ^(244)Pu present in these meteorites at the time of their formation. This estimate is based on the quantity of ^(244)Pu spontaneous fission Xe, a component whose resolution from other Xe components present must be based on observed isotopic compositions in the meteorite and assumed compositions for the contributing components. In their comments, MYERS and KURODA (1991) advocate a different approach to component analysis of Xe than the one we used and arrive at correspondingly different estimates of fission Xe and ^(244)Pu abundances.