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DOE OSTI2016

Nuclear Data Sheets for A = 79

Nuclear spectroscopic information for known nuclides of mass number 79 (Ni,Cu,Zn,Ga,Ge,As,Se,Br,Kr,Rb, Sr,Y,Zr) has been evaluated and presented together with adopted energies, Jπ, and decay modes of levels in these nuclei. No data are yet available for excited states in {sup 79}Ni, {sup 79}Cu and {sup 79}Zr. The half–life of {sup 79}Se, a nuclide of importance in reactor–irradiated fuel composition has been measured by several independent groups and reported in a number of publications after 1995, and seems to be converging to a narrow margin of experimental values. These measurements were likely prompted by a recommendation made in the 1993 update of A = 79 nuclides (1993Si28), that since a 1949PaZZ report, there had been no measurement until 1993, and that based on simulation studies by 1993HeZW, the value listed in 1949PaZZ, and cited in all data tables and charts for 44 years, was quite likely in error, being too low by a factor of 10. According to conclusions in recent papers such as 2014Do20, there is still room for improvement in the measurement of this half–life, and further experiments are expected. This evaluation supersedes earlier Nuclear Data Sheets for A = 79 (2002Si13,1993Si28, 1982Si21,1975Ur03).

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2016

Role of (n,2n) reactions in transmutation of long-lived fission products

The conditions under which (n,γ) and (n,2n) reactions can help or hinder each other in neutron transmutation of long-lived fission products (LLFPs) are considered. Isotopic and elemental transmutation for the main long-lived fission products, {sup 79}Se, {sup 93}Zr, {sup 99}Tc, {sup 107}Pd, {sup 126}Sn, {sup 129}I, and {sup 135}Cs, are considered. The effect of (n,2n) reactions on the equilibrium amount of nuclei of the transmuted isotope and the neutron consumption required for the isotope processing is estimated. The aim of the study is to estimate the influence of (n,2n) reactions on efficiency of neutron LLFP transmutation. The code TIME26 and the libraries of evaluated nuclear data ABBN-93, JEF-PC, and JANIS system are applied. The following results are obtained: (1) The effect of (n,2n) reactions on the minimum number of neutrons required for transmutation and the equilibrium amount of LLFP nuclei is estimated. (2) It is demonstrated that, for three LLFP isotopes ({sup 126}Sn, {sup 129}I, and {sup 135}Cs), (n,γ) and (n,2n) reactions are partners facilitating neutron transmutation. The strongest effect of (n,2n) reaction is found for {sup 126}Sn transmutation (reduction of the neutron consumption by 49% and the equilibrium amount of nuclei by 19%).

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2016

Dry Pretreatment of Used Nuclear Fuel for Tritium Removal: A Review

Virtually all the elements in the periodic chart are generated as a result of atomic fission in nuclear fuel. Several of the elements are volatile or can readily react with other chemicals to form volatile molecules that can be released during the processing of used nuclear fuel for the recovery of the valuable products. Among the volatile fission products, {sup 129}I, {sup 14}C, {sup 3}H, {sup 85}Kr, and {sup 79}Se constitute the main environmental concern for uncontrolled release. Storage of used fuel allows the short-lived isotopes to decay significantly (e.g., {sup 3}H decays in half every 12.32 years and {sup 85}Kr every 10.76 years). However, depending on regulatory limits they may remain an environmental concern up to about 50-100 years of fuel storage. In contrast, the concern for environmental release of the highly mobile {sup 129}I and {sup 14}C remains for geological times (half-lives of 15.7 million years for {sup 129}I and 5730 years for {sup 14}C). Processing of used commercial nuclear fuel requires significant head-end operations to remove the fuel from the protective coverings (e.g., assemblies). The current industrial process includes cropping the end caps of the fuel assemblies, chopping of the fuel pins and/or bundles into short segments, and prolonged leaching of the segments using concentrated nitric acid (HNO{sub 3}). The infrastructure, processes, and waste treatment systems in the head-end operations, including the associated off-gas system, are some of the larger and more costly components of the entire plant. The bulk of the volatile fission products are released to the off-gas during the leaching and dissolution. However, a small but significant amount will transfer to the following steps of processing such as solvent extraction and will show up in many different waste streams. The effective capture of {sup 3}H and iodine throughout the different processes and disposition of associated waste streams is costly and complicated. Up-front removal and capture is highly desirable. Currently, at the U.S. Department of Energy national laboratories and internationally, several dry pretreatment technologies are being studied and developed with the potential to simplify and increase the safety of subsequent storage or chemical recycling processes. These studies include (1) alternative decladding methods, (2) oxidation of exposed fuel following either conventional shearing or chemical decladding, and (3) the collection and stabilization of released volatile radionuclides. Several dry processes are being developed for the up-front removal of tritium and other fission products. They can be combined with different decladding alternatives and, in general, produce a fine powder that can be fed to aqueous or pyrochemical separations processes. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2017

A renewed search for short-lived 126 Sn in the early Solar System: Hydride generation MC-ICPMS for high sensitivity Te isotopic analysis

Although there is limited direct evidence for supernova input into the nascent Solar System many models suggest it formed by the gravitational collapse of a molecular cloud that was triggered by a nearby supernova. Existing lines of evidence mostly in the form of short lived radionuclidespresent in the early Solar System are potentially consistent with this hypothesis but still allow for alternative explanations. Since the natural production of Sn-126 is thought to occur only in supernovae and this isotope has a short half-life (Sn-126 -> Te-126 t(1/2) = 235 ky) the discovery of extant Sn-126 would provide unequivocal proof of supernova input to the early Solar System. Previous attempts to quantify the initial abundance of Sn-126 by examining Sn-Te systematics in early solids have been hampered by difficulties in precisely measuring Te isotope ratios in these materials. Thus here we describe a novel technique that uses hydride generation to dramatically increase the ionization efficiency of Te-an approximately 30-fold increase over previous work. This introduction system when coupled to a MC-ICPMS enables highprecision Te isotopic analyses on samples with < 10 ng of Te. We used this technique to analyze Te from a unique set of calcium-aluminum-rich inclusions (CAIs) that exhibit an exceptionally large range in Sn/Te ratios facilitating the search for the short-lived isotope Sn-126. This sample set shows no evidence of live Sn-126 implying at most minor input of supernova material during the time at which the CAIs formed. However based on the petrology of this sample set combined with the higher than expected concentrations of Sn and Te as well as the lack of nucleosynthetic anomalies in other isotopes of Te suggest that the bulk of the Sn and Te recovered from these particular refractory inclusions is not of primary origin and thus does not represent a primary signature of Sn-Te systematics of the protosolar nebula during condensation of CAIs or their precursors. Although no evidence of supernova input was found based on Sn-Te systematics in this sample set hydride generation represents a powerful tool that can now be used to further explore Te isotope systematics in less altered materials.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

DOE OSTI2017

Identification of Near-infrared [Se iii] and [Kr vi] Emission Lines in Planetary Nebulae

We identify [Se iii] 1.0994 μ m in the planetary nebula (PN) NGC 5315 and [Kr vi] 1.2330 μ m in three PNe from spectra obtained with the Folded-Port InfraRed Echellette (FIRE) spectrometer on the 6.5 m Baade Telescope. Se and Kr are the two most widely detected neutron-capture elements in astrophysical nebulae, and can be enriched by s -process nucleosynthesis in PN progenitor stars. The detection of [Se iii] 1.0994 μ m is particularly valuable when paired with observations of [Se iv] 2.2864 μ m, as it can be used to improve the accuracy of nebular Se abundance determinations, and allows Se ionization correction factor (ICF) schemes to be empirically tested for the first time. We present new effective collision strength calculations for Se{sup 2+} and Kr{sup 5+}, which we use to compute ionic abundances. In NGC 5315, we find that the Se abundance computed from Se{sup 3+}/H{sup +} is lower than that determined with ICFs that incorporate Se{sup 2+}/H{sup +}. We compute new Kr ICFs that take Kr{sup 5+}/H{sup +} into account, by fitting correlations found in grids of Cloudy models between Kr ionic fractions and those of more abundant elements, and use these to derive Kr abundances in four PNe. Observations of [Se iii] and [Kr vi] in a larger sample of PNe, with a range of excitation levels, are needed to rigorously test the ICF prescriptions for Se and our new Kr ICFs.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2024

HTO and selenate diffusion through compacted Na-, Na–Ca-, and Ca-montmorillonite

Radionuclide transport in smectite clay barrier systems used for nuclear waste disposal is controlled by diffusion, with adsorption significantly retarding transport rates. While a relatively minor component of spent nuclear fuel, 79 Se is a major driver of the safety case for spent fuel disposal due to its long half-life (3.3×10 5 yr) and its low adsorption to clay (K D < 10 L/kg), thus a thorough understanding of Se diffusion through clay is critical for understanding the long-term safety of spent fuel disposal systems. Through-diffusion experiments with tritiated water (HTO, conservative tracer) and Se(VI) were conducted with a well-characterized, purified montmorillonite source clay (SWy-2) under a constant ionic strength (0.1 M) and three different electrolyte compositions: Na + , Ca 2+ , and a Na + -Ca 2+ mixture at pH 6.5 in order to probe the effects of electrolyte composition and interlayer cation composition on clay microstructure, Se(VI) aqueous speciation, and ultimately diffusion. Further, the results were modeled using a reactive transport modeling approach to determine values of porosity (ε), D e (effective diffusion coefficient), and K D (distribution coefficient for adsorption). HTO diffusive flux was higher in Ca-montmorillonite (D e =1.68×10 -10 m 2 s -1 ) compared to Na-montmorillonite (De=7.83×10 -11 m 2 s -1 ). This increase in flux is likely due to a greater degree of clay layer stacking in the presence of Ca 2+ compared to Na + , which leads to larger inter-particle pores. Overall, the Se(VI) flux was much lower than the HTO flux due to anion exclusion, with Se(VI) flux following the order Ca (D e = 1.03×10 -11 m 2 s -1 ) > Na–Ca (D e = 2.12×10 -12 m 2 s -1 ) > Na (D e = 1.28×10 -12 m 2 s -1 ). These differences in Se(VI) flux are due to a combination of factors, including (1) larger accessible porosity in Ca-montmorillonite due to clay layer stacking and smaller electrostatic effects compared to Na-montmorillonite, (2) larger accessible porosity for neutral-charge CaSeO4 species which makes up 32% of aqueous Se(VI) in the pure Ca system, and (3) possibly higher Se(VI) adsorption for Ca-montmorillonite. Through a combination of experimental and modeling work, this study highlights the compounding effects that electrolyte and counterion compositions can have on radionuclide transport through clay. Diffusion models that neglect these effects are not transferable from laboratory experimental conditions to in situ repository conditions.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗