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The Nuclear Fuel Cycle: Safe Management of Spent Nuclear Fuel

The aim for storage of spent nuclear fuel (SNF) either in wet or in dry storage systems is to ensure general safety objective s are met throughout a desired storage period. Staff at the Savannah River National Laboratory (SRNL), in collaborations with partners at other national laboratories, industry research organizations, and the University of South Carolina (UofSC), have performed materials aging testing and analyses, and have established nuclear materials aging management programs to support extended periods of safe storage of research reactor (RR) SNF and of commercial power reactor (PR) SNF pending ultimate disposal. Several example challenges include susceptibility of aluminum SNF from research reactors to corrosion in poor quality water (wet storage). In dry storage, aluminum SNF can release hydrogen via radiolysis of the hydrated oxides on the aluminum cladding. Austenitic stainless steel canisters used for dry storage are susceptible to chloride-induced stress corrosion cracking (outside-in attack) that threaten the confinement boundary provided by the canister. This paper further describes these challenges, among others, and the formulated solutions to support extended safe storage of SNF.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

A Classification of Commercial Nuclear Reactor Sites and the Subsequent Impacts on Preparing Spent Nuclear Fuel for Shipment - 17355

The US Department of Energy is conducting analyses to inform future decisions regarding an integrated waste management system for the acceptance of spent nuclear fuel (SNF) from commercial nuclear reactor sites. The ability to prepare SNF for shipment from reactor sites is likely to be restricted by ongoing operations at those sites. This report examines the extent to which those operations will restrict the reactor sites' availability to prepare SNF for shipment. Specifically, the analysis focuses on the impact and frequency of refueling operations within the commercial reactor sites in the US. In this report, a characterization of reactor sites into families is described. This characterization is based on the number of operating reactors on site, the length of refueling cycles for those reactors, and the configuration of spent fuel pools on site. Each reactor family is analyzed to estimate the amount of time for which each reactor site in the family would be available to prepare SNF shipments. This analysis is a work in progress, and the results are used to inform the development of new models of an integrated waste management system for commercial SNF. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Overview of Salt Repository Research and Development for Spent Nuclear Fuel and High-level Nuclear Waste in the United States - 20307

This paper summarizes the current US Department of Energy Office of Nuclear Energy's (DOE-NE) work towards developing and executing a research and development program that addresses both scientific and technical issues related to long-term disposal of spent nuclear fuel (SNF) and high-level waste (HLW) in a hypothetical bedded salt based geological repository. A primary goal of the program is to create a generic Geologic Disposal Safety Assessment (GDSA) Framework that can be used to help guide decisions on siting a possible future bedded salt repository. The generic GDSA work includes analysis of the impacts of heat generation caused by decay of short-lived radionuclides. We report progress in four primary areas. First, we discuss the development and recent modifications of a research and development road-map. Second, we briefly describe an experimental approach to better understand thermal processes in salt. Third, we highlight collaborations with the international research community that leverage salt-based repository science around the world. Finally, we discuss how our findings are being used to aid in the development of a generic safety assessment for a bedded salt repository containing SNF and HLW. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Nuclear Data Sheets for A = 65

The evaluators present in this publication spectroscopic data and level schemes from radioactive decay and nuclear reactions studies for all isobars with mass number A=65. Not much is known experimentally about {sup 65}V and {sup 65}Cr, although they are expected to decay by {beta}-emission. Spin/parity assignments for {sup 65}Mn, {sup 65}Fe, {sup 65}As, and {sup 65}Se are not firmly established.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Nuclear Data Sheets for A = 22

Evaluated spectroscopic data and level schemes from radioactive decay and nuclear reaction studies are presented for {sup 22}C, {sup 22}N, {sup 22}O, {sup 22}F, {sup 22}Ne, {sup 22}Na, {sup 22}Mg, {sup 22}Al, and {sup 22}Si. This evaluation for A = 22 supersedes the earlier one by R. B. Firestone (2005Fi16)

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Nuclear Data Sheets for A = 42

The experimental data are evaluated for known nuclides of mass number A = 42 (Al, Si, P, S, Cl, Ar, K, Ca, Sc, Ti, V, Cr). Detailed evaluated level properties and related information are presented, including adopted values of level and γ–ray energies, decay data (energies, intensities and placement of radiations), and other spectroscopic data. This work supersedes earlier full evaluations of A = 42 published by B. Singh, J.A. Cameron – Nucl.Data Sheets 92, 1 (2001) and P.M. Endt – Nucl. Phys. A521, 1 (1990); Errata and Addenda Nucl. Phys. A529, 763 (1991); Errata Nucl. Phys. A564, 609 (1993) (also P.M. Endt – Nucl. Phys. A633, 1 (1998) update). No excited states are known in {sup 42}Al, {sup 42}P, {sup 42}V and {sup 42}Cr, and structure information for {sup 42}Si and {sup 42}S is quite limited. There are no decay schemes available for the decay of {sup 42}Al, {sup 42}Si, {sup 42}P, {sup 42}V and {sup 42}Cr, while the decay schemes of {sup 42}Cl and {sup 42}Ti are incomplete in view of scarcity of data, and large gap between their Q–values and the highest energy levels populated in corresponding daughter nuclei. Structures of {sup 42}Ca, {sup 42}K, {sup 42}Sc and {sup 42}Ar nuclides remain the most extensively studied via many different nuclear reactions and decays.

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O and H diffusion in uraninite: Implications for fluid-uraninite interactions, nuclear waste disposal, and nuclear forensics

Diffusion coefficients for oxygen and hydrogen were determined from a series of natural uraninite H2O experiments between 50 and 700 C. Under hydrous conditions there are two diffusion mechanisms: (1) an initial extremely fast-path diffusion mechanism that overprinted the oxygen isotopic composition of the entire crystals regardless of temperature and (2) a slower volume-diffusive mechanism dominated by defect clusters that displace or eject nearest neighbor oxygen atoms to form two interstitial sites and two partial vacancies, and by vacancy migration. Using the volume diffusion coefficients in the temperature range of 400 600 C, diffusion coefficients for oxygen can be represented by D = 1.90e5 exp (123,382 J/RT) cm2/s and for temperatures between 100 and 300 C the diffusion coefficients can be represented by D = 1.95e10 exp (62484 J/ RT) cm2/s, where the activation energies for uraninite are 123.4 and 62.5 kJ/mol, respectively. Hydrogen diffusion in uraninite appears to be controlled by similar mechanisms as oxygen. Using the volume diffusion coefficients for temperatures between 50 and 700 C, diffusion coefficients for hydrogen can be represented by D = 9.28e6 exp (156,528 J/RT) cm2/s for temperatures between 450 and 700 C and D = 1.39e14 exp (34518 J/RT) cm2/s for temperatures between 50 and 400 C, where the activation energies for uraninite are 156.5 and 34.5 kJ/mol, respectively. Results from these new experiments have implications for isotopic exchange during natural UO2 water interactions. The exceptionally low d18O values of natural uraninites (i.e. 32& to 19.5&) from unconformity-type uranium deposits in Saskatchewan, in conjunction with theoretical and experimental uraninite water and UO3 water fractionation factors, suggest that primary uranium mineralization is not in oxygen isotopic equilibrium with coeval clay and silicate minerals. The low d18O values have been interpreted as resulting from the low temperature overprinting of primary uranium mineralization in the presence of relatively modern meteoric fluids having d18O values of ca. 18&, despite petrographic and U Pb isotope data that indicate limited alteration. Our data show that the anomalously low oxygen isotopic composition of the uraninite from the Athabasca Basin can be due to meteoric water overprinting under reducing conditions, and meteoric water or groundwater can significantly affect the oxygen isotopic composition of spent nuclear fuel in a geologic repository, with minimal change to the chemical composition or texture. Moreover, the rather fast oxygen and hydrogen diffusion coefficients for uraninite, especially at low temperatures, suggest that oxygen and hydrogen diffusion may impart characteristic isotopic signals that can be used to track the route of fissile material.

08 HYDROGEN↗

Nuclear Data Sheets for A = 248

Detailed level schemes, decay schemes, and the experimental data on which they are based are presented for all nuclei with mass number A=248. The experimental reaction and decay data are evaluated; inconsistencies and discrepancies are noted; and adopted values are given for various level properties (including spin and parity, halflife, and configuration), γ properties (including energy, intensity, and multipole character) and α properties (including energy, intensity, and hindrance factor). This evaluation replaces the A=248 evaluation published by A. Akovali in Nuclear Data Sheets 87, 249 (1999)

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Nuclear Data Sheets for A = 86

The experimental nuclear spectroscopic data for known nuclides of mass number 86 (Ga, Ge, As, Se, Br, Kr, Rb, Sr, Y, Zr, Nb, Mo, Tc) have been evaluated and presented together with Adopted properties for levels and γ rays. New high-spin data are available for {sup 86}Se, {sup 86}Br, {sup 86}Kr, {sup 86}Sr, {sup 86}Y, {sup 86}Zr and {sup 86}Mo; and lifetime data for high-spin states in {sup 86}Y and {sup 86}Zr. No significant new data since the 2001 NDS for A=86 have been reported for {sup 86}Rb and {sup 86}Nb. No data are yet available for excited states in {sup 86}Ga and {sup 86}As. The decay scheme of radioactive {sup 86}Ge is unknown, while those for {sup 86}Ga, {sup 86}As, 47.4 min isomer of {sup 86}Y, {sup 86}Nb and {sup 86}Tc are deemed as incomplete. Isomerism in {sup 86}Nb remains unconfirmed. This work supersedes the data presented in the previous NDS evaluation of A=86 published by 2001Si43.

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Nuclear Data Sheets for A = 227

The evaluated spectroscopic data are presented for ten known nuclides of mass 227 (Po, At, Rn, Fr, Ra, Ac, Th, Pa, U, Np). For {sup 227}Po, {sup 227}At, {sup 227}Rn, {sup 227}Pa, {sup 227}U and {sup 227}Np nuclei, only the ground-state information is available. Their decay characteristics are mostly unknown. Levels in {sup 227}Fr are known only from the decay of {sup 227}Rn to {sup 227}Fr. This decay scheme at present cannot be normalized to deduce γ intensities per 100 decays due to lack of knowledge about multipolarities of many low-energy transitions. The levels in {sup 227}Ra, {sup 227}Ac and {sup 227}Th are known from several decays and reactions, including particle-transfer data for {sup 227}Ra and {sup 227}Ac. The decay scheme of {sup 227}Ra to {sup 227}Ac was last studied in 1971 using small Ge detectors. Improved γ-ray intensity data need to be obtained with a better γ-detection system. The datasets for {sup 227}Ac have undergone extensive revisions, including detailed data for 231Pa α decay from 1986BaYK report, and single-proton transfer data from 1986MaYU thesis. High-spin (J>13/2 or so) structures are known only for 227Th. Level lifetime data are quite scarce for all the nuclides in this mass chain, thus limiting the knowledge of reduced transition probabilities. Band structures for {sup 227}Fr, {sup 227}Ra, {sup 227}Ac and {sup 227}Th are known in detail, together with evidence of weak octupole deformation and consequent parity-doublet structures. This evaluation was carried out as part of a joint IAEA-ICTP workshop for Nuclear Structure and Decay Data, organized and hosted by the IAEA, Vienna and ICTP, Trieste, March 24–28, 2014. The evaluation work was coordinated by B. Singh (McMaster). This work supersedes previous A=227 evaluation (2001Br31) published by E. Browne which covered literature before May 2001.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Nuclear Data Sheets for A = 26

Evaluated spectroscopic data and level schemes from radioactive decay and nuclear reaction studies are presented for {sup 26}O, {sup 26}F, {sup 26}Ne, {sup 26}Na, {sup 26}Mg, {sup 26}Al, {sup 26}Si, {sup 26}P, and {sup 26}S. This evaluation for A = 26 supersedes the earlier one by P. M. Endt (1998En04) and updates for some nuclides in ENSDF. Highlights of this evaluation are the following: This evaluation includes search results for {sup 26}S nuclide and its proton–decay mode (2011Fo08). An isomeric state (2.2 ms) in {sup 26}F has been discovered by 2013Le03. The state is proposed at 643.4 keV 1 from γ–ray measurements. Internal-transition and beta-decay branches for the state are also determined. New excited levels in {sup 26}Ne have been identified from {sup 26}F β{sup −} decay (2.2 ms). For some {sup 26}Si resonance states conflicting spin-parity assignments exist in the literature. These are identified by footnotes. 2015Do07 ({sup 3}He,nγ) propose the first 0+ state above proton separation energy at an excitation energy of 5890 keV and suggested for additional independent measurements to confirm or refute the existence of 5946 keV 4. 2016Ch09 consider 5946 keV level as a distinct excited state in their reanalysis of the literature data with possible spin-parity assignment of 0+ or 4+ This evaluation also includes discovery of an isomeric state, at 164.1 keV 1, in {sup 26}P by 2014NiZZ.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Nuclear Data Sheets for A=256

Available nuclear structure information for the known A=256 nuclei (Cf, Es, Fm, Md, No, Lr, Rf and Db) is presented together with Adopted properties of levels and gamma rays. This evaluation supersedes data in the previous evaluations of A=256 nuclides by 1999Ak02, 1989Sc26, 1981Sc06 and 1976Sc02.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Nuclear Data Sheets for A=59☆

-- Abstract: Evaluated spectroscopic data and level schemes from radioactive decay and nuclear reaction studies are presented for {sup 59}Sc, {sup 59}Ti, {sup 59}V, {sup 59}Cr, {sup 59}Mn, {sup 59}Fe, {sup 59}Co, {sup 59}Ni, {sup 59}Cu, {sup 59}Zn, {sup 59}Ga, and {sup 59}Ge. This evaluation for A=59 supersedes the earlier one by C. M. Baglin (2002Ba42) and updates for some nuclides in the ENSDF database. Highlights: of this evaluation are the following: In {sup 59}Fe, a new level at 568.45 keV (3/2{sup −}) has been added. This resolves a doublet at 570 keV, which was reflected in earlier evaluations (1983An22, 1993Ba85, 2002Ba42) and literature as well. Conflicting spin assignments for 2153.62 keV level of {sup 59}Co [9/2,13/2 in (α,pγ); (13/2) in ({sup 15}N,4nγ); 15/2 in (p,p′γ), (7/2{sup −}) in (n,n′γ)] exist in the literature and additional experimental work is needed to resolve the issue.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗