Recent efforts have been made toward the integration of the back-end of the nuclear fuel cycle in the United States. The back-end integration seeks to address several management challenges: 1) current storage practices are not optimized for transport and disposal; 2) the impact of interim storage on the disposal strategy needs to be evaluated; and 3) the back-end is affected by—and affects—nuclear fuel cycle and energy policy choices. The back-end integration accounts for the various processes of nuclear waste management—onsite storage, consolidated storage, transport and geological disposal. Ideally, these processes should be fully coupled so that benefits and impacts can be assessed at the level of the full fuel cycle. The paper summarizes the causes and consequences of the absence of integration at the back-end of the nuclear fuel cycle in the U.S., critically reviews ongoing integration efforts, and suggests a framework that would support the back-end integration.

The “safety case” approach has been developed to address the issue of evaluating the performance of a geologic repository in the face of the large uncertainty that results for evaluations that extend over hundreds of thousands of years. This paper reviews the concept of the safety case as it has been defined by the international community. We contrast the safety case approach with that presently used in the U.S. repository program. Especially, we focus on the role of uncertainty quantification. There are inconsistencies between the initial proposal to dealing with uncertainties in a safety case and current U.S. practice. The paper seeks to better define the safety case concept so that it can be usefully applied to the regulatory framework of the U.S. repository program.

The final disposal of nuclear waste is at the interface between the technologies of the nuclear fuel cycle that produce the waste and the natural hydrologic and geochemical cycles of geologic repositories. Despite this broad interdisciplinary scope, nuclear waste management, as practiced, remains “balkanized” among the relevant disciplines. The individual subdisciplines continue to work in relative isolation from one another: materials science dealing with the immobilization of nuclear waste; engineering science dealing with the design, construction and operation of the repository; geoscience dealing with the long-term behavior of host rocks and the hydrology; health science dealing with the effects of radiation; social sciences dealing with the issues of trust, risk and ethics. Understanding how these very different disciplines interact is fundamental to creating and managing a nuclear waste organization. Based on a comprehensive review of the scholarly and scientific literature of waste management, we have analyzed the evolution and structure of research in nuclear waste management between 1979 and 2017. Focusing on materials science, we show that some research themes have been isolated from the most central themes of nuclear waste management. Moreover, we observed a relative decline of the fundamental research in materials science. This decline was evidenced by a drop in the number of articles published in the proceedings of the MRS symposia “Scientific Basis for Nuclear Waste Management” since 2000. We argue for the need to more precisely and inclusively define the field of nuclear waste management.

U60 ([UO2(O2)(OH)]60 60− in water) is a uranyl peroxide nanocluster with a fullerene topology and O h symmetry. U60 clusters can exist in crystalline solids or in liquids; however, little is known of their behavior at high pressures. We compressed the U60-bearing material: Li68K12(OH)20[UO2(O2)(OH)]60(H2O)310 ( $Fm\bar 3$ ; a = 37.884 Å) in a diamond anvil cell to determine its response to increasing pressure. Three length scales and corresponding structural features contribute to the compression response: uranyl peroxide bonds (<0.5 nm), isolated single nanoclusters (2.5 nm), and the long-range periodicity of nanoclusters within the solid (>3.7 nm). Li68K12(OH)20[UO2(O2)(OH)]60(H2O)310 transformed to a tetragonal structure below 2 GPa and irreversibly amorphized between 9.6 and 13 GPa. The bulk modulus of the tetragonal U60-bearing material was 25 ± 2 GPa. The pressure-induced amorphous phase contained intact U60 clusters, which were preserved beyond the loss of long-range periodicity. The persistence of U60 clusters at high pressure may have been enhanced by the interaction between U60 nanoclusters and the alcohol pressure medium. Once formed, U60 nanoclusters persist regardless of their associated long-range ordering—in crystals, amorphous solids, or solutions.

Gd2TixZr2−xO7 (x = 0 to 2) pyrochlore was irradiated by 30 MeV C60 clusters, which provide an extremely high ionizing energy density. High-resolution transmission electron microscopy revealed a complex ion-track structure in Gd2Ti2O7 and Gd2TiZrO7, consisting of an amorphous core and a shell of a disordered, defect-fluorite structure. As compared with the irradiation by 1.5 GeV U ions with the highest energy loss, the track structure is consistent with tracks created by monoatomic swift heavy ions, but the diameters (with the entire diameter of 17 nm for Gd2Ti2O7 and 15 nm for Gd2TiZrO7) are significantly larger due to the much smaller velocity and higher energy density of the C60 ions. Ion tracks created by monoatomic ions are challenging to describe by HRTEM, as the boundary between disordered fluorite and pyrochlore matrix is less distinct. However, the C60 irradiation shows a clearly resolved ion track with completely crystalline, disordered, defect-fluorite structure around an amorphous core. Based on the distinct boundaries of the track morphology, inelastic thermal-spike calculations were used to describe the track size and extract critical energy densities for the interpretation of the complex core–shell morphologies for the different pyrochlore compositions.

Recent efforts to characterize the nanoscale structural and chemical modifications induced by energetic ion irradiation in nuclear materials have greatly benefited from the application of synchrotron-based x-ray diffraction (XRD) and x-ray absorption spectroscopy (XAS) techniques. Key to the study of actinide-bearing materials has been the use of small sample volumes, which are particularly advantageous, as the small quantities minimize the level of radiation exposure at the ion-beam and synchrotron user facility. This approach utilizes energetic heavy ions (energy range: 100 MeV–3 GeV) that pass completely through the sample thickness and deposit an almost constant energy per unit length along their trajectory. High energy x-rays (25–65 keV) from intense synchrotron light sources are then used in transmission geometry to analyze ion-induced structural and chemical modifications throughout the ion tracks. We describe in detail the experimental approach for utilizing synchrotron radiation (SR) to study the radiation response of a range of nuclear materials (e.g., ThO2 and Gd2TixZr2−xO7). Also addressed is the use of high-pressure techniques, such as the heatable diamond anvil cell, as a new means to expose irradiated materials to well-controlled high-temperature (up to 1000 °C) and/or high-pressure (up to 50 GPa) conditions. This is particularly useful for characterizing the annealing kinetics of irradiation-induced material modifications.

Candidate materials for actinide immobilization are subject to alpha-decay event doses that accumulate to values of more than 1020 alpha-decays per gram (tens displacements per atom, dpa) over the extended periods of geologic disposal. To evaluate the radiation-response of actinide-bearing materials, two experimental techniques have been used to accelerate the damage accumulation process: ion-beam irradiations and 244Cm-doping experiments. Based on modern characterization techniques, such as high-resolution transmission electron microscopy, and experimental results that involve ion-beam irradiation and chemical doping with highly active actinides, crystalline ceramics for the immobilization of actinides can be divided into three groups on the basis of their critical doses, Dc, i.e., the dose required for amorphization at 300 K: (i) low resistance to radiation damage accumulation (Dc ∼ 0.2 dpa) – murataite, Ti-perovskite, Fe-garnet; (ii) resistant (0.4 < Dc < 0.6 dpa) – Al-garnet, Ti–Zr-pyrochlore, Al-perovskite; and (iii) highly resistant (Dc > 0.8 dpa) – Zr-, Zr–Ti-, and Sn-pyrochlores. Phases with low critical temperatures (Tc below 600 K) will not become amorphous in a deep geologic repository, as long as the temperature remains between 300 and 550 K, but rather, they will remain crystalline. Only Zr-rich pyrochlore is fully resistant to radiation damage and will remain crystalline over the entire period of its disposal.

A synthetic cubic pyrochlore, Gd2Ti2O7 (Fd3̅m) irradiated with swift heavy ions is compared with a compositionally-related composition La2Ti2O7 (P21), which has a monoclinic, layered, perovskite-type structure. Irradiation experiments were performed at the GSI Helmholtz Center with 181Ta ions and 129Xe ions at specific energies of 11MeV/amu. At these energies the ions pass entirely through the sample thickness of ∼ 40 μm. Angle-dispersive synchrotron powder x-ray diffraction (XRD) measurements were completed and an increasing ion-induced amorphization with increasing ion fluence was for both phases. The ion track cross-sections for the radiation-induced crystalline-to-amorphous transformation, as determined from the evolution of the integrated peak intensities as a function of fluence, reveal that La2Ti2O7 (track diameter, d ∼ 7.2 nm with 181Ta and 5.1 nm with 129Xe) is more susceptible to amorphization than Gd2Ti2O7 (d ∼ 6.2 nm with 181Ta and 4.6 nm with 129Xe). The radiation response of the two titanate compounds can be understood in the context of their different structures and cation ionic radius ratios rA/rB, where the susceptibility of radiation of titanate pyrochlores is proportionate with this radius ratio. The higher electronic linear energy loss of the 181Ta ions as compared with 129Xe ions leads to a consistent increase of volume amorphized per ion in both materials, which manifests as a larger track diameter.

This year marks the 101st anniversary of the sinking of the “unsinkable” RMS Titanic. On April 15, 1912, the Titanic struck an iceberg in the North Atlantic Ocean on its maiden voyage from Southampton, UK, to New York City. There was no single cause for the loss of the Titanic, rather the improbable combination of errors in human design and decision combined with unforeseeable circumstance lead to the loss of over 1,500 lives. The failure appears to have occurred over a range of spatial and temporal scales – from the atomic-scale process of embrittlement of iron rivets to global-scale fluctuations in climate and ocean currents. Regardless of the specific combination of causes, this failure in design and practice led to impressive improvements in both. Disaster and tragedy are harsh teachers, but critical to improvement and progress.

The important question for the nuclear waste management community is how do we learn and improve our waste management strategies in the absence of being able to fail. A geologic repository “operates” over a very distant time frame, and today’s scientists and engineers will never have the benefit of studying a failed system. In place of a failure that is followed by improvement and progress, we can only offer a general consensus on disposal strategies supported by a wide array of evidence and risk assessments. However, it may well be that consensus leads to complacency and compromise, both of which are harbingers of disaster. With this concern in mind, this is the time to review our fundamental approach, particularly the methodologies used in risk assessments that have us calculate risk out to one million years. The structure of standards and implementing regulations, as well as the standard-of-proof for compliance, should be reexamined in order to determine whether their requirements are scientifically possible or reasonable. The demonstration of compliance must not only be compelling, but must also be able to sustain scientific scrutiny and public inquiry. We should benefit from the sobering reality of how difficult it is to anticipate future failures even over a few decades. We should be humbled by the realization that for a geologic repository we are analyzing the performance, success vs. failure, over spatial and temporal scales that stretch over tens of kilometers and out to a hundreds of thousands of years.

A chemical decomposition and related phase transformation have been observed in 2.2 GeV 197Au irradiated SnO2 nanopowder. X-ray diffraction (XRD), Raman spectroscopy, and transmission electron microscopy (TEM) were used to characterize the transformation from tetragonal SnO2 (P42/mnm) into tetragonal SnO (P4/nmm). Rietveld refinement of the XRD data determined the structures and proportion of these phases up to a fluence of 2.4×1013 ions/cm2. The initially intense diffraction maxima corresponding to SnO2 gradually decrease in intensity with an increase in fluence. At a fluence of approximately 3.9×1012 ions/cm2, diffraction maxima corresponding to SnO become clearly evident and increase in intensity as fluence increases. Both Raman and TEM analyses confirm the transformation from tetragonal SnO2 to SnO. The XRD refinement results are consistent with a multiple-impact model of transformation, confirmed by TEM as no single tracks were observed. Previous swift heavy ion irradiations of SnO2 have led only to changes in grain size, degrees of crystallinity, and the formation of “holes”. The inconsistency in results is discussed in depth. The proposed mechanism for the currently observed transformation is the interrelation of defect accumulation and thermal-spike mechanisms. The formation of SnO, apparent O loss from the transformation regions, and associated Sn reduction are discussed in terms of thermodynamic, kinetic, and thermal-spike model considerations.

We have calculated X-ray powder-diffraction data for schoepite, [(UO2)8O2(OH)12](H2O)12, using unit-cell and atomic parameters from the crystal structure (a 14.337, b 16.813, c 14.781, Z=4, Dx=4.87 gcm−3). Schoepite crystallizes in space group P21ca but is strongly pseudo- centrosymmetric, and observed reflections (Irel>0.1%) conform to space group Pbca. The six strongest reflections for schoepite are [d(Å), hkl (relative intensity)] 7.365, 002 (100), 3.253, 242 (55), 3.626, 240 (36), 3.223, 402 (25), 3.683, 004 (20), 2.584, 244 (18). The calculated intensities of reflections that distinguish space group Pbca from space group Pbna (the space group of metaschoepite), i.e., h0l with h odd and l even, are weak, and may not be evident in experimental powder patterns. The a axis of schoepite (14.34 Å) is significantly longer than that of synthetic metaschoepite (13.98 Å), and the two phases can best be distinguished by their unit-cell parameters. However, potential overlap of the strongest reflections can make identification and unit-cell determination difficult, especially for fine-grained material. Natural samples commonly contain intergrowths of schoepite, metaschoepite, and dehydrated schoepite. The calculated powder pattern for schoepite agrees well with data reported for natural schoepite (PDF 13-241) but shows discrepancies with the data from synthesis products. Data for “synthetic schoepite” indicate that this product was a mixture. Powder data labeled “paraschoepite” in the Powder Diffraction File do not correspond to the mineral of that name.

During this century, humankind must deal with increasing demand for energy and the growing impact of burning fossil fuels. Nuclear power, which presently produces 14% of global electricity, is a low-carbon-emissions alternative. However, the sustainability of nuclear power depends on the amounts of uranium and thorium available, the economics of their recovery from ore deposits, and the safety and security of nuclear materials. Unlike combustion of hydrocarbons, which determines the amount of fuel needed for a given amount of energy, nuclear reactions can create additional fissile isotopes. Hence, the choice of nuclear fuel cycle profoundly affects the size of the nuclear resource, as well as nuclear waste management and the risk of proliferation of nuclear weapons. We argue that uranium resources, identified and yet to be discovered, could sustain increases in nuclear power generation by a factor of two or three through the end of this century, even without advanced closed-fuel-cycle technologies.

In this paper, I discuss the basis for the following recommendations for the development of standards and regulations for the long-term disposal of spent nuclear fuel and high-level nuclear waste in a geologic repository:

• • The standard and supporting regulations for the licensing of a geologic repository should be generic - applicable to all potential sites. These standards and regulations should be finalized prior to the site-selection process.

• • Site-selection should be based on a set of common-sense criteria [1]. If during site characterization process it is discovered that the site does not meet the technical criteria, the site should be abandoned. These criteria should not only consider the characteristics of the site, but should also include careful consideration of the degree to which a site can be analyzed. Unnecessary complexity may jeopardize the confidence in the analysis of a suitable site.

• • The standard must acknowledge and adapt its structure and standard-of-proof to the fact that there are two time-scales of interest: the human time-scale that extends to some thousands of years and the geologic time-scale that extends to many hundreds of thousands of years. Reasonable and robust containment at both time scales is possible, but the type of analysis and standard-of-proof will be different for each.

• • Because there are two time-scales and because the types of “proof” for each are very different, the total system analysis of performance, reduced to a single numerical estimate of risk at some very distant time, should be abandoned. The standard should not require scientists and engineers to complete an analysis that is at its best opaque and at its worst not believable.

Systematic first-principles calculations based on density functional theory were performed on a wide range of Ln2TiO5 compositions (Ln = La, Ce, Pr, Nd, Sm, Gd, Tb, Dy and Y) in order to understand the correlation between structural, elastic and electronic properties. A complete set of elastic parameters including elastic constants, Hill’s bulk moduli, shear moduli, Young’s moduli and Poisson’s ratio, were calculated. All Ln2TiO5 are ductile in nature, and analysis of densities of states and charge densities suggests that the oxide bonds are highly ionic.

The resurgence of nuclear power as a strategy for reducing greenhouse gas (GHG) emissions has, in parallel, revived interest in the environmental impact of actinides. Just as GHG emissions are the main environmental impact of the combustion of fossil fuels, the fate of actinides, consumed and produced by nuclear reactions, determines whether nuclear power is viewed as an environmentally “friendly” source of energy. In this article, we summarize the sources of actinides in the nuclear fuel cycle, how actinides are separated by chemical processing, the development of actinide-bearing materials, and the behavior of actinides in the environment. At each stage, actinides present a unique and complicated behavior because of the 5f electronic configurations.

The dynamics of track development due to the passage of relativistic heavy ions through solids is a long-standing issue relevant to nuclear materials, age dating of minerals, space exploration, and nanoscale fabrication of novel devices. We have integrated experimental and simulation approaches to investigate nanoscale phase transitions under the extreme conditions created within single tracks of relativistic ions in Gd2O3(TiO2)x and Gd2Zr2–xTixO7. Track size and internal structure depend on energy density deposition, irradiation temperature, and material composition. Based on the inelastic thermal spike model, molecular dynamics simulations follow the time evolution of individual tracks and reveal the phase transition pathways to the concentric track structures observed experimentally. Individual ion tracks have nanoscale core-shell structures that provide a unique record of the phase transition pathways under extreme conditions.