[en] The recent arms reduction treaties between the U.S. and Russia have resulted in inventories of plutonium in excess of current defense needs. Storage of this material poses significant, and unnecessary, risks of diversion, especially for Russia whose infrastructure for protecting these materials has been weakened since the collapse of the Soviet Union. Moreover, maintaining and protecting these materials in their current form is costly. The United States has about sixty metric tons of excess plutonium, half of which is high-purity weapon material. This high purity material will be converted into mixed oxide (MOX) fuel for use in nuclear reactors. The less pure excess plutonium does not meet the specifications for MOX fuel and will not be purified to meet the fuel specifications. Instead, it will be immobilized directly in a ceramic. The ceramic will be encased in a high level waste (HLW) glass monolith (i.e., the can-in-canister option) thus making a form that simulates the intrinsic security of spent nuclear fuel. The immobilized product will be placed in a HLW repository. To meet the repository requirements, the product must be shown to be durable for the intended storage time, the host matrix must be stable in the radiation environment, the solubility and leaching characteristics of the plutonium in the host material must be established, and optimum processing parameters must be determined for the entire compositional envelope of feed materials. In order to provide technically sound solutions to these issues, thermodynamic data are essential in developing an understanding of the chemistry and phase equilibria of the actinide-bearing mineral waste forms proposed as immobilization matrices. However, the relevant thermodynamic data (e.g., enthalpy, entropy, and heat capacity) for the ceramic forms are severely lacking and this information gap directly affects the Energy Department's ability to license the disposal matrices and methods. High-temperature solution calorimetry is one of the most powerful techniques, sometimes the only technique, for providing the fundamental thermodynamic data needed to establish optimum material fabrication parameters, and more importantly, understand and predict the behavior of the mineral materials in the environment. The purpose of this project is to experimentally determine the enthalpy of formation of actinide orthosilicates, the enthalpies of formation of actinide substituted zircon, zirconolite and pyrochlore, and develop an understanding of the bonding characteristics and stabilities of these materials

[en] The end of the Cold War raised the need for the technical community to be concerned with the disposition of excess nuclear weapon material. The plutonium will either be converted into mixed-oxide fuel for use in nuclear reactors or immobilized in glass or ceramic waste forms and placed in a repository. The stability and behavior of plutonium in the ceramic materials as well as the phase behavior and stability of the ceramic material in the environment is not well established. In order to provide technically sound solutions to these issues, thermodynamic data are essential in developing an understanding of the chemistry and phase equilibria of the actinide-bearing mineral waste form materials proposed as immobilization matrices. Mineral materials of interest include zircon, zirconolite, and pyrochlore. High temperature solution calorimetry is one of the most powerful techniques, sometimes the only technique, for providing the fundamental thermodynamic data needed to establish optimum material fabrication parameters, and more importantly understand and predict the behavior of the mineral materials in the environment. The purpose of this project is to experimentally determine the enthalpy of formation of actinide orthosilicates, the enthalpies of formation of actinide substituted zirconolite and pyrochlore, and develop an understanding of the bonding characteristics and stabilities of these materials

[en] We present changes in volume, immersion density, and tensile property observed from accelerated aged plutonium alloys. Accelerated alloys (or spiked alloys) are plutonium alloys enriched with approximately 7.5 weight percent of the faster-decaying ²³⁸Pu to accelerate the aging process by approximately 17 times the rate of un-aged weapons-grade plutonium. After sixty equivalent years of aging on spiked alloys, the dilatometry shows the samples at 35 C have swelled in volume by 0.15 to 0.17 % and now exhibit a near linear volume increase due to helium in-growth. The immersion density of spiked alloys shows decrease in density, similar normalized volumetric changes (expansion) for spiked alloys. Tensile tests show increasing yield and engineering ultimate strength as spiked alloys are aged. (authors)

[en] We must anticipate that the day is approaching when details of nuclear weapons design and fabrication will become common knowledge. On that day we must be particularly certain that all special nuclear materials (SNM) are adequately accounted for and protected and that we have a clear understanding of the utility of nuclear materials to potential adversaries. To this end, this paper examines the attractiveness of materials mixtures containing SNM and alternate nuclear materials associated with the plutonium-uranium reduction extraction (Purex), uranium extraction (UREX), coextraction (COEX), thorium extraction (THOREX), and PYROX (an electrochemical refining method) reprocessing schemes. This paper provides a set of figures of merit for evaluating material attractiveness that covers a broad range of proliferant state and subnational group capabilities. The primary conclusion of this paper is that all fissile material must be rigorously safeguarded to detect diversion by a state and must be provided the highest levels of physical protection to prevent theft by subnational groups; no 'silver bullet' fuel cycle has been found that will permit the relaxation of current international safeguards or national physical security protection levels. The work reported herein has been performed at the request of the U.S. Department of Energy (DOE) and is based on the calculation of 'attractiveness levels' that are expressed in terms consistent with, but normally reserved for, the nuclear materials in DOE nuclear facilities. The methodology and findings are presented. Additionally, how these attractiveness levels relate to proliferation resistance and physical security is discussed.

[en] Full text: A modified nitride-based uranium fuel to support the small, secured, transportable, and autonomous reactor (SSTAR) concept is initiated at Lawrence Livermore National laboratory (LLNL). This fuel and material research project centers on the evaluation and manufacturing of uranium nitride fuel imbedded with other inert (e.g. ZrN) or neutron-absorbing materials (e.g. HfN) to enhance the fuel properties to achieve long core life. This paper discusses how a modified nitride fuel with chemically-compatible inert additives (ZrN, HfN, etc) could be suitable as replacement fuel for research and test reactors. Mono-uranium nitride fuel pellet is manufactured at the LLNL. Existing facilities and equipment can be employed to fabricate modified uranium nitride fuel cladded in aluminum cladding. Preliminary fuel examination indicated that high uranium loading can be achieved in uranium nitride: at 80 theoretical density, 10.8 g/cc is uranium. Uranium nitride is also favorable in its thermal properties: the thermal conductivity of mono-nitride is compatible to that of silicate (∼25 W/mK), and its melting temperature is much higher than that of metal (2630 deg. C for UN vs. 1100 deg. C for U metal). Out-of-pile experiment is planned to examine the corrosion properties of uranium nitride fuel in water coolant. (author)

[en] This paper examines the material attractiveness of used-fuel assemblies in a hypothetical scenario in which terrorists steal one or more assemblies in order to use the special nuclear materials (SNM) within an assembly in a nuclear explosive device. For assessing material attractiveness, this paper uses the Figure of Merit (FOM) that was used in earlier studies to examine the attractiveness of the SNM associated with the reprocessing of used light water reactor (LWR) fuel by various reprocessing schemes. However, for a theft scenario the mass used in the Acquisition Factor of the FOM is the mass of the stolen object conta ining SNM ; whereas the mass used for analyzing the material attractiveness of the products of various reprocessing schemes in the earlier studies was a fraction of the bare critical mass in recognition that a successful proliferator must avoid a criticality accident. This paper will indicate how long after discharge the radiation emanating from a cooling assembly is no longer self-protecting. Additionally, this paper will give the time scale for the SNM within the assembly to become more attractive. These studies were performed at the request of the United States Department of Energy (DOE), and are based on the calculation of ''attractiveness levels'' that has been couched in terms chosen for consistency with those normally used for nuclear materials in DOE nuclear facilities. The methodology and key findings will be presented. Additionally, this paper discusses how the results presented herein impact the application of safeguards and the securitization of SNM, and how they could be used to help inform policy makers.

[en] This paper summarises the results of an extension to an earlier study [1] that examined the attractiveness of materials mixtures containing special nuclear materials (SNM) associated with the Purex, Urex+ and COEX reprocessing schemes. This study focuses on the materials associated with the Urex, COEX, Thorex and PYROX reprocessing schemes. This study also examines what is required to render plutonium as 'unattractive.' Furthermore, combining the results of this study with those from the earlier study permits a comparison of the uranium- and thorium-based fuel cycles on the basis of the attractiveness of the SNM associated with each fuel cycle. Both studies were performed at the request of the United States Department of Energy (DOE), and are based on the calculation of 'attractiveness levels' that has been couched in terms chosen for consistency with those normally used for nuclear materials in DOE nuclear facilities [2]. The methodology and key findings will be presented. Additionally, how these attractiveness levels relate to proliferation resistance (e.g. by increasing impediments to the diversion, theft, undeclared production of SNM for the purpose of acquiring a nuclear weapon), and how they could be used to help inform policy makers, will be discussed. (authors)

[en] We present dimensional and density changes in an aging plutonium alloy enriched with 7.3 at.% of ²³⁸Pu and reference alloys of various ages. After 45 equivalent years of aging, the enriched alloys at 35 deg. C have swelled in length by 0.048-0.052% and now exhibit a near linear dimensional increase, without void swelling. Based on X-ray diffraction measurements, the lattice expansion by self-irradiation appears to be the primary cause for dimensional changes during the initial 2-3 years of aging. Following the initial transient, the density change is primarily cause by a constant helium in-growth rate as a result of α-particle decay

[en] This paper reports the continued evaluation of the attractiveness of materials mixtures containing special nuclear materials (SNM) associated with various proposed nuclear fuel cycles. Specifically, this paper examines two closed fuel cycles. The first fuel cycle examined is a thorium fuel cycle in which a pressurized heavy water reactor (PHWR) is fueled with mixtures of plutonium/thorium and ²³³U/thorium. The used fuel is then reprocessed using the THOREX process and the actinides are recycled. The second fuel cycle examined consists of conventional light water reactors (LWR) whose fuel is reprocessed for actinides that are then fed to and recycled until consumed in fast-spectrum reactors: fast reactors and accelerator driven systems (ADS). As reprocessing of LWR fuel has already been examined, this paper will focus on the reprocessing of the scheme's fast-spectrum reactors' fuel. This study will indicate what is required to render these materials as having low utility for use in nuclear weapons. Nevertheless, the results of this paper suggest that all reprocessing products evaluated so far need to be rigorously safeguarded and provided high levels of physical protection. These studies were performed at the request of the United States Department of Energy (DOE). The methodology and key findings will be presented.

[en] This paper is an extension to earlier studies that examined the attractiveness of materials mixtures containing special nuclear materials (SNM) and alternate nuclear materials (ANM) associated with the PUREX, UREX, COEX, THOREX, and PYROX reprocessing schemes. This study extends the figure of merit (FOM) for evaluating attractiveness to cover a broad range of proliferant state and sub-national group capabilities. The primary conclusion of this study is that all fissile material needs to be rigorously safeguarded to detect diversion by a state and provided the highest levels of physical protection to prevent theft by sub-national groups; no 'silver bullet' has been found that will permit the relaxation of current international safeguards or national physical security protection levels. This series of studies has been performed at the request of the United States Department of Energy (DOE) and is based on the calculation of 'attractiveness levels' that are expressed in terms consistent with, but normally reserved for nuclear materials in DOE nuclear facilities. The expanded methodology and updated findings are presented. Additionally, how these attractiveness levels relate to proliferation resistance and physical security are discussed.