Fundamental Thermodynamics of Actinide-Bearing Mineral Waste Forms

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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 ... continued below

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Williamson, Mark A.; Ebbinghaus, Bartley B. & Navrotsky, Alexandria June 1, 1999.

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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.

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  • Other Information: PBD: 1 Jun 1999

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  • Report No.: EMSP-60118--1999
  • Grant Number: FG07-97ER45673
  • DOI: 10.2172/828524 | External Link
  • Office of Scientific & Technical Information Report Number: 828524
  • Archival Resource Key: ark:/67531/metadc788686

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  • June 1, 1999

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  • Dec. 3, 2015, 9:30 a.m.

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  • Nov. 3, 2016, 1:16 p.m.

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Williamson, Mark A.; Ebbinghaus, Bartley B. & Navrotsky, Alexandria. Fundamental Thermodynamics of Actinide-Bearing Mineral Waste Forms, report, June 1, 1999; Los Alamos, New Mexico. (digital.library.unt.edu/ark:/67531/metadc788686/: accessed September 23, 2017), University of North Texas Libraries, Digital Library, digital.library.unt.edu; crediting UNT Libraries Government Documents Department.