Nonequilibrium thermodynamical model for spent fuel dissolution rate

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A non-equilibrium thermodynamic model is developed for the dissolution response of uranium oxide spent fuels waste forms. The objective is to derive function forms for the dissolution rate that are consistent with quasi-static, irreversible thermodynamic processes. These function forms contain thermodynamic chemical potentials of both the solid (spent fuels) and the solution (water chemistries) along with a set of coefficients and parameters that can be evaluated by numerical regression of dissolution test data. Currently, detailed knowledge is not available for the atomic (mechanistic) steps and the sequence of chemical/electro-chemical reaction steps to describe the dissolution process over the range of ... continued below

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4 p.

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Stout, R.B. November 1, 1995.

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A non-equilibrium thermodynamic model is developed for the dissolution response of uranium oxide spent fuels waste forms. The objective is to derive function forms for the dissolution rate that are consistent with quasi-static, irreversible thermodynamic processes. These function forms contain thermodynamic chemical potentials of both the solid (spent fuels) and the solution (water chemistries) along with a set of coefficients and parameters that can be evaluated by numerical regression of dissolution test data. Currently, detailed knowledge is not available for the atomic (mechanistic) steps and the sequence of chemical/electro-chemical reaction steps to describe the dissolution process over the range of spent fuel inventory, potential water chemistries, and temperatures. The existing approach is obtaining an experimental data base of dissolution rates for a subset of spent fuels over a range of controlled, aggressive water chemistries and temperatures. With a numerical regression algorithm, these data are used to evaluate empirical parameters in a rate law. The function form of this rate law is a product polynomial of the bulk water chemistry concentrations and temperature. In its present form, this function form does not have an explicit thermodynamic dependence on the uranium oxide waste form. In addition, the use of bulk concentrations in the function form for the regression analysis of the dissolution data would not explicitly account for a dependence from possible surface to bulk concentration differences due to surface adsorption and dipole layers. The following thermodynamic model uses analysis methods and physical concepts taken primarily from classical mechanics, colloidal foundations, thermodynamics, electro-chemistry, and geochemistry.

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4 p.

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INIS; OSTI as DE96007552

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  • 7. annual international high-level radioactive waste management conference, Las Vegas, NV (United States), 29 Apr - 3 May 1996

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  • Other: DE96007552
  • Report No.: UCRL-JC--122737
  • Report No.: CONF-960421--9
  • Grant Number: W-7405-ENG-48
  • Office of Scientific & Technical Information Report Number: 202338
  • Archival Resource Key: ark:/67531/metadc665769

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  • November 1, 1995

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  • June 29, 2015, 9:42 p.m.

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  • Feb. 19, 2016, 8:28 p.m.

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Stout, R.B. Nonequilibrium thermodynamical model for spent fuel dissolution rate, article, November 1, 1995; California. (digital.library.unt.edu/ark:/67531/metadc665769/: accessed June 24, 2018), University of North Texas Libraries, Digital Library, digital.library.unt.edu; crediting UNT Libraries Government Documents Department.