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Non-Equilibrium Thermodynamic Dissolution Theory for Multi-Component Solid/Liquid Surfaces involving Surface Adsorption and Radiolysis Kinetics.

DE200515013436

Publication Date	2001
Personal Author	Stout, R. B.
Page Count	32
Abstract	A theoretical expression is developed for the dissolution rate response for multi-component radioactive materials that have surface adsorption kinetics and radiolysis kinetics when wetted by a multi-component aqueous solution. An application for this type of dissolution response is the performance evaluation of multi-component spent nuclear fuels(SNFs) for long term interim storage and for geological disposition. Typically, SNF compositions depend on initial composition, uranium oxide and metal alloys being most common, and on reactor burnup which results in a wide range of fission product and actinide concentrations that decay by alpha, beta, and gamma radiation. These compositional/burnup ranges of SNFS, whether placed in interim storage or emplaced in a geologic repository, will potentially be wetted by multi-component aqueous solutions, and these solutions may be further altered by radiolytic aqueous species due to three radiation fields. The solid states of the SNFS are not thermodynamically stable when wetted and will dissolve, with or without radiolysis. The following development of a dissolution theory is based on a non-equilibrium thermodynamic analysis of energy reactions and energy transport across a solid-liquid phase change discontinuity that propagates at a quasi-steady, dissolution velocity. The integral form of the energy balance equation is used for this spatial surface discontinuity analysis. The integral formulation contains internal energy functional of classical thermodynamics for both the SNFS solid state and surface adsorption species, and the adjacent liquid state, which includes radiolytic chemical species. The steady-state concentrations of radiolytic chemical species are expressed by an approximate analysis of the decay radiation transport equation.
Keywords	Radioactive materials Surface adsorption Radiolysis kinetics Surfaces Theoretical expressions Dissolution rate responses Multi-component Aqueous solutions Storage Spent nuclear fuels Thermodynamic dissolution theory Geological disposition
Source Agency	Technical Information Center Oak Ridge Tennessee
Corporate Authors	Lawrence Livermore National Lab., CA.; Department of Energy, Washington, DC.
Supplemental Notes	Sponsored by Department of Energy, Washington, DC.
Document Type	Technical Report
NTIS Issue Number	200602

Non-Equilibrium Thermodynamic Dissolution Theory for Multi-Component Solid/Liquid Surfaces involving Surface Adsorption and Radiolysis Kinetics.

Non-Equilibrium Thermodynamic Dissolution Theory for Multi-Component Solid/Liquid Surfaces involving Surface Adsorption and Radiolysis Kinetics.
DE200515013436

Publication Date	2001
Personal Author	Stout, R. B.
Page Count	32
Abstract	A theoretical expression is developed for the dissolution rate response for multi-component radioactive materials that have surface adsorption kinetics and radiolysis kinetics when wetted by a multi-component aqueous solution. An application for this type of dissolution response is the performance evaluation of multi-component spent nuclear fuels(SNFs) for long term interim storage and for geological disposition. Typically, SNF compositions depend on initial composition, uranium oxide and metal alloys being most common, and on reactor burnup which results in a wide range of fission product and actinide concentrations that decay by alpha, beta, and gamma radiation. These compositional/burnup ranges of SNFS, whether placed in interim storage or emplaced in a geologic repository, will potentially be wetted by multi-component aqueous solutions, and these solutions may be further altered by radiolytic aqueous species due to three radiation fields. The solid states of the SNFS are not thermodynamically stable when wetted and will dissolve, with or without radiolysis. The following development of a dissolution theory is based on a non-equilibrium thermodynamic analysis of energy reactions and energy transport across a solid-liquid phase change discontinuity that propagates at a quasi-steady, dissolution velocity. The integral form of the energy balance equation is used for this spatial surface discontinuity analysis. The integral formulation contains internal energy functional of classical thermodynamics for both the SNFS solid state and surface adsorption species, and the adjacent liquid state, which includes radiolytic chemical species. The steady-state concentrations of radiolytic chemical species are expressed by an approximate analysis of the decay radiation transport equation.
Keywords	Radioactive materials Surface adsorption Radiolysis kinetics Surfaces Theoretical expressions Dissolution rate responses Multi-component Aqueous solutions Storage Spent nuclear fuels Thermodynamic dissolution theory Geological disposition
Source Agency	Technical Information Center Oak Ridge Tennessee
Corporate Authors	Lawrence Livermore National Lab., CA.; Department of Energy, Washington, DC.
Supplemental Notes	Sponsored by Department of Energy, Washington, DC.
Document Type	Technical Report
NTIS Issue Number	200602