skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: First principles Candu fuel model and validation experimentation

Abstract

Many modeling projects on nuclear fuel rest on a quantitative understanding of the co-existing phases at various stages of burnup. Since the various fission products have considerably different abilities to chemically associate with oxygen, and the O/M ratio is slowly changing as well, the chemical potential (generally expressed as an equivalent oxygen partial pressure) is a function of burnup. Concurrently, well-recognized small fractions of new phases such as inert gas, noble metals, zirconates, etc. also develop. To further complicate matters, the dominant UO{sub 2} fuel phase may be non-stoichiometric and most of minor phases have a variable composition dependent on temperature and possible contact with the coolant in the event of a sheathing defect. A Thermodynamic Fuel Model to predict the phases in partially burned Candu nuclear fuel containing many major fission products has been under development. This model is capable of handling non-stoichiometry in the UO{sub 2} fluorite phase, dilute solution behaviour of significant solute oxides, noble metal inclusions, a second metal solid solution U(Pd-Rh-Ru)3, zirconate and uranate solutions as well as other minor solid phases, and volatile gaseous species. The treatment is a melding of several thermodynamic modeling projects dealing with isolated aspects of this important multi-component system.more » To simplify the computations, the number of elements has been limited to twenty major representative fission products known to appear in spent fuel. The proportion of elements must first be generated using SCALES-5. Oxygen is inferred from the concentration of the other elements. Provision to study the disposition of very minor fission products is included within the general treatment but these are introduced only on an as needed basis for a particular purpose. The building blocks of the model are the standard Gibbs energies of formation of the many possible compounds expressed as a function of temperature. To these data are added mixing terms associated with the appearance of the component species in particular phases. To validate the model, coulometric titration experiments relating the chemical potential of oxygen to the moles of oxygen introduced to SIMFUEL are underway. A description of the apparatus to oxidize and reduce samples in a controlled way in a H{sub 2}/H{sub 2}O mixture is presented. Existing measurements for irradiated fuel, both defected and non-defected, are also being incorporated into the validation process. (authors)« less

Authors:
; ; ;  [1];  [2];  [3]; ; ;  [4]
  1. Royal Military College of Canada, Department of Chemistry and Chemical Engineering, P.O. Box 17000 Station Forces, Kingston, Ontario K7K 7B4 (Canada)
  2. Atomic Energy of Canada Limited - Chalk River Ontario, Ontario KOJ IJ0 (Canada)
  3. Atomic Energy of Canada Limited - 430 Bayside Drive, Saint John, NB E2J 1A8 (Canada)
  4. Atomic Energy of Canada Limited - Chalk River Laboratories, Chalk River Ontario, Ontario KOJ IJ0 (Canada)
Publication Date:
Research Org.:
American Nuclear Society, 555 North Kensington Avenue, La Grange Park, IL 60526 (United States)
OSTI Identifier:
21229268
Resource Type:
Conference
Resource Relation:
Conference: 2007 LWR Fuel Performance Meeting / TopFuel 2007, San Francisco, CA (United States), 30 Sep - 3 Oct 2007; Other Information: Country of input: France; 44 refs; Related Information: In: Proceedings of the 2007 LWR Fuel Performance Meeting / TopFuel 2007 'Zero by 2010', 683 pages.
Country of Publication:
United States
Language:
English
Subject:
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS; 37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; BURNUP; CALCULATION METHODS; FISSION PRODUCTS; FLUORITE; HYDROGEN; OXYGEN; PARTIAL PRESSURE; SIMULATION; SOLID SOLUTIONS; SPENT FUELS; TITRATION; URANATES; URANIUM DIOXIDE; VALIDATION; ZIRCONATES

Citation Formats

Corcoran, E C, Kaye, M H, Lewis, B J, Thompson, W T, Akbari, F, Royal Military College of Canada, Department of Chemistry and Chemical Engineering, P.O. Box 17000 Station Forces, Kingston, Ontario K7K 7B4, Higgs, J D, Royal Military College of Canada, Department of Chemistry and Chemical Engineering, P.O. Box 17000 Station Forces, Kingston, Ontario K7K 7B4, Verrall, R A, He, Z, and Mouris, J F. First principles Candu fuel model and validation experimentation. United States: N. p., 2007. Web.
Corcoran, E C, Kaye, M H, Lewis, B J, Thompson, W T, Akbari, F, Royal Military College of Canada, Department of Chemistry and Chemical Engineering, P.O. Box 17000 Station Forces, Kingston, Ontario K7K 7B4, Higgs, J D, Royal Military College of Canada, Department of Chemistry and Chemical Engineering, P.O. Box 17000 Station Forces, Kingston, Ontario K7K 7B4, Verrall, R A, He, Z, & Mouris, J F. First principles Candu fuel model and validation experimentation. United States.
Corcoran, E C, Kaye, M H, Lewis, B J, Thompson, W T, Akbari, F, Royal Military College of Canada, Department of Chemistry and Chemical Engineering, P.O. Box 17000 Station Forces, Kingston, Ontario K7K 7B4, Higgs, J D, Royal Military College of Canada, Department of Chemistry and Chemical Engineering, P.O. Box 17000 Station Forces, Kingston, Ontario K7K 7B4, Verrall, R A, He, Z, and Mouris, J F. Sun . "First principles Candu fuel model and validation experimentation". United States.
@article{osti_21229268,
title = {First principles Candu fuel model and validation experimentation},
author = {Corcoran, E C and Kaye, M H and Lewis, B J and Thompson, W T and Akbari, F and Royal Military College of Canada, Department of Chemistry and Chemical Engineering, P.O. Box 17000 Station Forces, Kingston, Ontario K7K 7B4 and Higgs, J D and Royal Military College of Canada, Department of Chemistry and Chemical Engineering, P.O. Box 17000 Station Forces, Kingston, Ontario K7K 7B4 and Verrall, R A and He, Z and Mouris, J F},
abstractNote = {Many modeling projects on nuclear fuel rest on a quantitative understanding of the co-existing phases at various stages of burnup. Since the various fission products have considerably different abilities to chemically associate with oxygen, and the O/M ratio is slowly changing as well, the chemical potential (generally expressed as an equivalent oxygen partial pressure) is a function of burnup. Concurrently, well-recognized small fractions of new phases such as inert gas, noble metals, zirconates, etc. also develop. To further complicate matters, the dominant UO{sub 2} fuel phase may be non-stoichiometric and most of minor phases have a variable composition dependent on temperature and possible contact with the coolant in the event of a sheathing defect. A Thermodynamic Fuel Model to predict the phases in partially burned Candu nuclear fuel containing many major fission products has been under development. This model is capable of handling non-stoichiometry in the UO{sub 2} fluorite phase, dilute solution behaviour of significant solute oxides, noble metal inclusions, a second metal solid solution U(Pd-Rh-Ru)3, zirconate and uranate solutions as well as other minor solid phases, and volatile gaseous species. The treatment is a melding of several thermodynamic modeling projects dealing with isolated aspects of this important multi-component system. To simplify the computations, the number of elements has been limited to twenty major representative fission products known to appear in spent fuel. The proportion of elements must first be generated using SCALES-5. Oxygen is inferred from the concentration of the other elements. Provision to study the disposition of very minor fission products is included within the general treatment but these are introduced only on an as needed basis for a particular purpose. The building blocks of the model are the standard Gibbs energies of formation of the many possible compounds expressed as a function of temperature. To these data are added mixing terms associated with the appearance of the component species in particular phases. To validate the model, coulometric titration experiments relating the chemical potential of oxygen to the moles of oxygen introduced to SIMFUEL are underway. A description of the apparatus to oxidize and reduce samples in a controlled way in a H{sub 2}/H{sub 2}O mixture is presented. Existing measurements for irradiated fuel, both defected and non-defected, are also being incorporated into the validation process. (authors)},
doi = {},
journal = {},
number = ,
volume = ,
place = {United States},
year = {2007},
month = {7}
}

Conference:
Other availability
Please see Document Availability for additional information on obtaining the full-text document. Library patrons may search WorldCat to identify libraries that hold this conference proceeding.

Save / Share: