Thermodynamic Properties of UO2, as Predicted by the New Equation of State

This chapter contains the description of the eventually recommended equation of state for uranium oxide, called here INTAS-99-EOS, as expressed in terms of models and sub-models presented in the previous Chapters. In the frame of the chemical model approach, this equation probably represents the most comprehensive EOS of UO2±x, affordable by optimal use of the presently available theoretical tools and experimental databases. The equation is of a MIX type, as sketched in Chapter 2; the details of its structure are explained and discussed in Chapters 3 to 6. After a recapitulation of the fundamental hypotheses and a summary of the main features, this Chapter is dedicated to the presentation of an extensive set of numerical calculations and to the comparison with predictions of alternative models.

[1]  C. F. Curtiss,et al.  Molecular Theory Of Gases And Liquids , 1954 .

[2]  L. Verlet,et al.  Perturbation Theory and Equation of State for Fluids , 1969 .

[3]  P. Fowler,et al.  The polarizabilities and dispersion coefficients for ions in the solid group IV oxides , 1994 .

[4]  Neil W. Ashcroft,et al.  Structure and Resistivity of Liquid Metals , 1966 .

[5]  H. Reiss Refined Theory of Ion Pairing. I. Equilibrium Aspects , 1956 .

[6]  S. Shenker,et al.  Equation of State for Dense Gases , 1971 .

[7]  E. Rudnyi,et al.  The electron affinity of UO3 , 1992 .

[8]  I. J. Fritz Elastic properties of UO2 at high pressure , 1976 .

[9]  M. G. Chasanov,et al.  Total pressure of uranium-bearing species over molten urania☆ , 1972 .

[10]  C. Alcock,et al.  Thermodynamic Properties of Individual Substances , 1994 .

[11]  A. R. Hall Elastic moduli and internal friction of some uranium ceramics , 1970 .

[12]  L. Verlet,et al.  Perturbation theory for the thermodynamic properties of simple liquids , 1972 .

[13]  A. Adamson Physical chemistry of surfaces , 1960 .

[14]  M. Wertheim,et al.  EXACT SOLUTION OF THE PERCUS-YEVICK INTEGRAL EQUATION FOR HARD SPHERES , 1963 .

[15]  Redlich-Kwong equation of state for the fast breeder oxide fuel UO2 , 1982 .

[16]  Ye,et al.  Mean spherical approximation for a simple model of electrolytes. II. Correlation functions and thermodynamics: Numerical results , 1988 .

[17]  F. Firk,et al.  Energy Spectrum of Photoneutrons from the Reaction O 16 (γ,n)O 15 , 1962 .

[18]  W. Ebeling,et al.  Physics of Nonideal Plasmas , 1992 .

[19]  J. Hansen,et al.  Statistical mechanics of simple coulomb systems , 1980 .

[20]  Keith E. Gubbins,et al.  Theory of molecular fluids , 1984 .

[21]  E. A. Fischer A New Evaluation of the Urania Equation of State Based on Recent Vapor Pressure Measurements , 1989 .

[22]  B. Larsen Studies in statistical mechanics of Coulombic systems. I. Equation of state for the restricted primitive model , 1976 .

[23]  J. K. Fink,et al.  Thermophysical properties of uranium dioxide , 2000 .

[24]  J. B. Conway,et al.  High‐Temperature Enthalpy and Heat of Fusion of UO2 , 1968 .

[25]  I. Barin Thermochemical data of pure substances , 1989 .

[26]  Ivo Nezbeda,et al.  Statistical thermodynamics of simple liquids and their mixtures , 1980 .

[27]  L. Mistura,et al.  A perturbed hard core equation of state for oxide nuclear fuels , 1985 .

[28]  Leonard Leibowitz,et al.  Equation of state of uranium dioxide , 1979 .

[29]  M. O'Keeffe,et al.  Ionic conductivity of some alkaline earth halides , 1975 .

[30]  M. Gillan,et al.  A molecular dynamics study of solid and liquid UO2 , 1988 .

[31]  E. A. Fischer,et al.  Critical assessment of equation of state data for UO2 , 1976 .

[32]  Christine Guéneau,et al.  Thermodynamic assessment of the uranium–oxygen system , 2002 .

[33]  M. Born,et al.  Dynamische Gittertheorie der Kristalle , 1933 .

[34]  E. A. Mason,et al.  The virial equation of state , 1969 .

[35]  I. Iosilevski,et al.  Phase Transition in Simplest Plasma Models , 2006, 0902.2353.

[36]  Koji Morita,et al.  Thermodynamic properties and equations of state for fast reactor safety analysis: Part II: Properties of fast reactor materials , 1998 .

[37]  R. F. Strickland-Constable Chemical Phase Theory , 1958 .

[38]  C. Ronchi,et al.  Laboratory Measurement of the Heat Capacity of Urania up to 8000 K: I. Experiment , 1993 .

[39]  J. Lebowitz,et al.  Thermodynamic Properties of Mixtures of Hard Spheres , 1964 .

[40]  J. Bates,et al.  Elastic constants of single crystal UO2 at 25° C , 1965 .

[41]  M. G. Chasanov,et al.  Enthalpy of liquid uranium dioxide to 3500 °K☆ , 1971 .

[42]  J. Lebowitz,et al.  Sphericalization of nonspherical interactions , 1983 .

[43]  J. Lewis,et al.  Thermodynamic properties and self-diffusion of molten sodium chloride. A molecular dynamics study , 1975 .

[44]  John S. Rowlinson,et al.  On the Continuity of the Gaseous and Liquid States , 2004 .

[45]  R. Peierls,et al.  Zur Theorie des Diamagnetismus von Leitungselektronen , 1933 .

[46]  M. Bober,et al.  Vapor pressure determination of liquid UO/sub 2/ using a boiling point technique , 1987 .

[47]  R. J. Baxter,et al.  Ornstein–Zernike Relation and Percus–Yevick Approximation for Fluid Mixtures , 1970 .

[48]  E. Thiele Comparison of the Classical Theories of Unimolecular Reactions. II. A Model Calculation , 1963 .

[49]  A. Panagiotopoulos Molecular simulation of phase equilibria: simple, ionic and polymeric fluids , 1992 .

[50]  Computer simulation of highly compressed molecular hydrogen , 2001 .

[51]  C. D. Novion,et al.  Constantes elastiques des carbures, nitrures et oxydes d'uranium et de plutonium , 1969 .

[52]  O. D. Slagle,et al.  Compressibility of molten UO2 , 1971 .

[53]  K. E. Starling,et al.  Equilibrium Thermodynamic Properties of the Mixture of Hard Spheres , 1971 .

[54]  M. G. Chasanov,et al.  Enthalpy of solid uranium dioxide from 2500 °K to its melting point , 1969 .

[55]  Juan J. Carbajo,et al.  A review of the thermophysical properties of MOX and UO , 2001 .

[56]  Kurt Binder,et al.  A Guide to Monte Carlo Simulations in Statistical Physics , 2000 .

[57]  M. Tribus Thermostatics and thermodynamics , 1961 .

[58]  P. Blackburn Oxygen pressures over fast breeder reactor fuel (I) A model for UO2±x☆ , 1973 .

[59]  Joseph O. Hirschfelder,et al.  Contribution of Bound, Metastable, and Free Molecules to the Second Virial Coefficient and Some Properties of Double Molecules , 1959 .

[60]  M. Gillan Liquid-vapour equilibrium in the restricted primitive model for ionic liquids , 1983 .

[61]  K. E. Starling,et al.  Equation of State for Nonattracting Rigid Spheres , 1969 .

[62]  J. Lebowitz,et al.  Mean Spherical Model Integral Equation for Charged Hard Spheres I. Method of Solution , 1972 .

[63]  E. Yakub Integral equations for conventional correlation functions of simple dimerizing fluids , 1992 .

[64]  Martin Steinbrück,et al.  Core Loss during a Severe Accident (COLOSS). , 2003 .

[65]  N. Pyper,et al.  Studies in multiconfiguration Dirac–Fock theory. Part 3.—Interpretation of the electronic structure of neutral and ionized states of uranium , 1978 .

[66]  S. Yamanaka,et al.  Molecular dynamics study of mixed oxide fuel , 2001 .

[67]  B. Cheynet,et al.  Progress in the thermodynamic modelling of the O–U binary system , 2002 .

[68]  Hiroshi Iyetomi,et al.  Statistical physics of dense plasmas: Thermodynamics, transport coefficients and dynamic correlations , 1987 .

[69]  V. V. Sychev,et al.  Thermodynamic Properties of Methane , 1987 .

[70]  K. Pitzer,et al.  The restricted primitive model for ionic fluids , 1987 .

[71]  B. Guillot,et al.  Coexisting phases and criticality in NaCl by computer simulation , 1994 .

[72]  J. Sengers,et al.  Critical fluctuations and the equation of state of Van der Waals , 2004 .

[73]  S. K. Kapil Evaluation of the thermodynamic critical constants for uranium di-oxide , 1976 .

[74]  W. Ebeling,et al.  Quantum statistics of coulomb systems: Thermodynamic functions and phase transitions , 1986 .

[75]  Kazuhiro Yamada,et al.  Evaluation of thermal properties of uranium dioxide by molecular dynamics , 2000 .

[76]  W. Ebeling,et al.  An Analytical Calculation of the Equation of State and the Critical Point in a Dense Classical Fluid of Charged Hard Spheres , 1980 .

[77]  M. Tetenbaum,et al.  Total pressure of uranium-bearing species over oxygen-deficient urania☆ , 1970 .

[78]  H. S. Kamath,et al.  Classical molecular dynamics simulation of UO2 to predict thermophysical properties , 2003 .

[79]  R. W. Ohse High‐Temperature Vapor‐Pressure Studies of UO2 by the Effusion Method and Its Thermodynamic Interpretation , 1966 .

[80]  J. Barker,et al.  Perturbation Theory and Equation of State for Fluids. II. A Successful Theory of Liquids , 1967 .

[81]  R. Reid,et al.  The Properties of Gases and Liquids , 1977 .

[82]  W. Ebeling,et al.  Theory of bound states and ionization equilibrium in plasmas and solids , 1976 .

[83]  H. C. Andersen,et al.  Role of Repulsive Forces in Determining the Equilibrium Structure of Simple Liquids , 1971 .

[84]  D. A. Young Thermodynamics of nuclear materials International atomic energy agency, Vienna, proceedings series, 808 pages, 1962, 66s, $ 11.00, NF 44, DM 38.50 , 1963 .

[85]  J. A. Christensen THERMAL EXPANSION AND CHANGE IN VOLUME OF URANIUM DIOXIDE ON MELTING , 1963 .

[86]  K. Pitzer,et al.  Equation of State and Thermodynamic Properties of Gases at High Temperatures. I. Diatomic Molecules , 1959 .

[87]  E. A. Guggenheim Modern thermodynamics by the methods of Willard Gibbs , 1933 .