Differences in oxidation behavior of used CANDU fuel during prolonged storage in moisture-saturated air and dry air at 150 °C

In the Canadian research and development program on fuel storage, used CANDU (Canada deuterium uranium) UO[sub 2] fuel bundles are being exposed in experimental vessels to both dry and moisture-saturated air environments at 150 C. At intervals of several years, individual fuel elements, which were deliberately defected before storage, are recovered for destructive examination to determine the extent of UO[sub 2] oxidation that has occurred. The most recent examinations took place after 99.5 and 69 months of storage under dry and moist conditions, respectively. The progress of oxidation in the two different storage environments is compared, and the results of fuel examination by optical microscopy, scanning electron microscopy, X-ray photoelectron spectroscopy (XPS), and X-ray powder diffraction (XRD) are described. Interpretation of the results is complicated by the different O[sub 2]/UO[sub 2] ratios in the two types of storage vessel and the fact that oxygen was completely consumed during at least some of the storage intervals. Nonetheless, it is clear that the presence of moisture promotes a more generally distributed oxidation of UO[sub 2] grain boundaries. The probably involvement of radiolytic processes in the moist oxidation reaction and possible reasons for the sensitization of certain regions of the fuel to moistmore » oxidation are discussed. In addition to oxidation of UO[sub 2], the XPS spectra provide evidence for the radiation-induced incorporation of oxygen and nitrogen into adventitious carbon (adsorbed hydrocarbons) on the UO[sub 2] surfaces.« less

[1]  P. Taylor,et al.  Crystallization of U3O8 and hydrated UO3 on UO2 fuel in aerated water near 200°C☆ , 1991 .

[2]  G. López,et al.  XPS O 1s binding energies for polymers containing hydroxyl, ether, ketone and ester groups , 1991 .

[3]  S. Sunder,et al.  XPS studies of UO2 oxidation by alpha radiolysis of water at 100°C☆ , 1990 .

[4]  Concentration profiles of neutron-induced radioactivities in UO2 fuel specimens , 1990 .

[5]  Peter Taylor,et al.  Formation of uranium trioxide hydrates on UO2 fuel in air-steam mixtures near 200°C☆ , 1989 .

[6]  F. Doern,et al.  X‐ray photoelectron spectroscopy on radioactive materials using a McPherson ESCA‐36 equipped with an SSL position‐sensitive detector , 1989 .

[7]  L. E. Thomas,et al.  Microstructural examination of oxidized spent PWR fuel by transmission electron microscopy , 1989 .

[8]  B. J. Wrona,et al.  Oxidation Behavior of Nonirradiated UO2 , 1989 .

[9]  B. J. Wrona,et al.  Oxidation behavior of spent UO/sub 2/ fuel , 1989 .

[10]  David W. Shoesmith,et al.  The corrosion of nuclear fuel (UO2) in oxygenated solutions , 1991 .

[11]  W. H. Hocking,et al.  Corrosion of stellite-6 in lithiated and borated high-temperature water , 1988 .

[12]  G. C. Allen,et al.  Oxidation of crystalline UO2 studied using X-ray photoelectron spectroscopy and X-ray diffraction , 1987 .

[13]  Hansjoachim Matzke,et al.  Atomic transport properties in UO2 and mixed oxides (U, Pu)O2 , 1987 .

[14]  I. J. Hastings,et al.  Air Oxidation of UO2 Fuel Fragments at 175° to 400°C , 1986 .

[15]  Ian J. Hastings,et al.  Postirradiation behavior of UO2 fuel I: elements at 220 to 250°C in air , 1983 .

[16]  F. A. Johnson,et al.  The diffusion coefficients of gaseous and volatile species during the irradiation of uranium dioxide , 1982 .

[17]  M. G. Bailey,et al.  Anodic oxidation of UO2 , 1981 .

[18]  N. McIntyre,et al.  Chemical information from XPS—applications to the analysis of electrode surfaces , 1981 .

[19]  P. Taylor,et al.  An X-ray diffraction study of the formation of β-UO2.33 on UO2 pellet surfaces in air at 229 to 275°C , 1980 .

[20]  M. Notley,et al.  Irradiation-induced volume changes in commercial UO2 fuel: Comparison with model prediction , 1978 .

[21]  T. Vandergraaf,et al.  The Canadian Spent Fuel Storage Canister: Some Materials Aspects , 1977 .

[22]  S. Macewen,et al.  A model for in-reactor densification of UO2 , 1975 .

[23]  I. Cohen,et al.  A metallographic and X-ray study of the limits of oxygen solubility in the UO2-ThO2 system , 1966 .

[24]  D. Walker THE OXIDATION OF URANIUM DIOXIDES , 1965 .

[25]  H. Hoekstra,et al.  The low temperature oxidation of UO2 and U4O9 , 1961 .

[26]  A. R. Jones,et al.  Radiation-induced reactions in the N2-O2-H2O system. , 1959, Radiation research.

[27]  S. Aronson,et al.  Kinetic Study of the Oxidation of Uranium Dioxide , 1957 .