Surface Mediated Processes in the Interaction of Spent Fuel or {alpha}-doped UO{sub 2} with H{sub 2}
- Studsvik Nuclear AB, Nykoeping, 611 82 (Sweden)
- Nuclear Chemistry, Chalmers University of Technology, Goeteborg, 412 96 (Sweden)
In most deep disposal concepts, large amounts of hydrogen are expected to be produced by the anoxic corrosion of massive iron containers. At repository temperatures, hydrogen is quite inert and is not expected to contribute to the redox capacity of the deep groundwaters. In several recent works, a large impact of dissolved hydrogen on the dissolution of the LWR or MOX fuel and UO{sub 2}(s) doped with {sup 233}U or {sup 238}Pu has been observed. For hydrogen concentrations above a certain limit, the dissolution rates of these highly radioactive materials drop to very low values. A discussion of the results obtained with spent fuel or {alpha}-doped UO{sub 2} in the presence of a range of hydrogen concentrations is presented. Typical for all measurements under such conditions are the very low long term concentrations of uranium and other redox-sensitive radionuclides, such as Tc and the minor actinides. The concentrations of U are systematically lower than the values measured during UO{sub 2}(s) solubility measurements carried out in the presence of strong reducing agents. Measurements of the radiolytic oxygen after long leaching periods result in values below detection limit. The investigation of the surface of spent fuel or UO{sub 2}(s) pellets doped with {sup 233}U by XPS after long periods of testing shows absence of oxidation. The kinetics of the release of non-redox sensitive elements such as Sr and Cs, used to estimate fuel matrix dissolution rates, is also discussed. An attempt is made to propose potential mechanisms responsible for the observed behaviour, based mainly on data from studies on the interaction of water adsorbed on the surfaces of metal oxides or actinide oxides with radiation. Another important effect observed in recent studies is the existence of a threshold for the specific alpha activity below which no measurable influence of the alpha radiolysis on the uranium release from UO{sub 2} is observed. The importance of such a threshold for the behaviour of spent fuel under repository conditions encompassing very long time scales will be discussed, as well as the necessity to better investigate the mechanisms of recombination reactions in a thin water layer on the surface of actinide oxides affected by {alpha}- radiolysis. (authors)
- Research Organization:
- Materials Research Society, 506 Keystone Drive, Warrendale, PA, 15086-7573 (United States)
- OSTI ID:
- 21091532
- Resource Relation:
- Conference: Symposium Actinides 2008 - Basic Science, Applications and Technology, San Francisco, CA (United States), 24-28 Mar 2008; Other Information: Country of input: France; 66 refs.; Full text available at: http://www.mrs.org/s{sub m}rs/bin.asp?CID=12409&DID=212468&DOC=FILE.PDF; Related Information: In: Proceedings of the symposium Actinides 2008 - Basic Science, Applications and Technology, by Chung, B.; Thompson, J.; Shuh, D.; Albrecht-Schmitt, T.; Gouder, T. (eds.), v. 1104, [260] pages.
- Country of Publication:
- United States
- Language:
- English
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Related Subjects
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY
CONTAINERS
CORROSION
DOPED MATERIALS
FUEL PELLETS
GROUND WATER
HYDROGEN
IRON
KINETICS
LEACHING
MIXED OXIDE FUELS
OXIDATION
PLUTONIUM 238
RADIOACTIVE MATERIALS
RADIOLYSIS
SPENT FUELS
SURFACES
URANIUM 233
URANIUM DIOXIDE
X-RAY PHOTOELECTRON SPECTROSCOPY