Examination of long-stored uranium metal
A small quantity of unirradiated uranium from Magnox fuel elements is currently held in archive storage. Some of these samples date back to the late fifties. This material has been stored, untreated, in unsealed containers in air at ambient temperature, humidity and pressure conditions. Such conditions are relevant to those that may exist in a passive storage facility. A sample of this material has been subject to optical, electron-optical and Raman spectroscopic examination to determine the extent of corrosion and the composition of corrosion product arising from long-term, low-temperature oxidation of uranium metal in air. The examinations have established that, even after a period in excess of 40 years, there was no observable spalling of uranium oxide from the sample during storage. The extent of oxidation of the metal, derived by SEM analysis, was slight and insignificant in relation to overall structural stability of the material. Raman spectroscopy data showed that the bulk of the oxide layer was comprised of hyper-stoichiometric UO{sub 2}, with U{sub 4}O{sub 9} being the dominant component. The oxygen/uranium ratio was observed to be decreased at the metal/oxide interface, with a very thin layer that consisted of mainly UO{sub 2} at the metal surface. At the oxide/air interface, a very thin U{sub 3}O{sub 8} layer was detected. U{sub 4}O{sub 9} is relatively mechanically stable, due to a significantly higher density than UO{sub 2} and U{sub 3}O{sub 8}. It is likely that the lower internal stresses in the thick U{sub 4}O{sub 9} layer have resulted in less oxide film cracking than would be expected from UO{sub 2} or U{sub 3}O{sub 8} and hence the low oxidation rate observed. These results suggest that storage of uranium metal in air over decades is a safe and credible option. (authors)