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Search for higher oxides of Pu: A photoemission study
Authors:T. Gouder  A. Seibert  J. Rebizant
Affiliation:a European Commission, Joint Research Centre, Institute for Transuranium Elements, Postfach 2340, 76125 Karlsruhe, Germany
b Charles University, Faculty of Mathematics and Physics, Department of Condensed Matter Physics, Ke Karlovu 5, 121 16 Prague 2, Czech Republic
Abstract:
After decades of believing in a very stable PuO2, suitable for final storage of nuclear waste, the existence of a higher oxide, PuO2+x, was recently claimed. This would have far reaching consequences on the strategies of storage of Pu-based waste. Its formation therefore has been discussed controversially for several years.In this work, existence and stability of the higher oxide, PuO2+x, has been probed by photoelectron spectroscopy study of PuO2 exposed to atomic oxygen. The validity of this approach is first tested on UO2, which oxidizes readily to UO3. Under the same reaction conditions, PuO2 is only covered by a chemisorbed layer of oxygen, which desorbs at elevated temperature. The study excludes the stability of any higher binary Pu oxide as a bulk species.
Keywords:Uranium   Plutonium   Oxidation   Corrosion   Chemisorption   Photoelectron emission
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