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Pu-Bearing Materials - From Fundamental Science To Storage Standards

Published online by Cambridge University Press:  01 February 2011

Shiu-Wing Tam  and
Yung Liu
Shiu-Wing Tam
Affiliation:
tam@anl.gov, Argonne National Laboratory, Decision & Information Sciences Div., 9700 S. Cass Avenue, Bldg. 900, MS-12, Argonne, IL, 60439, United States, 630-252-6602, 630-252-5715
Yung Liu
Affiliation:
yyliu@anl.gov, Argonne National Laboratory, Decision & Information Sciences Div., 9700 S. Cass Avenue, Bldg. 900, MS-12, Argonne, IL, 60439, United States
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Abstract

The behavior of plutonium (Pu) oxides in the presence of water/moisture in a confined space and the associated issues of hydrogen and oxygen generation due to radiolysis have important implications for the storage and transportation of Pu-bearing materials. This paper reviews the results of recent studies of gas generation in the Pu-O-H system, including the determination of release rates via engineering-scale measurement. The observations of the significant differences in gas generation behavior between “pure” Pu-bearing materials and those that contain salt impurities are addressed. In conjunction with the discussion of these empirical observations, the work also addresses recent scientific advances in the investigations of the Pu-O-H system using state-of-the-art ab initio electronic structure calculations, as well as advanced synchrotron techniques to determine the electronic structure of the various Pu-containing phases. The role of oxidizing species such as the hydroxyl radical from the radiolysis of water is examined. Discussed also is the challenge in the predictive ab-initio calculations of the electronic structure of the Pu-H-O system, due to the nature of the 5f valence electrons in Pu. Coupled with the continuing material surveillance program, it is anticipated that this work may help determine the electronic structure of the various Pu-containing phases and the role of impurity salts on gas generation and the long-term stability of oxygen/hydrogen-containing plutonium oxides beyond PuO2.

Keywords

actinideelectronic structurestorage
Type
Research Article
Information
MRS Online Proceedings Library (OPL) , Volume 1104: Symposium NN – Actinides 2008—Basic Science, Applications and Technology , 2008 , 1104-NN03-08
Copyright
Copyright © Materials Research Society 2008

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