AVS 65th International Symposium & Exhibition
    Actinides and Rare Earths Focus Topic Thursday Sessions
       Session AC+AS+SA-ThM

Paper AC+AS+SA-ThM11
Comparison of the Oxidation Rates for Alpha Versus Delta Plutonium by X-ray Photoelectron Spectroscopy

Thursday, October 25, 2018, 11:20 am, Room 202C

Session: Nuclear Power, Forensics, and Other Applications
Presenter: Art Nelson, Lawrence Livermore National Laboratory
Authors: A.J. Nelson, Lawrence Livermore National Laboratory
S.B. Donald, Lawrence Livermore National Laboratory
D.J. Roberts, Lawrence Livermore National Laboratory
W. McLean, Lawrence Livermore National Laboratory
Correspondent: Click to Email

X-ray photoemission spectroscopy (XPS) was used to characterize differences in the oxidation rates for polycrystalline α-Pu versus δ-Pu related to variations in grain size and surface electronic structure. The evolution of the Pu 4f core-level chemical shift as a function of oxygen exposure at ambient temperature was quantified in oxidation profiles. In addition, the X-ray excited Pu NOO Auger line-shapes were combined with the chemical shift of the Pu 4f7/2 photoelectron line that defines the Auger parameter and results in a reliable method for determining oxidation states independent of binding energy calibration. The oxidation profiles reveal that α-Pu oxidizes faster than δ-Pu, both resulting in the PuO2/Pu2O3/Pu oxide structure. This data was used to a produce chemical state (Wagner) plot for select plutonium oxides.

This work was performed under the auspices of the U.S. Dept. of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344.