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research article

Hydrogen trapping in delta-Pu: insights from electronic structure calculations

Taylor, Christopher D.
•
Hernandez, Sarah C.
•
Francis, Michael F.
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2013
Journal of Physics: Condensed Matter

Density functional theory calculations have been performed to provide details of the structural and charge-transfer details related to the solid solution of hydrogen in (delta)-plutonium. We follow the Flanagan model that outlines the process by which hydrogen interacts with a metal to produce hydride phases, via a sequence of surface, interstitial and defect-bound (trapped) states. Due to the complexities of the electronic structure in plutonium solid-state systems, we take the pragmatic approach of adopting the 'special quasirandom structure' to disperse the atomic magnetic moments. We find that this approach produces sound structural and thermodynamic properties in agreement with the available experimental data. In delta-Pu, hydrogen has an exothermic binding energy to all of the states relevant in the Flanagan model, and, furthermore, is anionic in all these states. The charge transfer is maximized (i.e. most negative for hydrogen) in the hydride phase. The pathway from surface to hydride is sequentially exothermic, in the order surface < interstitial < grain boundary < vacancy < hydride (hydride being the most exothermic state). Thus, we find that there is no intermediate state that involves an endothermic increase in energy, consistent with the general experimental observations that the hydriding reaction in plutonium metal can proceed with zero apparent activation barrier.

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Type
research article
DOI
10.1088/0953-8984/25/26/265001
Web of Science ID

WOS:000320329400002

Author(s)
Taylor, Christopher D.
Hernandez, Sarah C.
Francis, Michael F.
Schwartz, Daniel S.
Ray, Asok K.
Date Issued

2013

Publisher

Iop Publishing Ltd

Published in
Journal of Physics: Condensed Matter
Volume

25

Issue

26

Article Number

265001

Editorial or Peer reviewed

REVIEWED

Written at

OTHER

EPFL units
LAMMM  
Available on Infoscience
October 1, 2013
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/95763
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