The thermodynamics of hydride precipitation: the importance of entropy, enthalpy and disorder
File(s)Lumley_manuscript_Acta.pdf (1.66 MB)
Accepted version
Author(s)
Type
Journal Article
Abstract
The precipitation of zirconium hydrides from Zr solid solution was investigated using first-principles lattice dynamics simulations. These included the temperature-dependent vibrational enthalpy and vibrational entropy combined with the configurational entropy terms. In contrast with previous approaches, it was found that the latent enthalpy alone is not sufficient to fully describe precipitation of hydrides; a full thermodynamic assessment is required. In particular, the vibrational enthalpy of precipitation assists in stabilizing hexagonal close-packed hydrides and is especially important in forming the metastable zeta phase. The configurational entropy change during precipitation favours face-centred cubic hydrides. Given this, at concentrations below 300 ppm H, no hydride precipitation is predicted, suggesting that when hydrides are seen in those materials it is because the local concentration of H is greater than that measured globally. While gamma hydride is the most stable phase, it is very close in energy to the delta phase.
Date Issued
2014-10-15
Date Acceptance
2014-07-10
Citation
Acta Materialia, 2014, 79 (1), pp.351-362
ISSN
1359-6454
Publisher
Elsevier
Start Page
351
End Page
362
Journal / Book Title
Acta Materialia
Volume
79
Issue
1
Copyright Statement
© 2014 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved. NOTICE: this is the author’s version of a work that was accepted for publication in Acta Materialia. Changes resulting from the publishing process, such as peer review, editing, corrections, structural formatting, and other quality control mechanisms may not be reflected in this document. Changes may have been made to this work since it was submitted for publication. A definitive version was subsequently published in ACTA MATERIALIA, Vol.: 79, (2014) DOI: 10.1016/j.actamat.2014.07.019
Identifier
http://gateway.webofknowledge.com/gateway/Gateway.cgi?GWVersion=2&SrcApp=PARTNER_APP&SrcAuth=LinksAMR&KeyUT=WOS:000342718400034&DestLinkType=FullRecord&DestApp=ALL_WOS&UsrCustomerID=1ba7043ffcc86c417c072aa74d649202
Subjects
Science & Technology
Technology
Materials Science, Multidisciplinary
Metallurgy & Metallurgical Engineering
Materials Science
Zirconium hydride
Thermodynamics
Density functional theory
Precipitation
ZIRCONIUM HYDRIDE
AB-INITIO
HYDROGEN
ZIRCALOY-2
EMBRITTLEMENT
SOLUBILITY
STABILITY
DIFFUSION
PHASES
SYSTEM
Publication Status
Published
Date Publish Online
2014-08-16