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Title: Understanding the Stability of Salt-Inclusion Phases for Nuclear Waste-forms through Volume-based Thermodynamics

Abstract

Formation enthalpies and Gibbs energies of actinide and rare-earth containing SIMs with silicate and germanate frameworks are reported. Volume-based thermodynamics (VBT) techniques complemented by density functional theory (DFT) were adapted and applied to these complex structures. VBT and DFT results were in closest agreement for the smaller framework silicate structure, whereas DFT in general predicts less negative enthalpies across all SIMs, regardless of framework type. Both methods predict the rare-earth silicates to be the most stable of the comparable structures calculated, with VBT results being in good agreement with the limited experimental values available from drop solution calorimetry.

Authors:
; ; ; ; ; ; ;
Publication Date:
Research Org.:
Univ. of South Carolina, Columbia, SC (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Scientific User Facilities Division
OSTI Identifier:
1483656
Alternate Identifier(s):
OSTI ID: 1483648; OSTI ID: 1483649
Grant/Contract Number:  
SC0016574
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Scientific Reports
Additional Journal Information:
Journal Volume: 8; Journal Issue: 1; Journal ID: ISSN 2045-2322
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY

Citation Formats

Moore, Emily E., Kocevski, Vancho, Juillerat, Christian A., Morrison, Gregory, Zhao, Mingyang, Brinkman, Kyle S., zur Loye, Hans-Conrad, and Besmann, Theodore M. Understanding the Stability of Salt-Inclusion Phases for Nuclear Waste-forms through Volume-based Thermodynamics. United States: N. p., 2018. Web. doi:10.1038/s41598-018-32903-3.
Moore, Emily E., Kocevski, Vancho, Juillerat, Christian A., Morrison, Gregory, Zhao, Mingyang, Brinkman, Kyle S., zur Loye, Hans-Conrad, & Besmann, Theodore M. Understanding the Stability of Salt-Inclusion Phases for Nuclear Waste-forms through Volume-based Thermodynamics. United States. doi:10.1038/s41598-018-32903-3.
Moore, Emily E., Kocevski, Vancho, Juillerat, Christian A., Morrison, Gregory, Zhao, Mingyang, Brinkman, Kyle S., zur Loye, Hans-Conrad, and Besmann, Theodore M. Wed . "Understanding the Stability of Salt-Inclusion Phases for Nuclear Waste-forms through Volume-based Thermodynamics". United States. doi:10.1038/s41598-018-32903-3. https://www.osti.gov/servlets/purl/1483656.
@article{osti_1483656,
title = {Understanding the Stability of Salt-Inclusion Phases for Nuclear Waste-forms through Volume-based Thermodynamics},
author = {Moore, Emily E. and Kocevski, Vancho and Juillerat, Christian A. and Morrison, Gregory and Zhao, Mingyang and Brinkman, Kyle S. and zur Loye, Hans-Conrad and Besmann, Theodore M.},
abstractNote = {Formation enthalpies and Gibbs energies of actinide and rare-earth containing SIMs with silicate and germanate frameworks are reported. Volume-based thermodynamics (VBT) techniques complemented by density functional theory (DFT) were adapted and applied to these complex structures. VBT and DFT results were in closest agreement for the smaller framework silicate structure, whereas DFT in general predicts less negative enthalpies across all SIMs, regardless of framework type. Both methods predict the rare-earth silicates to be the most stable of the comparable structures calculated, with VBT results being in good agreement with the limited experimental values available from drop solution calorimetry.},
doi = {10.1038/s41598-018-32903-3},
journal = {Scientific Reports},
number = 1,
volume = 8,
place = {United States},
year = {Wed Oct 17 00:00:00 EDT 2018},
month = {Wed Oct 17 00:00:00 EDT 2018}
}

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Works referenced in this record:

Projector augmented-wave method
journal, December 1994


Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
journal, July 1996


Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996


From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999