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

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:
Grant/Contract Number:
SC0016574
Type:
Accepted Manuscript
Journal Name:
Scientific Reports
Additional Journal Information:
Journal Volume: 8; Journal Issue: 1; Journal ID: ISSN 2045-2322
Publisher:
Nature Publishing Group
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
Country of Publication:
United States
Language:
English
Subject:
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY
OSTI Identifier:
1483656
Alternate Identifier(s):
OSTI ID: 1483648; OSTI ID: 1483649

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., 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.. 2018. "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 = {2018},
month = {10}
}

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