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Title: Temperature-Dependent Properties of Molten Li2BeF4Salt Using Ab Initio Molecular Dynamics

Abstract

Molten lithium tetrafluoroberyllate (Li2BeF4) salt, also known as FLiBe, with a 2:1 mixture of LiF and BeF2 is being proposed as a coolant and solvent in advanced nuclear reactor designs, such as the molten salt reactor or the fluoride salt cooled high-temperature reactor. We present the results on the structure and properties of FLiBe over a wide range of temperatures, 0–2000 K, from high-throughput ab initio molecular dynamics simulation using a supercell model of 504 atoms. The variations in the local structures of solid and liquid FLiBe with temperature are discussed in terms of a pair distribution function, coordination number, and bond angle distribution. The temperature-dependent electronic structure and optical and mechanical properties of FLiBe are calculated. The optical and mechanical property results are reported for the first time. The results above and below the melting temperature (~732 K) are compared with the experimental data and with data for crystalline FLiBe. The electronic structure and interatomic bonding results are discussed in correlation with the mechanical strength. A novel concept of total bond order density (TBOD), an important quantum mechanical parameter, is used to characterize the internal cohesion and strength in the simulated models. The results show a variation in themore » rate of change in properties in solid and liquid phases with anomalous behavior across the melting region. The observed trend is the decrease in mechanical strength, band gap, and TBOD in a nonlinear fashion as a function of temperature. The refractive index shows a surprising minimum at 850 K, among the tested temperatures, which lies above the melting point. These findings provide a new platform to understand the interplay between the temperature-dependent structures and properties of FLiBe salt.« less

Authors:
 [1]; ORCiD logo [1];  [2];  [3];  [3]; ORCiD logo [1]
+ Show Author Affiliations
  1. Univ. of Missouri, Kansas City, MO (United States)
  2. Missouri State University, Springfield, MO (United States)
  3. Univ. of Wisconsin, Madison, WI (United States)
Publication Date:
Research Org.:
University of California, Berkeley, CA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1816529
Grant/Contract Number:  
AC03-76SF00098
Resource Type:
Accepted Manuscript
Journal Name:
ACS Omega
Additional Journal Information:
Journal Volume: 6; Journal Issue: 30; Journal ID: ISSN 2470-1343
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; crystals; electronic structure; ions; liquids; salts

Citation Formats

Baral, Khagendra, San, Saro, Sakidja, Ridwan, Couet, Adrien, Sridharan, Kumar, and Ching, Wai-Yim. Temperature-Dependent Properties of Molten Li2BeF4Salt Using Ab Initio Molecular Dynamics. United States: N. p., 2021. Web. doi:10.1021/acsomega.1c02528.
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Baral, Khagendra, San, Saro, Sakidja, Ridwan, Couet, Adrien, Sridharan, Kumar, & Ching, Wai-Yim. Temperature-Dependent Properties of Molten Li2BeF4Salt Using Ab Initio Molecular Dynamics. United States. https://doi.org/10.1021/acsomega.1c02528
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Baral, Khagendra, San, Saro, Sakidja, Ridwan, Couet, Adrien, Sridharan, Kumar, and Ching, Wai-Yim. Wed . "Temperature-Dependent Properties of Molten Li2BeF4Salt Using Ab Initio Molecular Dynamics". United States. https://doi.org/10.1021/acsomega.1c02528. https://www.osti.gov/servlets/purl/1816529.
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@article{osti_1816529,
title = {Temperature-Dependent Properties of Molten Li2BeF4Salt Using Ab Initio Molecular Dynamics},
author = {Baral, Khagendra and San, Saro and Sakidja, Ridwan and Couet, Adrien and Sridharan, Kumar and Ching, Wai-Yim},
abstractNote = {Molten lithium tetrafluoroberyllate (Li2BeF4) salt, also known as FLiBe, with a 2:1 mixture of LiF and BeF2 is being proposed as a coolant and solvent in advanced nuclear reactor designs, such as the molten salt reactor or the fluoride salt cooled high-temperature reactor. We present the results on the structure and properties of FLiBe over a wide range of temperatures, 0–2000 K, from high-throughput ab initio molecular dynamics simulation using a supercell model of 504 atoms. The variations in the local structures of solid and liquid FLiBe with temperature are discussed in terms of a pair distribution function, coordination number, and bond angle distribution. The temperature-dependent electronic structure and optical and mechanical properties of FLiBe are calculated. The optical and mechanical property results are reported for the first time. The results above and below the melting temperature (~732 K) are compared with the experimental data and with data for crystalline FLiBe. The electronic structure and interatomic bonding results are discussed in correlation with the mechanical strength. A novel concept of total bond order density (TBOD), an important quantum mechanical parameter, is used to characterize the internal cohesion and strength in the simulated models. The results show a variation in the rate of change in properties in solid and liquid phases with anomalous behavior across the melting region. The observed trend is the decrease in mechanical strength, band gap, and TBOD in a nonlinear fashion as a function of temperature. The refractive index shows a surprising minimum at 850 K, among the tested temperatures, which lies above the melting point. These findings provide a new platform to understand the interplay between the temperature-dependent structures and properties of FLiBe salt.},
doi = {10.1021/acsomega.1c02528},
journal = {ACS Omega},
number = 30,
volume = 6,
place = {United States},
year = {Wed Jul 21 00:00:00 EDT 2021},
month = {Wed Jul 21 00:00:00 EDT 2021}
}
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