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Title: Carbon diffusion in molten uranium: an ab initio molecular dynamics study

Abstract

In this work we used ab initio molecular dynamics (AIMD) within the framework of density functional theory (DFT) and the projector-augmented wave (PAW) method to study carbon diffusion in liquid uranium at temperatures above 1600 K. The electronic interactions of carbon and uranium were described using the local density approximation (LDA). The self-diffusion of uranium based on this approach is compared with literature computational and experimental results for liquid uranium. The temperature dependence of carbon and uranium diffusion in the melt was evaluated by fitting the resulting diffusion coefficients to an Arrhenius relationship. We found that the LDA calculated activation energy for carbon was nearly twice that of uranium: 0.55±0.03 eV for carbon compared to 0.32±0.04 eV for uranium. Structural analysis of the liquid uranium-carbon system is also discussed.

Authors:
ORCiD logo; ; ; ; ; ;
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1438983
Report Number(s):
PNNL-SA-129429
Journal ID: ISSN 0965-0393
DOE Contract Number:
AC05-76RL01830
Resource Type:
Journal Article
Resource Relation:
Journal Name: Modelling and Simulation in Materials Science and Engineering; Journal Volume: 26; Journal Issue: 3
Country of Publication:
United States
Language:
English
Subject:
Molecular dynamics computer simulation; Nuclear Process Science Initiative; Density Functional Theory; Diffusion; Actinide Chemistry; trace impurities

Citation Formats

Garrett, Kerry E., Abrecht, David G., Kessler, Sean H., Henson, Neil J., Devanathan, Ram, Schwantes, Jon M., and Reilly, Dallas D. Carbon diffusion in molten uranium: an ab initio molecular dynamics study. United States: N. p., 2018. Web. doi:10.1088/1361-651X/aaad72.
Garrett, Kerry E., Abrecht, David G., Kessler, Sean H., Henson, Neil J., Devanathan, Ram, Schwantes, Jon M., & Reilly, Dallas D. Carbon diffusion in molten uranium: an ab initio molecular dynamics study. United States. doi:10.1088/1361-651X/aaad72.
Garrett, Kerry E., Abrecht, David G., Kessler, Sean H., Henson, Neil J., Devanathan, Ram, Schwantes, Jon M., and Reilly, Dallas D. Tue . "Carbon diffusion in molten uranium: an ab initio molecular dynamics study". United States. doi:10.1088/1361-651X/aaad72.
@article{osti_1438983,
title = {Carbon diffusion in molten uranium: an ab initio molecular dynamics study},
author = {Garrett, Kerry E. and Abrecht, David G. and Kessler, Sean H. and Henson, Neil J. and Devanathan, Ram and Schwantes, Jon M. and Reilly, Dallas D.},
abstractNote = {In this work we used ab initio molecular dynamics (AIMD) within the framework of density functional theory (DFT) and the projector-augmented wave (PAW) method to study carbon diffusion in liquid uranium at temperatures above 1600 K. The electronic interactions of carbon and uranium were described using the local density approximation (LDA). The self-diffusion of uranium based on this approach is compared with literature computational and experimental results for liquid uranium. The temperature dependence of carbon and uranium diffusion in the melt was evaluated by fitting the resulting diffusion coefficients to an Arrhenius relationship. We found that the LDA calculated activation energy for carbon was nearly twice that of uranium: 0.55±0.03 eV for carbon compared to 0.32±0.04 eV for uranium. Structural analysis of the liquid uranium-carbon system is also discussed.},
doi = {10.1088/1361-651X/aaad72},
journal = {Modelling and Simulation in Materials Science and Engineering},
number = 3,
volume = 26,
place = {United States},
year = {Tue Mar 06 00:00:00 EST 2018},
month = {Tue Mar 06 00:00:00 EST 2018}
}