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Title: Interactions and immobilization of lanthanides with dopants in uranium-based metallic fuels

Abstract

In uranium-based fuels, production and migration of lanthanide fission products and subsequent chemical interactions with cladding constituents lead to fuel–cladding chemical interaction (FCCI), limiting fuel performance. In general, dopant addition to the fuel matrix to arrest lanthanides within the fuel by forming intermetallics is found to be effective in mitigating FCCI. Recently, we proposed ab-initio based alloy-design principles, which can be useful in identifying dopant(s) that can bind a lanthanide (Nd) inside the fuel matrix. Here, we demonstrate the robustness of such principles by performing a systematic study to choose dopants to form compounds with a range of experimentally-observed lanthanide fission products. Results reveal that for a given dopant, lanthanide Ce and La exhibit similar behavior in their compound-forming tendencies compared to Nd and Pr, which is linked to lanthanide intrinsic characteristics such as the electronic configurations. Our predicted lanthanide-dopant intermetallic formation is verified experimentally in selective cases. Finally, we showed alloy design principles that accurately identify previously known dopants like Pd, and also predict new dopants As and Se, that can be effective in binding all lanthanides within the uranium matrix. Altogether, this research helps to develop generic alloy-design principles for complex multi-component systems based on lanthanide and dopantmore » intrinsic characteristics.« less

Authors:
 [1];  [2];  [3];  [3];  [3];  [4];  [1]
  1. Univ. of Idaho, Moscow, ID (United States)
  2. Univ. of Idaho, Moscow, ID (United States); Center for Advanced Energy Studies, Idaho Falls, ID (United States); Idaho National Lab. (INL), Idaho Falls, ID (United States)
  3. Idaho National Lab. (INL), Idaho Falls, ID (United States)
  4. Univ. of Idaho, Moscow, ID (United States); Center for Advanced Energy Studies, Idaho Falls, ID (United States)
Publication Date:
Research Org.:
Univ. of Idaho, Moscow, ID (United States)
Sponsoring Org.:
USDOE Office of Nuclear Energy (NE), Nuclear Energy University Program (NEUP)
OSTI Identifier:
1645098
Grant/Contract Number:  
NE0008557; AC07-05ID14517
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Nuclear Materials
Additional Journal Information:
Journal Volume: 540; Journal Issue: C; Journal ID: ISSN 0022-3115
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS; Metallic fuel; FCCI; Fuel additive; First-principle calculations

Citation Formats

Khanal, Rabi, Jerred, Nathan, Benson, Michael T., Xie, Yi, Mariani, Robert D., Charit, Indrajit, and Choudhury, Samrat. Interactions and immobilization of lanthanides with dopants in uranium-based metallic fuels. United States: N. p., 2020. Web. https://doi.org/10.1016/j.jnucmat.2020.152372.
Khanal, Rabi, Jerred, Nathan, Benson, Michael T., Xie, Yi, Mariani, Robert D., Charit, Indrajit, & Choudhury, Samrat. Interactions and immobilization of lanthanides with dopants in uranium-based metallic fuels. United States. https://doi.org/10.1016/j.jnucmat.2020.152372
Khanal, Rabi, Jerred, Nathan, Benson, Michael T., Xie, Yi, Mariani, Robert D., Charit, Indrajit, and Choudhury, Samrat. Thu . "Interactions and immobilization of lanthanides with dopants in uranium-based metallic fuels". United States. https://doi.org/10.1016/j.jnucmat.2020.152372. https://www.osti.gov/servlets/purl/1645098.
@article{osti_1645098,
title = {Interactions and immobilization of lanthanides with dopants in uranium-based metallic fuels},
author = {Khanal, Rabi and Jerred, Nathan and Benson, Michael T. and Xie, Yi and Mariani, Robert D. and Charit, Indrajit and Choudhury, Samrat},
abstractNote = {In uranium-based fuels, production and migration of lanthanide fission products and subsequent chemical interactions with cladding constituents lead to fuel–cladding chemical interaction (FCCI), limiting fuel performance. In general, dopant addition to the fuel matrix to arrest lanthanides within the fuel by forming intermetallics is found to be effective in mitigating FCCI. Recently, we proposed ab-initio based alloy-design principles, which can be useful in identifying dopant(s) that can bind a lanthanide (Nd) inside the fuel matrix. Here, we demonstrate the robustness of such principles by performing a systematic study to choose dopants to form compounds with a range of experimentally-observed lanthanide fission products. Results reveal that for a given dopant, lanthanide Ce and La exhibit similar behavior in their compound-forming tendencies compared to Nd and Pr, which is linked to lanthanide intrinsic characteristics such as the electronic configurations. Our predicted lanthanide-dopant intermetallic formation is verified experimentally in selective cases. Finally, we showed alloy design principles that accurately identify previously known dopants like Pd, and also predict new dopants As and Se, that can be effective in binding all lanthanides within the uranium matrix. Altogether, this research helps to develop generic alloy-design principles for complex multi-component systems based on lanthanide and dopant intrinsic characteristics.},
doi = {10.1016/j.jnucmat.2020.152372},
journal = {Journal of Nuclear Materials},
number = C,
volume = 540,
place = {United States},
year = {2020},
month = {7}
}

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