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

JOURNAL OF NUCLEAR MATERIALS

卷:540

Article

Khanal, Rabi^1,4  Jerred, Nathan^1,2,3  Benson, Michael T.³  Xie, Yi³  Mariani, Robert D.³  Charit, Indrajit^1,2  Choudhury, Samrat¹ 

[1] Univ Idaho, Dept Chem & Mat Engn, Moscow, ID 83844 USA

[2] Ctr Adv Energy Studies, Idaho Falls, ID 83401 USA

[3] Idaho Natl Lab, POB 1625, Idaho Falls, ID 83415 USA

[4] Oak Ridge Natl Lab, Computat Sci & Engn Div, POB 2009, Oak Ridge, TN 37830 USA

关键词: Metallic fuel;    FCCI;    Fuel additive;    First-principle calculations;   

DOI  :  10.1016/j.jnucmat.2020.152372

来源: Elsevier

【 摘 要 】

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. Overall, this research helps to develop generic alloy-design principles for complex multi-component systems based on lanthanide and dopant intrinsic characteristics. (C) 2020 Elsevier B.V. All rights reserved.

【 授权许可】

Free