Local Structure and Magnetism of La1–xMxPO4 (M = Sm, 239Pu, 241Am) Explained by Experimental and Computational Analyses

With their high chemical and self-irradiation stability, crystalline monazites are among the most promising materials for the encapsulation of nuclear wastes. Yet, the local and magnetic structures of the matrices doped with low-content actinide cation, depicted as most resistant, are still unclear....

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Bibliographic Details
Published in:Journal of physical chemistry. C 2021-10, Vol.125 (40)
Main Authors: Martel, Laura, Islam, Md. Ashraful, Popa, Karin, Vigier, Jean-François, Colineau, Eric, Bolvin, Hélène, Griveau, Jean-Christophe
Format: Article
Language:English
Subjects:
Chemical Sciences
Inorganic chemistry
or physical chemistry
Theoretical and
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Summary:With their high chemical and self-irradiation stability, crystalline monazites are among the most promising materials for the encapsulation of nuclear wastes. Yet, the local and magnetic structures of the matrices doped with low-content actinide cation, depicted as most resistant, are still unclear. This limits the development of theoretical approaches predicting their behavior under extreme conditions—self-irradiation and long-term leaching. Here, we characterize the model matrices La1–xMxPO4 (0 ≤ x ≤ 0.10)—with M = Sm, 239Pu, 241Am—by X-ray diffraction and solid-state 31P NMR. As an example, we confirm that La0.96241Am0.04PO4 has higher self-irradiation resistance compared to 241AmPO4. Further, computational analyses show that magnetic properties of the Pu complex are strongly affected by the J-mixing and the paramagnetic NMR shifts are dominated by the Fermi contact contribution, arising from delocalization of the spin density of the cation toward the phosphorus through the bonds.
ISSN:1932-7447
1932-7455
DOI:10.1021/acs.jpcc.1c03957