Abstract
The chemistry of molten salts has attracted great research interest owing to their wide applications in diverse fields. In the pyrochemical reprocessing of spent nuclear fuel or molten salt nuclear reactors, lanthanide elements as the principal fission products bring about changes in the composition and properties of molten salts. Herein, we report a comprehensive study on the coordination chemistry of the representative trivalent lanthanide ions (La3+/Nd3+) in LiCl-KCl-CsCl using a multiscale strategy combining Raman spectroscopy, deep learning, and large-scale molecular dynamics (MD) simulations. The neural network potential (NNP)-based MD and Raman spectroscopy studies revealed that La3+/Nd3+ ions prefer to form persistent octahedron complexes with the six-coordinated species as the dominant species at high temperatures. Compared to LaCl63-, NdCl63- shows higher stability with obviously longer lifetimes in LiCl-KCl-CsCl, as confirmed by the observed stronger interaction of Nd3+-Cl- pairs. The total and partial structure factors further indicated the formation of a more stable network structure in LiCl-KCl-CsCl containing NdCl3. Besides, the temperature exerts a larger influence on the local structures of the La3+ species compared to the Nd3+ analogues. According to the potential mean force calculations, the bond dissociation energies follow the order Ln-Cl > Li-Cl > K-Cl > Cs-Cl in LiCl-KCl-CsCl-LnCl3. The NNP-based large-scale MD simulations have been verified to be an efficient and powerful way in molten salt chemistry research.
Published Version
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