Theoretical prediction on the redox potentials of rare-earth ions by deep potentials

J Zhao and WS Liang and GM Lu, IONICS, 27, 2079-2088 (2021).

DOI: 10.1007/s11581-021-03988-0

Redox potential is a crucial electrochemical parameter in the electrorefining process of spent fuel reprocessing. Unfortunately, the harsh measurement environment of spent fuel makes it difficult to obtain. With the continuous updating of computing technology, people have developed the method for calculating the redox potentials using first-principles molecular dynamics (FPMD), but limited by the calculation cost, the simulation scale and time of FPMD are restricted. To make the calculation results more convincing, this work used deep potential (DP) to realize redox potential calculation on a larger time scale. We extracted datasets from FPMD calculations and used these to train and validate the DP, and compared energies, forces, and radial distribution functions that are evaluated using DFT and DP, to demonstrate that DP can achieve DFT accuracy. Using La3+/La as the reference electrode, the redox potentials of Ce3+/Ce, Pr3+/Pr, and Y3+/Y in the LiCl-KCl mixed molten salt system at 723 K were calculated. The results matched well with the FPMD results and experimental data. This work fully demonstrates the feasibility of the DP in calculating the redox potentials. Simultaneously, it provides new idea for obtaining accurate data in the process of spent fuel reprocessing.

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