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Effects of Zr(IV) on the electrochemical behavior of UO2F2 and the electrodeposition of UO2
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DOI：10.1016/j.pnucene.2026.106491.png)
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Abstract
En 中文
In molten-salt electrochemical dry reprocessing, the presence of zirconium markedly affects the selective separation and recovery of uranium. In this work, a LiCl-KCl-UO2F2 molten salt system is employed to systematically examine the influence mechanisms of Zr(IV) on the electrochemical behavior of uranyl ions and on UO2 electrodeposition. Cyclic voltammetry and square-wave voltammetry analyses indicate that Zr(IV) undergoes a two-step, two-electron reduction in the molten salt, with reduction potentials more negative than those of the two-step reduction of uranyl ions, demonstrating that Zr(IV) does not directly participate in the electrochemical reduction of uranyl species. The reduction of Zr(IV) to Zr(II) is a diffusion-controlled quasi-reversible process. The diffusion coefficients determined by cyclic voltammetry and square wave voltammetry are 5.06 × 10−5 and 5.73 × 10−5 cm2 s−1, respectively. XRD, Raman and SEM-EDS analyses of the electrolytic products demonstrate that a small amount of Zr(IV) induces the formation of xZrO2·(1-x)UO2 solid solution, leading to a decrease in the lattice parameter of UO2; a high content of Zr(IV) transforms the main phase of the solid solution into ZrO2. The presence of Zr(IV) reduces the current efficiency of UO2 electrodeposition at 6 h from 84.25% (without Zr) to 42.01% (with Zr). The recovery yield of U is also decreased from 65.78% (without Zr) to 25.31% (with Zr).
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