Deep Eutectic Solvent-Driven Recycling of Uranium Scrap: A Sustainable Electrochemical Pathway to Pure UO ₂ and Stable U(VI) Species

Recycling of uranium-bearing scrap is essential for a sustainable closed nuclear fuel cycle. This work demonstrates a low-temperature, green electrochemical route for direct recycling of scrap metallic uranium using a hydrophobic deep eutectic solvent (HTPPBr:2DA). Anodic dissolution of uranium turnings leads to a dual outcome: precipitation of phase-pure UO2 and stabilization of dissolved U(VI) as a highly stable uranyl complex in the DES. Comprehensive spectroscopic, electrochemical, structural, and theoretical investigations confirm the oxidation states, coordination environment, and redox behavior of uranium species. The results establish a “wealth-from-waste” strategy, offering an environmentally benign alternative to conventional high-temperature and acid-based processes with potential application in closed-loop nuclear fuel cycle management.