Electrochemically assisted leaching of rare earth carbonates in non-aqueous green solvents: Solvent design, characterization, and process optimization

This study presents a systematic approach to the design, characterization, and application of non-aqueous green solvents (NAGSs) for the leaching of rare earth carbonate hydrates (RECHs). Four NAGSs based on choline chloride, ethylene glycol, and various carboxylic acids were synthesized and evaluated for their physicochemical and electrochemical properties. Among the evaluated formulations, the choline chloride-ethylene glycol-Na2EDTA & sdot;2H2O mixture (N1) and the chloride-levulinic acid mixture (N2) were found were found suitable for both traditional and electrochemically assisted leaching due to their optimal viscosity, conductivity, and electrochemical stability. Electrochemical assistance significantly enhanced leaching efficiency, with improvements ranging from 22 % to over 300 % for certain elements compared to conventional methods. Mechanistic investigations revealed that the application of an oxidative potential facilitates the protonation and dissolution of RECHs, likely through the generation of localized acidic environments and the formation of intermediate species. The FTIR analysis confirmed the dissolution of carbonate phases and the formation of rare earth-ligand complexes, particularly in the N1 system, where new bands associated with carboxylate and amine coordination were observed. Importantly, the proposed electrochemically assisted method can be applied to different primary or secondary sources in both aqueous and non-aqueous solutions. The results demonstrate the advantages of combining non-aqueous green solvents with electrochemical assistance as an environmentally benign alternative to conventional acid-based leaching, especially for challenging carbonate forms of rare earth elements. This work provides important guidelines for the development of sustainable hydrometallurgical processes, with future directions including solvent recyclability, selective recovery, and environmental assessment.