The i-SANEX process has been developed as a promising strategy for the separation of trivalent lanthanide-actinides, which can effectively overcome the poor solubility of N-donors in nonpolar solvents. In this study, four hydrophilic phenanthroline-based ligands (L1-L4) with different terminal groups were synthesized to evaluate their water solubility and masking effects on An(III) in aqueous solutions using competitive extraction dominated by TODGA. Among these ligands, BHEO-DAPhen (L1), featuring an ethoxyethanol-modified side chain, demonstrated the best overall performance in both solubili...