Highly selective hydrophilic ligands were believed to be an efficient way to overcome the massive amount of hazardous organic solvent used in the liquid−liquid extraction process and stood as a new frontier in the Lns(III)/Ans(III) partition. Current reported hydrophilic ligands suffer from harsh preparation conditions, inferior extraction performances, limited available chemical structures, and inability to carry out extraction under high acidity. In this article, we report a simple yet efficient carboxylic group modified phenanthroline-diimide ligand which displayed unexpected Lns(III)/Ans(III) and Ans(III)/Ans(III) separation capabilities in 1.5 M HNO 3 . Unique dimeric architectures for Eu(III) complexes were observed, which could be the origin of the outperforming selectivity and acid resistance. We believe this crystal engineering approach could inspire a renaissance in searching for new functional groups and coordination modes for efficient, highacid-tolerance Lns(III)/Ans(III) separation ligands.
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