Theoretical investigation on the ligands constructed from phenanthroline and five-membered N-heterocyclic rings for bonding and separation properties of Am(<scp>iii</scp>) and Eu(<scp>iii</scp>)

Wu, Shouqiang; Li, An Yong

doi:10.1039/d3cp05101c

Phys. Chem. Chem. Phys.

2024

DOI: 10.1039/d3cp05101c

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Theoretical investigation on the ligands constructed from phenanthroline and five-membered N-heterocyclic rings for bonding and separation properties of Am(iii) and Eu(iii)

Shouqiang Wu,

An Yong Li

Abstract: The ligands, derived from the combination of phenanthroline and various five-membered N-heterocyclic rings, were subject to a comprehensive investigation for their potential in the extraction and separation of actinides and lanthanides.

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Tetradentate Ligand’s Chameleon-Like Behavior Offers Recognition of Specific Lanthanides

Pramanik,

Li,

Driscoll

et al. 2024

J. Am. Chem. Soc.

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The surging demand for high-purity individual lanthanides necessitates the development of novel and exceptionally selective separation strategies. At the heart of these separation systems is an organic compound that, based on its structural features, selectively recognizes the lighter or heavier lanthanides in the trivalent lanthanide (Ln) series. This work emphasizes the significant implications resulting from modifying the donor group configuration within an N,O-based tetradentate ligand and the changes in the solvation environment of Ln ions in the process of separating Lns, with the unique ability to achieve peak selectivity in the light, medium, and heavy Ln regions. The structural rigidity of the bis-lactam-1,10-phenanthroline ligand enforces size-based selectivity, displaying an exceptional affinity for Lns having larger ionic radii such as La. Modifying the ligand by eliminating one preorganization element (phenanthroline → bipyridine) results in the fast formation of complexes with light Lns, but, in the span of hours, the peak selectivity shifts toward middle Ln (Sm), resulting in time-resolved separation. As expected, at low nitric acid concentrations, the neutral tetradentate ligand complexes with Ln3+ ions. However, the change in extraction mechanism is observed at high nitric acid concentrations, leading to the formation and preferential extraction of anionic heavy Ln species, [Ln(NO3) x+3] x−, that self-assemble with two ligands that have undergone protonation, forming intricate supramolecular architectures. The tetradentate ligand that is structurally balanced with restrictive and unrestrictive motifs demonstrates unique, controllable selectivity for light, middle, and heavy Lns, underscoring the pivotal role of solvation and ion interactions within the first and second coordination spheres.

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Tetradentate Ligand’s Chameleon-Like Behavior Offers Recognition of Specific Lanthanides

Pramanik,

Li,

Driscoll

et al. 2024

J. Am. Chem. Soc.

View full text Add to dashboard Cite

show abstract

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Theoretical investigation on the ligands constructed from phenanthroline and five-membered N-heterocyclic rings for bonding and separation properties of Am(iii) and Eu(iii)

Abstract: The ligands, derived from the combination of phenanthroline and various five-membered N-heterocyclic rings, were subject to a comprehensive investigation for their potential in the extraction and separation of actinides and lanthanides.

Cited by 1 publication

References 49 publications

Tetradentate Ligand’s Chameleon-Like Behavior Offers Recognition of Specific Lanthanides

Tetradentate Ligand’s Chameleon-Like Behavior Offers Recognition of Specific Lanthanides

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