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Tuning Selectivity and Stability in Heteroleptic Lanthanide Adducts by Ligand Design. | LitMetric

Tuning Selectivity and Stability in Heteroleptic Lanthanide Adducts by Ligand Design.

Inorg Chem

Department of Inorganic and Analytical Chemistry, University of Geneva, 30 quai E. Ansermet, CH-1211 Geneva 4, Switzerland.

Published: February 2024

Terdentate ligands - and their heteroleptic [Ln(hfac)] complexes (Ln = La, Eu, Gd, Er, or Y; H-hfac = 1,1,1,5,5,5-hexafluoropentane-2,4-dione) exhibit multifactorial correlations between the ligand's structural frameworks, including their level of preorganization and steric congestion and their affinities and selectivities for catching the trivalent lanthanide containers [Ln(hfac)]. The polyaromatic ligand scaffolds could be stepwise modulated via lanthanide-template synthetic strategies, using intermolecular rhodium-catalyzed insertion reactions. The increasing level of preorganization along the → → series leads to a duality in which larger thermodynamic formation constants with lanthanides in CDCl are accompanied by an unexpected decrease in the Ln-N affinities in the solid state, which could be assigned to a limited match between the lanthanide size and the enlarged preorganized cavities. On the contrary, a reduced stability is induced by the connection of additional methyl groups at position 1 of the benzimidazole moieties in and , which is accompanied by an optimization of metal-nitrogen bond lengths. This study contributes to the rational design of highly stable neutral heteroleptic lanthanide β-diketonate adducts that resist dissociation in solution, a prerequisite for photophysical applications using these highly luminescent systems at the molecular level.

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Source
http://dx.doi.org/10.1021/acs.inorgchem.3c03710DOI Listing

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