Article Dans Une Revue Angewandte Chemie International Edition Année : 2026

Programming Palladium Cage Geometry through Ligand Redox Modulation

Jean Nicolas
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Maksym Dekhtiarenko
David Canevet
Magali Allain
Marc Sallé
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Sébastien Goeb
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Résumé

Incorporating redox active ligands into coordination cages offers a direct way to reach architectures whose structure or composition can be modulated in response to changes in the oxidation state. An exTTF-based ditopic ligand L affords a M2L4 cage in presence of a palladium(II) salt (M). The resulting M2L4 cavity exhibits selective binding properties for medium length α, ω-dinitrile alkanes. Modifying the coordination geometry of the ligand by oxidation to its Lox state redirects the self-assembly process toward a M2Lox2 structure. The oxidized ligand can also be combined with a dibenzothiophene linker (L') to afford a heteroleptic M2LoxL'2 structure whose vacant coordination sites enable subsequent dimerization into an unprecedented M4L4L'4 architecture. Key intermediates and products were structurally authenticated by single-crystal x-ray diffraction. Notably, these processes are reversible. Reduction converts the M2LoxL'2 assembly back to the homoleptic M2L4 cage. This sequence illustrates how changes of oxidation state can reshape nuclearity and composition in metal organic assemblies.

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hal-05627661 , version 1 (20-05-2026)

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Jennifer Bou Zeid, Jean Nicolas, Maksym Dekhtiarenko, David Canevet, Magali Allain, et al.. Programming Palladium Cage Geometry through Ligand Redox Modulation. Angewandte Chemie International Edition, 2026, pp.e5709785. ⟨10.1002/anie.5709785⟩. ⟨hal-05627661⟩
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