Chemistry of palladium(II) with bis(3-amidopyridine) ligands

Yue, Nancy L. S.; Jennings, Michael C.; Puddephatt, Richard J.

doi:10.1016/j.ica.2016.02.022

Cited by 8 publications

(2 citation statements)

References 45 publications

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“…The bidentate ligand L3 possesses a central aromatic spacer and two terminal 3-pyridyl moieties connected by ester linkages. A few ligands of comparable designs with amide linkages are known, which form [Pd 2 L 4 ] complexes [45][46][47] . The amide linkages are somewhat rigid and are capable of interacting with counteranions inside the corresponding cavity, when suitably oriented thereby influencing the formation of smaller [Pd 2 L 4 ] complexes.…”

Section: Resultsmentioning

confidence: 99%

Self-assembled conjoined-cages

Samantray

Chand

2020

Nat Commun

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A self-assembled coordination cage usually possesses one well-defined three-dimensional (3D) cavity whereas infinite number of 3D-cavities are crafted in a designer metal-organic framework. Construction of a discrete coordination cage possessing multiple number of 3Dcavities is a challenging task. Here we report the peripheral decoration of a trinuclear [Pd 3 L 6 ] core with one, two and three units of a [Pd 2 L 4 ] entity for the preparation of multi-3D-cavity conjoined-cages of [Pd 4 (L a) 2 (L b) 4 ], [Pd 5 (L b) 4 (L c) 2 ] and [Pd 6 (L c) 6 ] formulations, respectively. Formation of the tetranuclear and pentanuclear complexes is attributed to the favorable integrative self-sorting of the participating components. Cage-fusion reactions and ligand-displacement-induced cage-to-cage transformation reactions are carried out using appropriately chosen ligand components and cages prepared in this work. The smaller [Pd 2 L 4 ] cavity selectively binds one unit of NO 3 − , F − , Cl − or Br − while the larger [Pd 3 L 6 ] cavity accommodates up to four DMSO molecules. Designing aspects of our conjoined-cages possess enough potential to inspire construction of exotic molecular architectures.

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Section: Resultsmentioning

confidence: 99%

Self-assembled conjoined-cages

Samantray

Chand

2020

Nat Commun

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“…This motif has been widely used for the development of aromatic oligoamide foldamers with highly predictable and stable structures . For metal based self‐assembly, ligands of this type have been used for the formation of small Pd 2 L 4 cages but never been shown to be applicable for larger structures . As the above interactions should limit the flexibility of the bend angle, we reasoned that large cages could be accessible.…”

Section: Figurementioning

confidence: 99%

Balancing Ligand Flexibility versus Rigidity for the Stepwise Self‐Assembly of M₁₂L₂₄ via M₆L₁₂ Metal–Organic Cages

Liu

Bobylev

et al. 2020

Chemistry A European J

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Non‐covalent interactions are important for directing protein folding across multiple intermediates and can even provide access to multiple stable structures with different properties and functions. Herein, we describe an approach for mimicking this behavior in the self‐assembly of metal–organic cages. Two ligands, the bend angles of which are controlled by non‐covalent interactions and one ligand lacking the above‐mentioned interactions, were synthesized and used for self‐assembly with Pd2+. As these weak interactions are easily broken, the bend angles have a controlled flexibility giving access to M2(L1)4, M6(L2)12, and M12(L2)24 cages. By controlling the self‐assembly conditions this process can be directed in a stepwise fashion. Additionally, the multiple endohedral hydrogen‐bonding sites on the ligand were found to play a role in the binding and discrimination of neutral guests.

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A Water Soluble Pd₂L₄ Cage for Selective Binding of Neu5Ac

Schaapkens

Sluis

Bobylev

et al. 2021

Chemistry A European J

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The sialic acid N‐acetylneuraminic acid (Neu5Ac) and its derivatives are involved in many biological processes including cell‐cell recognition and infection by influenza. Molecules that can recognize Neu5Ac might thus be exploited to intervene in or monitor such events. A key obstacle in this development is the sparse availability of easily prepared molecules that bind to this carbohydrate in its natural solvent; water. Here, we report that the carbohydrate binding pocket of an organic soluble [Pd2L4]4+ cage could be equipped with guanidinium‐terminating dendrons to give the water soluble [Pd2L4][NO3]16 cage 7. It was shown by means of NMR spectroscopy that 7 binds selectively to anionic monosaccharides and strongest to Neu5Ac with Ka=24 M−1. The cage had low to no affinity for the thirteen neutral saccharides studied. Aided by molecular modeling, the selectivity for anionic carbohydrates such as Neu5Ac could be rationalized by the presence of charge assisted hydrogen bonds and/or the presence of a salt bridge with a guanidinium solubilizing arm of 7. Establishing that a simple coordination cage such as 7 can already selectively bind to Neu5Ac in water paves the way to improve the stability, affinity and/or selectivity properties of M2L4 cages for carbohydrates and other small molecules.

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Chemistry of palladium(II) with bis(3-amidopyridine) ligands

Cited by 8 publications

References 45 publications

Self-assembled conjoined-cages

Self-assembled conjoined-cages

Balancing Ligand Flexibility versus Rigidity for the Stepwise Self‐Assembly of M₁₂L₂₄ via M₆L₁₂ Metal–Organic Cages

A Water Soluble Pd₂L₄ Cage for Selective Binding of Neu5Ac

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Chemistry of palladium(II) with bis(3-amidopyridine) ligands

Cited by 8 publications

References 45 publications

Self-assembled conjoined-cages

Self-assembled conjoined-cages

Balancing Ligand Flexibility versus Rigidity for the Stepwise Self‐Assembly of M12L24 via M6L12 Metal–Organic Cages

A Water Soluble Pd2L4 Cage for Selective Binding of Neu5Ac

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Balancing Ligand Flexibility versus Rigidity for the Stepwise Self‐Assembly of M₁₂L₂₄ via M₆L₁₂ Metal–Organic Cages

A Water Soluble Pd₂L₄ Cage for Selective Binding of Neu5Ac