A Switchable Palladium(II) Trefoil Entangled Tetrahedron with Temperature Dependence and Concentration Independence

Algar, Jess L.; Findlay, James A.; Evans, Jack D.; Preston, Dan

doi:10.1002/anie.202210476

Cited by 9 publications

(1 citation statement)

References 44 publications

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“…12a). 81 31-mono was similar in structure to 31-long , but with exchange of the pyrazole in the tridentate site for a second triazole, providing an easy route to substitution of the molecule. In 31-mono , a short monomethyl ethylene glycol chain was attached.…”

Section: Discussionmentioning

confidence: 93%

Directing metallo-supramolecular assembly through complementarity

Algar

Preston

2022

Chem. Commun.

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Section: Discussionmentioning

confidence: 93%

Directing metallo-supramolecular assembly through complementarity

Algar

Preston

2022

Chem. Commun.

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A Lantern‐Shaped Pd(II) Cage Constructed from Four Different Low‐Symmetry Ligands with Positional and Orientational Control: An Ancillary Pairings Approach

Preston,

Evans

2023

Angewandte Chemie

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One of the key challenges of metallo‐supramolecular chemistry is to maintain the ease of self‐assembly but, at the same time, create structures of increasingly high levels of complexity. In palladium(II) quadruply stranded lantern‐shaped cages, this has been achieved through either 1) the formation of heteroleptic (multi‐ligand) assemblies, or 2) homoleptic assemblies from low‐symmetry ligands. Heteroleptic cages formed from low‐symmetry ligands, a hybid of these two approaches, would add an additional rich level of complexity but no examples of these have been reported. Here we use a system of ancillary complementary ligand pairings at the termini of cage ligands to target heteroleptic assemblies: these complementary pairs can only interact (through coordination to a single Pd(II) metal ion) between ligands in a cis position on the cage. Complementarity between each pair (and orthogonality to other pairs) is controlled by denticity (tridentate to monodentate or bidentate to bidentate) and/or hydrogen‐bonding capability (AA to DD or AD to DA). This allows positional and orientational control over ligands with different ancillary sites. By using this approach, we have successfully used low‐symmetry ligands to synthesise complex heteroleptic cages, including an example with four different low‐symmetry ligands.

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Diastereoselective Self‐Assembly of Low‐Symmetry Pd_nL_2n Nanocages through Coordination‐Sphere Engineering**

Molinska,

Tarzia,

Male

et al. 2023

Angewandte Chemie

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Metal‐organic cages (MOCs) are popular host architectures assembled from ligands and metal ions/nodes. Assembling structurally complex, low‐symmetry MOCs with anisotropic cavities can be limited by the formation of statistical isomer libraries. We set out to investigate the use of primary coordination‐sphere engineering (CSE) to bias isomer selectivity within homo‐ and heteroleptic PdnL2n cages. Unexpected differences in selectivities between alternative donor groups led us to recognise the significant impact of the second coordination sphere on isomer stabilities. From this, molecular‐level insight into the origins of selectivity between cis and trans diastereoisomers was gained, highlighting the importance of both host‐guest and host‐solvent interactions, in addition to ligand design. This detailed understanding allows precision engineering of low‐symmetry MOC assemblies without wholesale redesign of the ligand framework, and fundamentally provides a theoretical scaffold for the development of stimuli‐responsive, shape‐shifting MOCs.

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A Switchable Palladium(II) Trefoil Entangled Tetrahedron with Temperature Dependence and Concentration Independence

Cited by 9 publications

References 44 publications

Directing metallo-supramolecular assembly through complementarity

Directing metallo-supramolecular assembly through complementarity

A Lantern‐Shaped Pd(II) Cage Constructed from Four Different Low‐Symmetry Ligands with Positional and Orientational Control: An Ancillary Pairings Approach

Diastereoselective Self‐Assembly of Low‐Symmetry Pd_nL_2n Nanocages through Coordination‐Sphere Engineering**

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A Switchable Palladium(II) Trefoil Entangled Tetrahedron with Temperature Dependence and Concentration Independence

Cited by 9 publications

References 44 publications

Directing metallo-supramolecular assembly through complementarity

Directing metallo-supramolecular assembly through complementarity

A Lantern‐Shaped Pd(II) Cage Constructed from Four Different Low‐Symmetry Ligands with Positional and Orientational Control: An Ancillary Pairings Approach

Diastereoselective Self‐Assembly of Low‐Symmetry PdnL2n Nanocages through Coordination‐Sphere Engineering**

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Product

Resources

About

Diastereoselective Self‐Assembly of Low‐Symmetry Pd_nL_2n Nanocages through Coordination‐Sphere Engineering**