3 years ago

Morphological Control of Heteroleptic cis- and trans-Pd2L2L′2 Cages

Morphological Control of Heteroleptic cis- and trans-Pd2L2L′2 Cages
Witold M. Bloch, Guido H. Clever, Wolf Hiller, Julian J. Holstein
Control over the integrative self-sorting of metallo-supramolecular assemblies opens up possibilities for introducing increased complexity and function into a single self-assembled architecture. Herein, the relationship between the geometry of three ligand components and morphology of three self-sorted heteroleptic [Pd2L2L′2]4+ cages is examined. Pd-mediated assembly of two bis-monodentate pyridyl ligands with native bite angles of 75° and 120° affords a cis-[Pd2L2L′2]4+ cage while the same reaction with two ligands with bite angles of 75° and 60° gives an unprecedented, self-penetrating structural motif; a trans-[Pd2(anti-L)2L′2]4+ heteroleptic cage with a “doubly bridged figure eight” topology. Each heteroleptic assembly can be formed by cage-to-cage conversion of the homoleptic precursors and morphological control of [Pd2L2L′2] cages is achieved by selective ligand displacement transformations in a system of three ligands and at least six possible cage products. A doubly bridged figure eight: Integrative self-sorting of geometrically distinct ligands and cages is regulated to form new [Pd2L2L′2] structures. For one example, X-ray analysis reveals a doubly bridged figure-eight topology which is an unprecedented motif for metallo-supramolecular structures. Furthermore, morphological control of a system of cages is achieved by highly selective ligand displacement transformations.

Publisher URL: http://onlinelibrary.wiley.com/resolve/doi

DOI: 10.1002/anie.201702573

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