Elaborated entanglements of strands are ubiquitously found in craftworks and industrial products on macroscale, but quite rare in nanoscale. We have been challenging construction of highly entangled nanostructures by means of latent entangling nature of a reversible metal–peptide chain. In this work, we succeeded in construction of highly entangled torus topologies from a flexible ditopic tripeptide ligand and silver(I) ions.1,2 First, we found complexation of ligand 1 with the GGG (G = Gly) sequence and silver(I) afforded two equilibrium products of highly symmetric structures. Crystallographic studies revealed these products were 7-crossing torus knot 2 and 8-crossing analogue 3. Seven and eight repeats of a common 1-crossing entangled motif resulted in such unique topological frameworks. In addition, poly[n]catenane 4, repeats of a 2-crossing entangled motif, was also obtained from the same building blocks in the different solvent conditions. Moreover, introduction of alkyl sidechains to the ligand afforded 9-crossing torus knot 5 and toroidal superhelix 6, an infinite form of torus knots, with retaining the 1-crossing entangled motifs. All these structures elucidated the metal–peptide folding and assembly process occurred in high regio- and stereoselectivities. Thus, we succeeded in engineering of highly entangled torus topologies by reversible metal–peptide chains.

Construction of Highly Entangled Torus Topologies via Folding and Assembly of Metal–Peptide Strands

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