Skip to main content

Research Repository

Advanced Search

Self-assembled poly-catenanes from supramolecular toroidal building blocks

Datta, Sougata; Kato, Yasuki; Higashiharaguchi, Seiya; Aratsu, Keisuke; Isobe, Atsushi; Saito, Takuho; Prabhu, Deepak D.; Kitamoto, Yuichi; Hollamby, Martin J.; Smith, Andrew J.; Dalgliesh, Robert; Mahmoudi, Najet; Pesce, Luca; Perego, Claudio; Pavan, Giovanni M.; Yagai, Shiki

Self-assembled poly-catenanes from supramolecular toroidal building blocks Thumbnail


Sougata Datta

Yasuki Kato

Seiya Higashiharaguchi

Keisuke Aratsu

Atsushi Isobe

Takuho Saito

Deepak D. Prabhu

Yuichi Kitamoto

Andrew J. Smith

Robert Dalgliesh

Najet Mahmoudi

Luca Pesce

Claudio Perego

Giovanni M. Pavan

Shiki Yagai


Mechanical interlocking of molecules (catenation) is a nontrivial challenge in modern synthetic chemistry and materials science1,2. One strategy to achieve catenation is the design of pre-annular molecules that are capable of both efficient cyclization and of pre-organizing another precursor to engage in subsequent interlocking3,4,5,6,7,8,9. This task is particularly difficult when the annular target is composed of a large ensemble of molecules, that is, when it is a supramolecular assembly. However, the construction of such unprecedented assemblies would enable the visualization of nontrivial nanotopologies through microscopy techniques, which would not only satisfy academic curiosity but also pave the way to the development of materials with nanotopology-derived properties. Here we report the synthesis of such a nanotopology using fibrous supramolecular assemblies with intrinsic curvature. Using a solvent-mixing strategy, we kinetically organized a molecule that can elongate into toroids with a radius of about 13 nanometres. Atomic force microscopy on the resulting nanoscale toroids revealed a high percentage of catenation, which is sufficient to yield ‘nanolympiadane’10, a nanoscale catenane composed of five interlocked toroids. Spectroscopic and theoretical studies suggested that this unusually high degree of catenation stems from the secondary nucleation of the precursor molecules around the toroids. By modifying the self-assembly protocol to promote ring closure and secondary nucleation, a maximum catenation number of 22 was confirmed by atomic force microscopy.

Journal Article Type Article
Acceptance Date May 19, 2020
Publication Date Jul 15, 2020
Journal Nature
Print ISSN 0028-0836
Publisher Nature Publishing Group
Peer Reviewed Peer Reviewed
Volume 583
Pages 400 - 405
Keywords Interlocked molecules; Supramolecular polymers
Publisher URL


You might also like

Downloadable Citations