Self-assembled poly-catenanes from supramolecular toroidal building blocks

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

研究成果: Article査読

106 被引用数 (Scopus)


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 interlocking3–9. 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.

出版ステータスPublished - 2020 7月 16

ASJC Scopus subject areas

  • 一般


「Self-assembled poly-catenanes from supramolecular toroidal building blocks」の研究トピックを掘り下げます。これらがまとまってユニークなフィンガープリントを構成します。