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Secondary nucleation as a strategy towards hierarchically organized mesoscale topologies in supramolecular polymerization

Nature Chemistry volume 17, pages 477–492 (2025)Cite this article

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Abstract

Developing new generic methodologies for organizing molecules into nano- to mesoscale structures of precise shapes and sizes is a research topic at the forefront of modern chemistry. Creating hierarchical molecular assembly, especially at the mesoscale, is important to realize functions reminiscent of those manifested by biomolecular assemblies in the mesoscopic regime. However, this is challenging due to the difficulty in maintaining stringent controllability over the organization of molecules at higher hierarchical levels, wherein weak non-directional intermolecular interactions rather than strong directional interactions typically play a predominant role. Recent studies have revealed that secondary nucleation, often experienced by one-dimensional assemblies such as supramolecular polymers that grow with spontaneous nucleation, is effective in the hierarchical construction of higher-order structures. Here we illustrate how secondary nucleation can be combined with the well-established precision synthesis of supramolecular polymers to realize precise control over hierarchical structures in the mesoscopic regime. We present a roadmap for creating hierarchical supramolecular polymers by exploiting secondary nucleation–elongation processes and discuss future prospects for the field.

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Fig. 1: Distribution of intermolecular interactions in hierarchical self-assembly.
Fig. 2: Utilizing secondary nucleation towards hierarchical supramolecular polymer topologies.
Fig. 3: Molecular design and role of solvent in inducing secondary nucleation.
Fig. 4: Stereoselective primary and secondary nucleation in supramolecular polymerization.
Fig. 5: Secondary nucleation on supramolecular polymer toroids leading to self-assembled polycatenanes.
Fig. 6: Synthesis of supramolecular polymer concentric toroids and corresponding block supramolecular polymers by secondary nucleation.
Fig. 7: Secondary nucleation in gels.

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Acknowledgements

This work was supported by the Japan Society for the Promotion of Science (KAKENHI grants JP22H00331 and JP23H04873 to S.Y. and JP22K20526 to S.D.) as part of the Grant-in-Aid for Transformative Research Areas project Materials Science of Meso-Hierarchy. H.I. and T.S. each acknowledge the Japan Society for the Promotion of Science for a Research Fellowship for Young Scientists (24KJ0529 and 21J20988, respectively).

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  1. Institute for Advanced Academic Research, Chiba University, Chiba, Japan

    Sougata Datta & Shiki Yagai

  2. Division of Advanced Science and Engineering, Graduate School of Engineering, Chiba University, Chiba, Japan

    Hiroki Itabashi & Takuho Saito

  3. Department of Applied Chemistry and Biotechnology, Graduate School of Engineering, Chiba University, Chiba, Japan

    Shiki Yagai

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  1. Sougata Datta
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Datta, S., Itabashi, H., Saito, T. et al. Secondary nucleation as a strategy towards hierarchically organized mesoscale topologies in supramolecular polymerization. Nat. Chem. 17, 477–492 (2025). https://doi.org/10.1038/s41557-025-01764-5

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