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Design and Structural Transformations of Zinc(II) Knotted Cage Frameworks.

Yuchong Yang1, Sabrina Y Hu1, Tanya K Ronson1

  • 1Yusuf Hamied Department of Chemistry, University of Cambridge, Cambridge, CB2 1EW, United Kingdom.

Angewandte Chemie (International Ed. in English)
|October 16, 2025
PubMed
Summary

Researchers developed a new method for synthesizing complex interwoven molecular architectures using tailored ligands and zinc coordination. This breakthrough allows for controlled transformations and tunable guest encapsulation in knotted cage frameworks.

Keywords:
Host–guest chemistryInterwoven structuresMetal‐organic cagesSelf‐assemblySubcomponent exchange

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Area of Science:

  • Supramolecular Chemistry
  • Materials Science
  • Organic Synthesis

Background:

  • Interwoven architectures are prevalent in biomolecules like proteins, DNA, and RNA.
  • Synthesizing artificial interwoven structures with complex topologies remains a significant challenge.
  • Controlled structural transformations of these artificial systems are not well-established.

Purpose of the Study:

  • To develop a rational design strategy for synthesizing artificial interwoven structures.
  • To enable controlled self-assembly of covalently linked knotted cage frameworks.
  • To investigate the role of structural rigidity in framework transformations and guest binding.

Main Methods:

  • Utilized tailored ligands and zinc coordination to direct self-assembly.
  • Employed a rational design strategy focusing on ligand rigidity.
  • Investigated the impact of peripheral crosslinkers and subcomponent addition sequence.

Main Results:

  • Successfully synthesized covalently linked trefoil perplexane and trefoil tetrahedral knotted cage frameworks.
  • Demonstrated two-way interconversion between interwoven and non-interwoven architectures.
  • Showcased tunable guest encapsulation and release, regulated by cage conformation and crosslinkers.

Conclusions:

  • Structural rigidity is key to governing framework transformations in self-assembled systems.
  • The sequence of subcomponent addition critically influences product outcomes by stabilizing intermediates.
  • This work provides a pathway for designing complex, transformable molecular architectures with tunable properties.