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The Topological Transformation of 4<sub>1</sub> Knot to 4<sub>1</sub><sup>2</sup> Link through Supramolecular Fusion

Pan‐Pan Hua, Junhua Bai, Huijun Feng, Junwen Wang, Lifang Zhang, Guo‐Xin Jin

2024Journal of the American Chemical Society20 citationsDOI

Abstract

Realizing topological transformation through supramolecular fusion is particularly challenging, as the self-assembly of disparate components often results in the orthogonal assembly of building blocks into distinct structures rather than the formation of a heteroleptic architecture. This study introduces a topological transformation, transitioning from a figure-eight knot (4 1 knot) to a Solomon link (4 1 2 link) through a supramolecular fusion process. By employing two structurally similar amino acid ligands ( L1 and L3 ) of varying lengths as bridge ligands, we obtained figure-eight knot 1 and a molecular tweezer-like compound 3 when individually complexed with binuclear Cp*Rh acceptor B1 . Our results revealed that subtle modifications to bridge ligands can lead to dramatic changes in their structures and recognition properties. Moreover, we successfully achieved the targeted formation of a heteroleptic Solomon link 4 by blending figure-eight knot 1 and compound 3 in a 1:1 ratio without the need for templates. This procedure effortlessly converted the 4 1 knot into a 4 1 2 link, thus marking a significant advancement in the topological transformation. This work not only marks the construction of the first heteroleptic Solomon link comprising two distinct metallamacrocycles but also demonstrates a process of supramolecular fusion-based topological transformation involving three distinct topological structures.

Topics & Concepts

Knot (papermaking)Supramolecular chemistryChemistryTransformation (genetics)FusionKnot theoryTopology (electrical circuits)CrystallographyCombinatoricsMathematicsCrystal structureMaterials scienceGeneComposite materialLinguisticsBiochemistryPhilosophySupramolecular Chemistry and ComplexesSupramolecular Self-Assembly in MaterialsChemical Synthesis and Analysis
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