The First Quantitative Synthesis of a Closed Three-Link Chain (613) Using Coordination and Noncovalent Interactions-Driven Self-Assembly
| Autor: | Jatinder Singh, Ki-Whan Chi, Eun-Hee Kim, Dong Hwan Kim, Rizky Hadiputra, Hyunuk Kim, Jaehoon Jung |
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| Rok vydání: | 2020 |
| Předmět: |
chemistry.chemical_classification
Chemistry Catenane Supramolecular chemistry General Chemistry 010402 general chemistry Topology 01 natural sciences Biochemistry Catalysis 0104 chemical sciences Colloid and Surface Chemistry Chain (algebraic topology) Molecular knot Non-covalent interactions Rectangle Link (knot theory) Borromean rings |
| Zdroj: | Journal of the American Chemical Society. 142:9327-9336 |
| ISSN: | 1520-5126 0002-7863 |
| DOI: | 10.1021/jacs.0c01406 |
| Popis: | Engineering of supramolecular topologies offers potential opportunities for tailoring their properties to various function and applications. However, the synthesis of interlocked or intertwined compounds, catenanes, links or knots, is a challenge. Previously, we used coordination-driven self-assembly and noncovalent interactions (NCIs) between metal-based acceptors and multipyridyl donors to create supramolecular topologies with increasing complexity. Self-assembling components of fixed length and geometry have been utilized for the production of topologies such as Borromean rings, Solomon links, Hopf's link, "rectangle in rectangle", and an 818 molecular knot. However, recent synthesis of a linear [3]catenane by us witnessed the importance of flexible ligands along with coordination-driven self-assembly and NCIs in self-assembling units. This flexibility provides distinctive angularity for the recognition of various NCIs and thus offers tremendous possibilities for realizing complex supramolecular topologies. This study proposed a selective and quantitative synthesis, and also the first X-ray characterization of a closed three-link chain (a prime link of [3]catenane with 6 crossings) via two component coordination-driven self-assembly. The experiments based upon concentration, guest template, and solvent effects were systematically presented. Furthermore, the experimental finding was supported by density functional theory calculations, which highlighted the necessity of the multiple NCIs along with appropriate geometry of the [2 + 2] rings. |
| Databáze: | OpenAIRE |
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