Selective Synthesis and Structural Transformation of a 4‐Ravel Containing Four Crossings and Featuring CpRh/Ir Fragments

Intricately interwoven topologies are continually being synthesized and are ultimately equally versatile and significant at the nanoscale level; however, reports concerning ravel structures, which are highly entwined new topological species, are extremely rare and fraught with tremendous synthesis c...

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Published in:Angewandte Chemie International Edition Vol. 62; no. 20; pp. e202301516 - n/a
Main Authors: Dang, Li‐Long, Zhang, Ting‐Ting, Chen, Tian, Zhao, Ying, Gao, Xiang, Aznarez, Francisco, Ma, Lu‐Fang, Jin, Guo‐Xin
Format: Journal Article
Language:English
Published: Germany Wiley Subscription Services, Inc 08.05.2023
Edition:International ed. in English
Subjects:
4-Ravel
Coordination-Driven Self-Assembly
Crystallography
Half-Sandwich Fragment
Magnetic resonance spectroscopy
Metal concentrations
NMR
NMR spectroscopy
Nuclear magnetic resonance
Organometallic Cages
Rare species
Self-assembly
Synthesis
Topology
π⋅⋅⋅π Interactions
π⋅⋅⋅π Interactions
Half-Sandwich Fragment
4-Ravel
Organometallic Cages
Coordination-Driven Self-Assembly
ISSN:1433-7851, 1521-3773, 1521-3773
Online Access:Get full text
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Summary:Intricately interwoven topologies are continually being synthesized and are ultimately equally versatile and significant at the nanoscale level; however, reports concerning ravel structures, which are highly entwined new topological species, are extremely rare and fraught with tremendous synthesis challenges. To solve the synthesis problem, a tetrapodontic pyridine ligand L1 with two types of olefinic bond units and two Cp*M‐based building blocks (E1, M=Rh; E2, M=Ir) featuring large conjugated planes was prepared to perform the self‐assembly. Two unprecedented [5+10] icosanuclear molecular 4‐ravels containing four crossings were obtained by parallel‐displaced π⋅⋅⋅π interactions in a single‐step strategy. Remarkably, reversible structural transformations between the 4‐ravel and the corresponding metallocage could be realized by concentration changes and solvent‐ and guest‐induced effects. X‐ray crystallographic data and NMR spectroscopy provide full confirmation of these phenomena. Two unprecedented [5+10] icosanuclear molecular 4‐ravels containing four crossings have been generated using a single‐step strategy. This topology is achieved by utilizing parallel‐displaced π⋅⋅⋅π interactions with carefully selected naphthoquinoyl Cp*M building blocks and X‐shaped pyridyl ligands.
Bibliography:These authors contributed equally to this work.
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ISSN:1433-7851
1521-3773
1521-3773
DOI:10.1002/anie.202301516