Dynamic Helicates Self-Assembly from Homo- and Heterotopic Dynamic Covalent Ligand Strands

Antonio Santoro, Jan Holub, Marta A. Fik-Jaskółka, Ghislaine Vantomme, Jean Marie Lehn (Corresponding author)

Research output: Contribution to journalArticleAcademicpeer-review

22 Citations (Scopus)

Abstract

The understanding and the application of reversible covalent reactions and coordination chemistry together with the proper design of the molecular frameworks, allow to achieve not only well-defined output architectures but also different grades of complex behavior. In this work, the dynamic nature of the helical systems offers an additional level of complexity by combining self-sorting on two levels: 1) the build-up of the ligand strand constituents from their components through dynamic covalent chemistry; 2) the assembly of the helicates from the ligands and the metal cations through dynamic metallo-supramolecular chemistry. The information encoded in the ligands constituent molecule was read differently (and accurately at the same time) by metal cations that varied in the coordination algorithms. It enabled the selective formation of a specific type of helicates from a wide library of helicates formed by the possible combination of subcomponents. Ligands containing dynamic tridentate and/or bidentate binding motifs in the same strand were studied to explore the helicates self-assembly with appropriate metal cations.

Original languageEnglish
Pages (from-to)15664-15671
Number of pages8
JournalChemistry - A European Journal
Volume26
Issue number67
DOIs
Publication statusPublished - 1 Dec 2020

Funding

We thank Dr. Olaf Führ, Prof. Dieter Fenske, Lydia Karmazin, Lydia Brelot and Corinne Bailly for the crystal structure determinations. We also thank Dr. Virginia Smith for related early work (see reference ). We thank the ANR (grant DYNAFUN), the ERC (Advanced Research Grant SUPRADAPT 290585), the University of Strasbourg Institute of Advanced Study (USIAS), the International Center for Frontier Research in Chemistry (icFRC) for financial support. A.S. thanks Prof. Sebastiano Campagna and the University of Messina for the Nanosolar project fellowship and the University of Strasbourg for a post‐doctoral fellowship. J.H. thanks the University of Strasbourg for a doctoral fellowship. M.A.F.J. thanks Prof. Violetta Patroniak and the French Embassy in Poland for the project fellowship, the University of Strasbourg for a research fellowship and National Science Centre in Poland (grant no. 2017/24/C/ST5/00181) for financial support. G.V. thanks the Ministère de l'Enseignement Supérieur et de la Recherche for a doctoral fellowship.

FundersFunder number
French Embassy in Poland
University of Messina for the Nanosolar
Centre International de Recherche aux Frontières de la Chimie
Seventh Framework Programme290585
European Research Council
Agence Nationale de la Recherche
Université de Strasbourg
Narodowe Centrum Nauki2017/24/C/ST5/00181
Ministère de l'Enseignement Supérieur et de la Recherche

    Keywords

    • double-helical structures
    • dynamic covalent chemistry
    • metallo-supramolecular structures
    • programmed self-assembly

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