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Dynamic Helicates Self-Assembly from Homo- and Heterotopic Dynamic Covalent Ligand Strands
Authors:Dr. Antonio Santoro  Dr. Jan Holub  Dr. Marta A. Fik-Jaskółka  Dr. Ghislaine Vantomme  Prof. Dr. Jean-Marie Lehn
Affiliation:1. Laboratoire de Chimie Supramoléculaire, ISIS, Université de Strasbourg, 8 Allée Gaspard Monge, 67000 Strasbourg, France

Present address: Department of Chemical, Biological, Pharmaceutical and Environmental Sciences, University of Messina, Viale F. Stagno d'Alcontres 31, 98166 Messina, Italy;2. Laboratoire de Chimie Supramoléculaire, ISIS, Université de Strasbourg, 8 Allée Gaspard Monge, 67000 Strasbourg, France

Present address: Institute of Chemical Research of Catalonia (ICIQ), Avinguda Països Catalans 16, 43007 Tarragona, Spain;3. Laboratoire de Chimie Supramoléculaire, ISIS, Université de Strasbourg, 8 Allée Gaspard Monge, 67000 Strasbourg, France

Present address: Faculty of Chemistry, Adam Mickiewicz University, Uniwersytetu Poznańskiego 8, 61-614 Poznań, Poland

Present address: Centre for Advanced Technology, Adam Mickiewicz University, Uniwersytetu Poznańskiego 10, 61-614 Poznań, Poland;4. Laboratoire de Chimie Supramoléculaire, ISIS, Université de Strasbourg, 8 Allée Gaspard Monge, 67000 Strasbourg, France

Present address: Institute for Complex Molecular Systems, Laboratory of Macromolecular and Organic Chemistry, Eindhoven University of Technology, P.O. Box 513, 5600, MB Eindhoven, The Netherlands;5. Laboratoire de Chimie Supramoléculaire, ISIS, Université de Strasbourg, 8 Allée Gaspard Monge, 67000 Strasbourg, France

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.
Keywords:double-helical structures  dynamic covalent chemistry  metallo-supramolecular structures  programmed self-assembly
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