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Reversible pH-Controlled Catenation of a Benzobisimidazole-Based Tetranuclear Rectangle
Authors:Maksym Dekhtiarenko  Dr Simon Pascal  Dr Mourad Elhabiri  Valerie Mazan  Dr David Canevet  Magali Allain  Dr Vincent Carré  Prof Frédéric Aubriet  Prof Zoia Voitenko  Prof Marc Sallé  Dr Olivier Siri  Dr Sébastien Goeb
Institution:1. Univ Angers, CNRS, MOLTECH-Anjou, 2 bd Lavoisier, 49045 Angers, France

Taras Shevchenko National University of Kyiv, 64/13 Volodymyrska st., Kyiv, 01033 Ukraine;2. Aix Marseille Univ, CNRS UMR 7325, Centre Interdisciplinaire de Nanoscience de Marseille (CINaM), Campus de Luminy, 13288 Marseille cedex 09, France;3. Université de Strasbourg, Université de Haute-Alsace, CNRS, LIMA, UMR 7042, Equipe Chimie Bioorganique et Médicinale, ECPM, 25 Rue Becquerel, 67000 Strasbourg, France;4. Univ Angers, CNRS, MOLTECH-Anjou, 2 bd Lavoisier, 49045 Angers, France;5. LCP-A2MC, FR 3624, Université de Lorraine, ICPM, 1 Bd Arago, 57078 Metz Cedex 03, France;6. Taras Shevchenko National University of Kyiv, 64/13 Volodymyrska st., Kyiv, 01033 Ukraine

Abstract:The development of methodologies to control on demand and reversibly supramolecular transformations from self-assembled metalla-structures requires the rational design of architectures able to answer to an applied stimulus. While solvent or concentration changes, light exposure or addition of a chemical have been largely explored to provide these transformations, the case of pH sensitive materials is less described. Herein, we report the first example of a pH-triggered dissociation of a coordination-driven self-assembled interlocked molecular link. It incorporates a pH sensitive benzobisimidazole-based ligand that can be selectively protonated on its bisimidazole moieties. This generates intermolecular electrostatic repulsions that reduces drastically the stability of the interlocked structure, leading to its dissociation without any sign of protonation of the pyridine moieties involved in the coordination bonds. Importantly, the dissociation process is reversible through addition of a base.
Keywords:benzobis(imidazole)  host?guest systems  metalla-cycles  self-assembly  pH  catenation
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