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Wetting the lock and key enthalpically favours polyelectrolyte binding

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Abstract

By using a combination of readily accessible experimental and computational experiments in water, we explored the factors governing the association between polyanionic dyn[4]arene and a series of α,ω-alkyldiammonium ions of increasing chain length. We found that the lock-and-key concept based on the best match between the apolar and polar regions of the molecular partners failed to explain the observed selectivities. Instead, the dissection of the energetic and structural contributions demonstrated that the binding events were actually guided by two crucial solvent-related phenomena as the chain length of the guest increases: the expected decrease of the enthalpic cost of guest desolvation and the unexpected increase of the favourable enthalpy of complex solvation. By bringing to light the decisive enthalpic impact of complex solvation during the binding of polyelectrolytes by inclusion, this study may provide a missing piece to a puzzle that one day could display the global picture of molecular recognition in water.

Graphical abstract: Wetting the lock and key enthalpically favours polyelectrolyte binding

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Publication details

The article was received on 05 Jul 2018, accepted on 06 Oct 2018 and first published on 08 Oct 2018


Article type: Edge Article
DOI: 10.1039/C8SC02966K
Citation: Chem. Sci., 2018, Advance Article
  • Open access: Creative Commons BY-NC license
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    Wetting the lock and key enthalpically favours polyelectrolyte binding

    E. Jeamet, J. Septavaux, A. Héloin, M. Donnier-Maréchal, M. Dumartin, B. Ourri, P. Mandal, I. Huc, E. Bignon, E. Dumont, C. Morell, J. Francoia, F. Perret, L. Vial and J. Leclaire, Chem. Sci., 2018, Advance Article , DOI: 10.1039/C8SC02966K

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