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Intermolecular Forces03:13

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Atoms and molecules interact through bonds (or forces): intramolecular and intermolecular. The forces are electrostatic as they arise from interactions (attractive or repulsive) between charged species (permanent, partial, or temporary charges) and exist with varying strengths between ions, polar, nonpolar, and neutral molecules. The different types of intermolecular forces are ion–dipole, dipole–dipole, hydrogen bonds, and dispersion; among these, dipole–dipole, hydrogen bonds, and dispersion...
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Heterogeneous Removal of Water-Soluble Ruthenium Olefin Metathesis Catalyst from Aqueous Media Via Host-Guest Interaction
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A cationic host displaying positive cooperativity in water.

Andrew D Hughes1, Eric V Anslyn

  • 1Department of Chemistry and Biochemistry, University of Texas, Austin, TX 78712, USA.

Proceedings of the National Academy of Sciences of the United States of America
|April 11, 2007
PubMed
Summary

Researchers studied host-guest binding using guanidinium and copper(II) hosts. They observed rare positive cooperativity in water, driven by enthalpy, enhancing binding affinity for polycarboxylate guests.

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Area of Science:

  • Supramolecular Chemistry
  • Coordination Chemistry
  • Host-Guest Chemistry

Background:

  • Guanidinium and Cu(II) moieties are known to bind polycarboxylates.
  • Positive cooperativity in synthetic host-guest systems in water is rare.
  • Understanding binding mechanisms is crucial for designing new materials.

Purpose of the Study:

  • To investigate the binding affinity of hosts containing both guanidinium and Cu(II) for polycarboxylate guests in water.
  • To explore the phenomenon of positive cooperativity in this synthetic host-guest system.
  • To elucidate the thermodynamic origin of the observed positive cooperativity.

Main Methods:

  • UV-visible spectroscopy to monitor binding interactions.
  • Isothermal titration calorimetry (ITC) to determine thermodynamic parameters.
  • Synthesis of a single scaffold incorporating both Cu(II) coordination site and diguanidinium moiety.

Main Results:

  • The combined guanidinium and Cu(II) host exhibited enhanced Gibbs free-energy release upon binding polycarboxylates compared to isolated moieties.
  • Positive cooperativity was observed, indicating synergistic binding.
  • ITC data revealed the positive cooperativity is enthalpically driven.
  • Proximity of cationic binding groups destabilizes the unbound host, amplifying binding exothermicity.

Conclusions:

  • Covalently linking guanidinium and Cu(II) binding sites on a single scaffold leads to significant positive cooperativity in polycarboxylate binding in water.
  • The observed positive cooperativity is primarily enthalpic, arising from pre-organization effects that destabilize the unbound host.
  • This study provides insights into designing synthetic receptors with enhanced binding affinities through cooperative effects.