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Hydroxide ion adsorption on self-assembled monolayers.

H Jürgen Kreuzer1, Richard L C Wang, Michael Grunze

  • 1Department of Physics and Atmospheric Science, Dalhousie University, Halifax, Nova Scotia B3H 3J5, Canada. h.j.kreuzer@dal.ca

Journal of the American Chemical Society
|July 3, 2003
PubMed
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Self-assembled monolayers (SAMs) in water preferentially adsorb hydroxyl ions, leading to negative surface charging. This phenomenon explains long-range forces between SAM surfaces and is influenced by hydration effects.

Area of Science:

  • Surface Science
  • Physical Chemistry
  • Computational Materials Science

Background:

  • Self-assembled monolayers (SAMs) are crucial in surface modification.
  • Understanding surface charge in aqueous environments is vital for interfacial phenomena.
  • Oligo(ethylene glycol) and n-alkane SAMs are common models for studying interfacial properties.

Purpose of the Study:

  • To investigate the preferential adsorption of ions on SAMs in contact with water.
  • To elucidate the mechanism of surface charging for different SAM terminations.
  • To explain the origin of long-range forces between opposing SAMs.

Main Methods:

  • Density functional calculations were employed to model ion adsorption.
  • The Born-Haber cycle was used to calculate excess binding energies.

Related Experiment Videos

  • Simulations considered methoxy- and hydroxide-terminated endgroups.

    • Main Results:

    • SAMs preferentially adsorb hydroxyl ions, resulting in negative surface charging.
    • An estimated charge density of approximately 1 microC/cm(2) was determined, aligning with experimental data.
    • Hydroxyl ion mobility within dense SAMs was observed, and hydronium ion penetration was analyzed.

    Conclusions:

    • The preferential adsorption of hydroxyl ions on SAMs leads to negative surface charge.
    • This negative charging mechanism explains observed long-range forces between SAM surfaces.
    • Hydration plays a critical role in the adsorption energetics and interfacial behavior of SAMs.