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First-Principles Prediction of Surface Wetting.

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Summary
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We developed a new method to predict solid-liquid interfacial tension (IFT) and wetting behavior using density functional theory and COSMO-RS. This approach shows good agreement with experimental data for various surfaces, aiding in understanding interfacial properties.

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Area of Science:

  • Physical Chemistry
  • Materials Science
  • Computational Chemistry

Background:

  • Solid-liquid interfacial tension (IFT) is crucial for understanding wetting phenomena.
  • Direct experimental measurement of solid-liquid IFT is challenging.
  • Accurate prediction methods are needed for materials design and process optimization.

Purpose of the Study:

  • To develop and validate a computational method for predicting the solvation contribution to solid-liquid IFT.
  • To assess the method's accuracy in predicting wetting behavior for diverse solid surfaces.
  • To provide a reliable tool for situations where direct IFT measurement is not feasible.

Main Methods:

  • Utilized density functional theory (DFT) combined with the COSMO-RS implicit solvent model.
  • Calculated solid-liquid IFT by incorporating solvation effects.
  • Benchmarked predictions against experimental contact angle measurements for silica wafers and self-assembled monolayers (SAMs).

Main Results:

  • The developed method accurately predicted wetting behavior for oil-wet to water-wet surfaces, including silica and carboxylic acid SAMs, when deprotonation was considered.
  • Good agreement was observed between predicted and experimental contact angles for most surfaces.
  • Discrepancies were noted for amine-terminated SAMs, potentially due to method limitations or surface impurities.

Conclusions:

  • The DFT and COSMO-RS based method provides a valuable tool for predicting solid-liquid IFT and wetting behavior.
  • Explicitly including surface deprotonation significantly improves prediction accuracy for certain materials.
  • The method's importance is highlighted by the difficulty in directly measuring solid-liquid IFT.