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Stand up for Electrostatics: The Disiloxane Case.

Carlos Martín-Fernández1, Ibon Alkorta2, M Merced Montero-Campillo3

  • 1Department of Chemistry, KU Leuven, Celestijnenlaan, 200F, 3001, Leuven, Belgium.

Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry
|March 2, 2022
PubMed
Summary

The Si-O-Si angle in disiloxane significantly influences its basicity. Molecular electrostatic potential (MEP) explains how this angle affects electrostatic interactions and tetrel bonds, crucial for understanding silicone chemistry.

Keywords:
basicitycooperative effectsmolecular electrostatic potentialnoncovalent interactionssiloxanes

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Area of Science:

  • Computational Chemistry
  • Materials Science
  • Quantum Chemistry

Background:

  • The basicity of silicones, like disiloxane, is a critical property influencing their chemical behavior and applications.
  • The Si-O-Si bond angle (α) is known to affect molecular properties, but its specific impact on disiloxane basicity requires detailed investigation.

Purpose of the Study:

  • To investigate the influence of the Si-O-Si angle (α) on the basicity of disiloxane (H₃Si-O-SiH₃).
  • To analyze the role of molecular electrostatic potential (MEP) in explaining the observed changes in basicity and non-covalent interactions.
  • To explore the cooperative effects in ternary complexes involving disiloxane, Lewis acids, and Lewis bases across varying α values.

Main Methods:

  • High-level ab initio calculations using the MP2/aug'-cc-pVTZ method.
  • Analysis of molecular electrostatic potential (MEP) to rationalize electrostatic interactions.
  • Investigation of tetrel bonds and cooperative effects in binary and ternary complexes.

Main Results:

  • Disiloxane basicity increases significantly as the Si-O-Si angle (α) decreases, which is well-explained by MEP analysis.
  • The MEP accurately rationalizes the effect of α on tetrel bonds formed between disiloxane and Lewis bases.
  • Non-covalent interactions in ternary complexes remain cooperative across all α values, though maximum binding energy doesn't always correlate with maximum cooperativity.

Conclusions:

  • The Si-O-Si angle is a key determinant of disiloxane basicity, primarily through electrostatic interactions.
  • Molecular electrostatic potential (MEP) serves as a powerful tool for predicting and understanding non-covalent interactions in silicones.
  • Understanding these angle-dependent interactions is crucial for designing silicone-based materials with tailored properties.