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Hypercoordinated Oligosilanes Based on Aminotrisphenols.

Mohammad Aghazadeh Meshgi1, Kirill V Zaitsev2, Mikhail V Vener3

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This study synthesized novel catenated silicon compounds using hypercoordinated silicon chlorides. The choice of solvate for potassium tris(trimethylsilyl)silanide dictates the reaction outcome, yielding different silicon chain structures.

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Area of Science:

  • Organosilicon Chemistry
  • Materials Science
  • Coordination Chemistry

Background:

  • Hypercoordinated silicon compounds are of interest due to their unique bonding and reactivity.
  • The synthesis of silicon-carbon and silicon-silicon bonds is crucial for developing new materials.
  • Understanding the influence of ligands on silicon coordination is key to controlling synthetic outcomes.

Purpose of the Study:

  • To synthesize novel catenated silicon derivatives using hypercoordinated silicon chlorides.
  • To investigate the effect of the potassium tris(trimethylsilyl)silanide solvate on the reaction pathway and product formation.
  • To characterize the synthesized compounds and elucidate their molecular structures.

Main Methods:

  • Synthesis of hypercoordinated silicon chlorides and catenated derivatives.
  • Reactions with potassium tris(trimethylsilyl)silanide solvates (THF and 18-crown-6).
  • Characterization using multinuclear NMR, UV-vis spectroscopy, and mass spectrometry.
  • Structural analysis via single-crystal X-ray diffraction.
  • Computational analysis using crystal density functional theory (DFT).

Main Results:

  • Successful synthesis of several catenated silicon compounds, including tris(trimethylsilyl)silyl derivatives.
  • Demonstrated that the solvate of potassium tris(trimethylsilyl)silanide influences product distribution, leading to either catenated products or unexpected side products.
  • X-ray analysis revealed hypercoordinated silicon atoms in a trigonal-bipyramidal environment.
  • DFT calculations confirmed weak Si←N interactions in a side product, with Si···N distances ranging from 2.23-2.78 Å.
  • Established correlations between structural features, NMR parameters, and ligand type in hypercoordinated catenated silicon compounds.

Conclusions:

  • The synthetic route provides access to novel hypercoordinated and catenated silicon structures.
  • Solvate effects play a critical role in directing the reactivity of potassium tris(trimethylsilyl)silanide.
  • The structural and spectroscopic data provide insights into the nature of hypercoordination and bonding in these silicon compounds.