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14-electron disilene palladium complex having strong pi-complex character.

Mitsuo Kira1, Yumiko Sekiguchi, Takeaki Iwamoto

  • 1Department of Chemistry, Graduate School of Science, Tohoku University, Aoba-ku, Sendai 980-8578, Japan. mkira@si.chem.tohoku.ac.jp

Journal of the American Chemical Society
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The synthesis of a novel 14-electron palladium-disilene complex was achieved, exhibiting unique bonding characteristics and strong pi-complex character. This finding advances the understanding of organometallic compounds and their electronic properties.

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Area of Science:

  • Organometallic Chemistry
  • Inorganic Chemistry
  • Materials Science

Background:

  • Disilenes are silicon analogs of alkenes, offering unique electronic and structural properties.
  • Palladium complexes with unsaturated ligands are crucial in catalysis and materials science.
  • Understanding the bonding modes of disilenes in metal complexes is key to predicting their reactivity.

Purpose of the Study:

  • To synthesize and characterize the first 14-electron disilene palladium complex.
  • To investigate the structural and electronic differences between 14-electron and 16-electron disilene palladium complexes.
  • To determine the extent of pi-complex character in the novel palladium-disilene complex.

Main Methods:

  • Synthesis of the 14-electron disilene palladium complex eta2-[tetrakis(tert-butyldimethylsilyl)disilene](tricyclohexylphosphine)palladium (4).
  • Solid-state structural analysis using X-ray crystallography.
  • Nuclear Magnetic Resonance (NMR) spectroscopy for electronic and dynamic studies.

Main Results:

  • Complex 4 was successfully synthesized, featuring unsymmetrical binding of the tricyclohexylphosphine ligand.
  • The Si-Si bond elongation and disilene moiety bending in complex 4 were significantly smaller compared to a 16-electron analog.
  • Complex 4 displayed the strongest pi-complex character among known disilene complexes.
  • NMR spectra indicated equivalent central Si nuclei and facile phosphine ligand flipping.

Conclusions:

  • The 14-electron palladium-disilene complex exhibits distinct structural and electronic properties compared to its 16-electron counterpart.
  • Complex 4 represents a significant advancement in the study of disilene coordination chemistry.
  • The observed facile ligand dynamics provide insights into the electronic environment within the complex.