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The first stable mononuclear silyl palladium hydrides.
Robert C Boyle1, Joel T Mague, Mark J Fink
1Department of Chemistry, Tulane University, New Orleans, LA 70118, USA.
Journal of the American Chemical Society
|March 13, 2003
Summary
Tertiary silanes react with palladium complexes to form silyl palladium hydrides. These compounds exhibit unique, temperature-dependent silicon-hydride exchange, suggesting a novel intermediate complex.
Area of Science:
- Organometallic Chemistry
- Coordination Chemistry
- Spectroscopy
Background:
- Low-valent palladium complexes are versatile catalysts in organic synthesis.
- Tertiary silanes are important silicon-containing reagents.
- Understanding ligand exchange dynamics is crucial for reaction mechanism elucidation.
Purpose of the Study:
- To investigate the reaction products between tertiary silanes and a specific low-valent palladium complex.
- To characterize the resulting silyl palladium hydride complexes.
- To explore the dynamic behavior and fluxional processes of these complexes in solution.
Main Methods:
- Reaction of tertiary silanes with the dinuclear palladium complex [(mu-dcpe)Pd]2.
- Characterization using Nuclear Magnetic Resonance (NMR) spectroscopy.
- Structural determination via X-ray crystallography for one complex.
Main Results:
- Formation of equilibrium mixtures containing mononuclear silyl palladium hydrides.
- Observation of rapid interchange between silicon and hydride coordination environments.
- Detection of significant temperature-dependent kinetic isotope effects.
Conclusions:
- The observed fluxional process involves dynamic silicon-hydride exchange.
- A proposed intermediate, a 2-eta-Si-H complex, facilitates this interchange.
- These findings provide insights into the reactivity and dynamic nature of silyl palladium hydride complexes.
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