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Quantitative and Mechanistic Mechanochemistry in Ferrocene Dissociation
Ye Sha1, Yudi Zhang2, Enhua Xu3
1Department of Chemistry and Biochemistry, University of South Carolina, Columbia, South Carolina 29208, United States.
ACS Macro Letters
|May 18, 2019
Summary
Ferrocene
Area of Science:
- Polymer Chemistry
- Organometallic Chemistry
- Materials Science
Background:
- Ferrocene is typically considered inert due to strong metal-cyclopentadienyl (Cp) bonds.
- Understanding bond lability under mechanical stress is crucial for polymer applications.
Purpose of the Study:
- To investigate the mechanochemical scission site in ferrocene-containing polymers.
- To elucidate the mechanism and energetics of Fe-Cp bond cleavage under ultrasonication.
Main Methods:
- Pulsed ultrasonication of polybutadiene-derived polymers with ferrocene.
- Quantitative bond strength analysis.
- Density Functional Theory (DFT) calculations.
Main Results:
- The iron-cyclopentadienyl (Fe-Cp) bond is the primary site of mechanochemical scission.
- Fe-Cp bond strength is comparable to labile azo initiator bonds.
- Mechanistic studies suggest a heterolytic scission pathway.
Conclusions:
- Ferrocene's Fe-Cp bond exhibits unexpected mechanical lability.
- Ultrasonication can selectively cleave ferrocene units in polymers.
- DFT calculations explain the origins of this mechanical weakness.
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