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Mechanochemistry of Cationic Cobaltocenium Mechanophore.
J Am Chem Soc
August 2021
Department of Chemistry and Biochemistry, University of South Carolina, Columbia, South Carolina 29208, United States.
Recent research on the mechanochemistry of metallocene mechanophores has shed light on the force-responsiveness of these thermally and chemically stable organometallic compounds. In this work, we report a combination of experimental and computational studies on the mechanochemistry of main-chain cobaltocenium-containing polymers. Ester derivatives of the cationic cobaltocenium, though isoelectronic to neutral ferrocene, are unstable in the nonmechanical control experimental conditions that were accommodated by their ferrocene analogs.
View Article and Find Full Text PDFDistal conformational locks on ferrocene mechanophores guide reaction pathways for increased mechanochemical reactivity.
Nat Chem
January 2021
Department of Chemistry, Duke University, Durham, NC, USA.
Mechanophores can be used to produce strain-dependent covalent chemical responses in polymeric materials, including stress strengthening, stress sensing and network remodelling. In general, it is desirable for mechanophores to be inert in the absence of force but highly reactive under applied tension. Metallocenes possess potentially useful combinations of force-free stability and force-coupled reactivity, but the mechanistic basis of this reactivity remains largely unexplored.
View Article and Find Full Text PDFGeneralizing metallocene mechanochemistry to ruthenocene mechanophores.
Chem Sci
May 2019
Department of Chemistry and Biochemistry , University of South Carolina, Columbia , South Carolina 29208 , USA . Email:
Recent reports have shown that ferrocene displays an unexpected combination of force-free stability and mechanochemical activity, as it acts as the preferred site of chain scission along the backbone of highly extended polymer chains. This observation raises the tantalizing question as to whether similar mechanochemical activity might be present in other metallocenes, and, if so, what features of metallocenes dictate their relative ability to act as mechanophores. In this work, we elucidate polymerization methodologies towards main-chain ruthenocene-based polymers and explore the mechanochemistry of ruthenocene.
View Article and Find Full Text PDFMetallocene as Mechanophore in Polymers Leads to Metal Ion Release & Oxidation.
Chimia (Aarau)
December 2018
Department of Chemistry, University of Fribourg, Switzerland;, Email:
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