Single-Molecule Activation and Quantification of Mechanically Triggered Palladium-Carbene Bond Dissociation.
Journal Article (Journal Article)
Metal-complexed N-heterocyclic carbene (NHC) mechanophores are latent reactants and catalysts for a range of mechanically driven chemical responses, but mechanochemical scission of the metal-NHC bond has not been experimentally characterized. Here we report the single-molecule force spectroscopy of ligand dissociation from a pincer NHC-pyridine-NHC Pd(II) complex. The force-coupled rate constant for ligand dissociation reaches 50 s-1 at forces of approximately 930 pN. Experimental and computational observations support a dissociative, rather than associative, mechanism of ligand displacement, with rate-limiting scission of the Pd-NHC bond followed by rapid dissociation of the pyridine moiety from Pd.
Full Text
Duke Authors
Cited Authors
- Razgoniaev, AO; Glasstetter, LM; Kouznetsova, TB; Hall, KC; Horst, M; Craig, SL; Franz, KJ
Published Date
- February 2021
Published In
Volume / Issue
- 143 / 4
Start / End Page
- 1784 - 1789
PubMed ID
- 33480680
Pubmed Central ID
- 33480680
Electronic International Standard Serial Number (EISSN)
- 1520-5126
International Standard Serial Number (ISSN)
- 0002-7863
Digital Object Identifier (DOI)
- 10.1021/jacs.0c13219
Language
- eng