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

Electronic International Standard Serial Number (EISSN)

  • 1520-5126

International Standard Serial Number (ISSN)

  • 0002-7863

Digital Object Identifier (DOI)

  • 10.1021/jacs.0c13219


  • eng