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Single-Molecule Activation and Quantification of Mechanically Triggered Palladium-Carbene Bond Dissociation.

Publication ,  Journal Article
Razgoniaev, AO; Glasstetter, LM; Kouznetsova, TB; Hall, KC; Horst, M; Craig, SL; Franz, KJ
Published in: Journal of the American Chemical Society
February 2021

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.

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Published In

Journal of the American Chemical Society

DOI

EISSN

1520-5126

ISSN

0002-7863

Publication Date

February 2021

Volume

143

Issue

4

Start / End Page

1784 / 1789

Related Subject Headings

  • General Chemistry
  • 40 Engineering
  • 34 Chemical sciences
  • 03 Chemical Sciences
 

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Razgoniaev, A. O., Glasstetter, L. M., Kouznetsova, T. B., Hall, K. C., Horst, M., Craig, S. L., & Franz, K. J. (2021). Single-Molecule Activation and Quantification of Mechanically Triggered Palladium-Carbene Bond Dissociation. Journal of the American Chemical Society, 143(4), 1784–1789. https://doi.org/10.1021/jacs.0c13219
Razgoniaev, Anton O., Logan M. Glasstetter, Tatiana B. Kouznetsova, Kacey C. Hall, Matias Horst, Stephen L. Craig, and Katherine J. Franz. “Single-Molecule Activation and Quantification of Mechanically Triggered Palladium-Carbene Bond Dissociation.Journal of the American Chemical Society 143, no. 4 (February 2021): 1784–89. https://doi.org/10.1021/jacs.0c13219.
Razgoniaev AO, Glasstetter LM, Kouznetsova TB, Hall KC, Horst M, Craig SL, et al. Single-Molecule Activation and Quantification of Mechanically Triggered Palladium-Carbene Bond Dissociation. Journal of the American Chemical Society. 2021 Feb;143(4):1784–9.
Razgoniaev, Anton O., et al. “Single-Molecule Activation and Quantification of Mechanically Triggered Palladium-Carbene Bond Dissociation.Journal of the American Chemical Society, vol. 143, no. 4, Feb. 2021, pp. 1784–89. Epmc, doi:10.1021/jacs.0c13219.
Razgoniaev AO, Glasstetter LM, Kouznetsova TB, Hall KC, Horst M, Craig SL, Franz KJ. Single-Molecule Activation and Quantification of Mechanically Triggered Palladium-Carbene Bond Dissociation. Journal of the American Chemical Society. 2021 Feb;143(4):1784–1789.
Journal cover image

Published In

Journal of the American Chemical Society

DOI

EISSN

1520-5126

ISSN

0002-7863

Publication Date

February 2021

Volume

143

Issue

4

Start / End Page

1784 / 1789

Related Subject Headings

  • General Chemistry
  • 40 Engineering
  • 34 Chemical sciences
  • 03 Chemical Sciences