Jump to main content
Jump to site search


Insight into Catalyst Speciation and Hydrogen Co-Evolution during Enantioselective Formic Acid-driven Transfer Hydrogenation with Bifunctional Ruthenium Complexes from Multi-technique operando Reaction Monitoring

Abstract

Transfer hydrogenation of acetophenone from formic acid / triethylamine mixtures catalysed by the Ikariya-Noyori complex [(mesitylene)RuCl(R,R)-(TsDPEN)] has been investiated by simultaneous high-resolution FlowNMR and FlowUV-Vis spectroscopies coupled with on-line sampling head-space mass spectrometry and chiral high-performance liquid chromatography using an integrated, fully automated recirculating flow setup. In line with previous observations, our combined results show a gradual switch from formic acid dehydrogenation to hydrogen transfer mediated by the same Ru-hydride complex, and point a Ru-formate species as the major catalyst intermediate. Hydrogen bonding in the formic acid / triethylamine mixture emerges as a sensitive 1H NMR probe for the transfer hydrogenation activity of the system.

Back to tab navigation

Supplementary files

Publication details

The article was received on 03 May 2019, accepted on 11 Jun 2019 and first published on 11 Jun 2019


Article type: Paper
DOI: 10.1039/C9FD00060G
Faraday Discuss., 2019, Accepted Manuscript
  • Open access: Creative Commons BY license
  •   Request permissions

    Insight into Catalyst Speciation and Hydrogen Co-Evolution during Enantioselective Formic Acid-driven Transfer Hydrogenation with Bifunctional Ruthenium Complexes from Multi-technique operando Reaction Monitoring

    D. Berry, I. Clegg, A. Codina, C. Lyall, J. P. Lowe and U. Hintermair, Faraday Discuss., 2019, Accepted Manuscript , DOI: 10.1039/C9FD00060G

    This article is licensed under a Creative Commons Attribution 3.0 Unported Licence. Material from this article can be used in other publications provided that the correct acknowledgement is given with the reproduced material.

    Reproduced material should be attributed as follows:

    • For reproduction of material from NJC:
      [Original citation] - Published by The Royal Society of Chemistry (RSC) on behalf of the Centre National de la Recherche Scientifique (CNRS) and the RSC.
    • For reproduction of material from PCCP:
      [Original citation] - Published by the PCCP Owner Societies.
    • For reproduction of material from PPS:
      [Original citation] - Published by The Royal Society of Chemistry (RSC) on behalf of the European Society for Photobiology, the European Photochemistry Association, and RSC.
    • For reproduction of material from all other RSC journals:
      [Original citation] - Published by The Royal Society of Chemistry.

    Information about reproducing material from RSC articles with different licences is available on our Permission Requests page.

Search articles by author

Spotlight

Advertisements