The activation mechanism of Ru-indenylidene complexes in olefin metathesis

César A. Urbina-Blanco, Albert Poater, Tomáš Lébl, Simone Manzini, Alexandra M. Z. Slawin, Luigi Cavallo, Steven P. Nolan

Research output: Contribution to journalArticlepeer-review

96 Scopus citations

Abstract

Olefin metathesis is a powerful tool for the formation of carbon-carbon double bonds. Several families of well-defined ruthenium (Ru) catalysts have been developed during the past 20 years; however, the reaction mechanism for all such complexes was assumed to be the same. In the present study, the initiation mechanism of Ru-indenylidene complexes was examined and compared with that of benzylidene counterparts. It was discovered that not all indenylidene complexes followed the same mechanism, highlighting the importance of steric and electronic properties of so-called spectator ligands, and that there is no single mechanism for the Ru-based olefin metathesis reaction. The experimental findings are supported quantitatively by DFT calculations. © 2013 American Chemical Society.
Original languageEnglish (US)
Pages (from-to)7073-7079
Number of pages7
JournalJournal of the American Chemical Society
Volume135
Issue number18
DOIs
StatePublished - Apr 25 2013

Bibliographical note

KAUST Repository Item: Exported on 2020-10-01
Acknowledgements: The research leading to these results has received funding from the European Community's Seventh Framework Programme (FP7/2007-2013) under grant agreement no CP-FP 211468-2 EUMET. SPN is a Royal Society Wolfson Research Merit Award holder. LC thanks BSC (QCM-2010-2-0020), and the HPC team of Enea for using the ENEA-GRID and the HPC facilities CRESCO in Portici (Italy) for access to remarkable computational resources. AP thanks the Spanish MICINN for a Ramon y Cajal contract (RYC-2009-05226), Generalitat de Catalunya (2012BE100824) and European Commission for a Career Integration Grant (CIG09-GA-2011-293900). Dr Julie Broggi is greatly acknowledged for preliminary research leading to this publication, Dr David J. Nelson and Prof. Fernando Febres Cordero are greatly acknowledged for helpful discussions. Umicore is greatly acknowledged for their generous donation of materials.

ASJC Scopus subject areas

  • Biochemistry
  • Colloid and Surface Chemistry
  • General Chemistry
  • Catalysis

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