Evidence for metal-surface interactions and their role in stabilizing Well-defined immobilized Ru-NHC alkene metathesis catalysts

Manoja Samantaray, Johan Alauzun, David Gajan, Santosh Kavitake, Ahmad Mehdi, Laurent Veyre, Moreno Lelli, Anne Lesage, Lyndon Emsley, Christophe Copéret*, Chloé Thieuleux

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

82 Scopus citations

Abstract

Secondary interactions are demonstrated to direct the stability of well-defined Ru-NHC-based heterogeneous alkene metathesis catalysts. By providing key stabilization of the active sites, higher catalytic performance is achieved. Specifically, they can be described as interactions between the metal center (active site) and the surface functionality of the support, and they have been detected by surface-enhanced 1 H- 29 Si NMR spectroscopy of the ligand and 31 P solid-state NMR of the catalyst precursor. They are present only when the metal center is attached to the surface via a flexible linker (a propyl group), which allows the active site to either react with the substrate or relax, reversibly, to the surface, thus providing stability. In contrast, the use of a rigid linker (here mesitylphenyl) leads to a well-defined active site far away from the surface, stabilized only by a phosphine ligand which under reaction conditions leaves probably irreversibly, leading to faster decomposition and deactivation of the catalysts.

Original languageEnglish (US)
Pages (from-to)3193-3199
Number of pages7
JournalJournal of the American Chemical Society
Volume135
Issue number8
DOIs
StatePublished - Mar 11 2013

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)
  • Biochemistry
  • Colloid and Surface Chemistry

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