Bimetallic rhodium complexes: precatalyst activation-triggered bimetallic enhancement for the hydrosilylation transformation

Raphael H. Lam, Sinead T. Keaveney, Barbara A. Messerle, Indrek Pernik*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

6 Citations (Scopus)

Abstract

To explore how to access bimetallic catalysts that can outperform their monometallic analogues, a set of mono- and bimetallic NHC/phosphine (NHC = N-heterocyclic carbene)-ligated rhodium(I) complexes were designed, synthesized, and characterized. The complexes were used as catalysts for the intermolecular hydrosilylation of diphenylacetylene. All four catalysts displayed significantly faster catalytic rates than the related complexes reported previously containing NHC/pyrazolyl donor ligands. The bimetallic catalyst design led to enhanced catalytic activity over the monometallic analogue. The data revealed that the degree of bimetallic enhancement was highly dependent on the reaction conditions, coligands used, and the substrate addition order. The catalytic trends, in combination with mechanistic studies using individual substrates and density functional theory calculations, exposed that the bimetallic benefits were strongly linked to the catalyst activation procedure.

Original languageEnglish
Pages (from-to)1999-2010
Number of pages12
JournalACS Catalysis
Volume13
Issue number3
Early online date23 Jan 2023
DOIs
Publication statusPublished - 3 Feb 2023

Keywords

  • bimetallic catalyst
  • bimetallic enhancement
  • hydrosilylation
  • reaction mechanism
  • rhodium

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