Well-Defined Cobalt(I) Dihydrogen Catalyst: Experimental Evidence for a Co(I)/Co(III) Redox Process in Olefin Hydrogenation

Kenan Tokmic, Charles R. Markus, Lingyang Zhu, Alison R. Fout

Research output: Contribution to journalArticlepeer-review

Abstract

The synthesis of a cobalt dihydrogen CoI-(H2) complex prepared from a CoI-(N2) precursor supported by a monoanionic pincer bis(carbene) ligand, MesCCC (MesCCC = bis(mesityl-benzimidazol-2-ylidene)phenyl), is described. This species is capable of H2/D2 scrambling and hydrogenating alkenes at room temperature. Stoichiometric addition of HCl to the CoI-(N2) cleanly affords the CoIII hydridochloride complex, which, upon the addition of Cp2ZrHCl, evolves hydrogen gas and regenerates the CoI-(N2) complex. Furthermore, the catalytic olefin hydrogenation activity of the CoI species was studied by using multinuclear and parahydrogen (p-H2) induced polarization (PHIP) transfer NMR studies to elucidate catalytically relevant intermediates, as well as to establish the role of the CoI-(H2) in the CoI/CoIII redox cycle.

Original languageEnglish (US)
Pages (from-to)11907-11913
Number of pages7
JournalJournal of the American Chemical Society
Volume138
Issue number36
DOIs
StatePublished - Sep 14 2016

ASJC Scopus subject areas

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

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