Redox-switched oxidation of dihydrogen using a non-innocent ligand

Mark R. Ringenberg, Swarna Latha Kokatam, Zachariah M. Heiden, Thomas B. Rauchfuss

Research output: Contribution to journalArticlepeer-review

Abstract

Organometallic complexes containing non-innocent ligands of the type Cp*Ir(tBAFPh)(1), where H2tBAFPh is 2-(2-trifluoromethyl)anilino-4,6-di-tert-butylphenol, were found to activate H2 in a redox-switchable manner. The 16e- complex 1 was inert with respect to H2, CO, as well as conventional basic substrates until oxidation. Oxidation of 16-electron 1 with 1 equiv of Ag+ resulted in ligand-centered oxidation affording salts of [1]+, which were characterized by crystallographically, EPR, and elemental analyses. [1]+ was reduced to 1 in the presence of H2 and the sterically hindered base, 2,6-(tBu)2C5H3N, via a pathway that is first-order in both metal and dihydrogen. Compound [1]+ forms adducts with MeCN, which inhibits catalysis. The catalytic oxidation of H2 was established by electrochemical methods to be associated with the monocation.

Original languageEnglish (US)
Pages (from-to)788-789
Number of pages2
JournalJournal of the American Chemical Society
Volume130
Issue number3
DOIs
StatePublished - Jan 23 2008

ASJC Scopus subject areas

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

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