Electronic and geometric effects of phosphatriazaadamantane ligands on the catalytic activity of an [FeFe] hydrogenase inspired complex

Aaron K. Vannucci, Shihua Wang, Gary S. Nichol, Dennis L. Lichtenberger, Dennis H. Evans, Richard S. Glass

Research output: Contribution to journalArticle

51 Scopus citations

Abstract

The [FeFe] hydrogenase enzyme active site inspired complexes [Fe 2(μ-C6H4S2)(CO)5PTA] (1PTA) and [Fe2(μ-C6H4S2)(CO) 4PTA2] (1PTA2) (PTA = 1,3,5-triaza-7- phosphaadamantane) were synthesized and characterized. The ability of 1PTA and 1PTA2 to catalytically produce molecular hydrogen in solution from the weak acid acetic acid was examined electrochemically and compared to previous studies on the all carbonyl containing analogue [Fe2(μ- C6H4S2)(CO)6] (1). Computational methods and cyclic voltammograms indicated that the substitution of CO ligands by PTA in 1 resulted in markedly different reduction chemistry. Both 1PTA and 1PTA2 catalytically produce molecular hydrogen from acetic acid, however, the mechanism by which 1 and 1PTA and 1PTA2 catalyze hydrogen differ in the initial reductive processes.

Original languageEnglish (US)
Pages (from-to)3050-3056
Number of pages7
JournalDalton Transactions
Volume39
Issue number12
DOIs
StatePublished - Mar 19 2010

ASJC Scopus subject areas

  • Inorganic Chemistry

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