Tuning the Fe(II/III) Redox Potential in Nonheme Fe(II)-Hydroxo Complexes through Primary and Secondary Coordination Sphere Modifications

Zachary Gordon, Michael J. Drummond, Ellen M. Matson, Justin A. Bogart, Eric J. Schelter, Richard L. Lord, Alison R. Fout

Research output: Contribution to journalArticlepeer-review

Abstract

The derivatization of the imino-functionalized tris(pyrrolylmethyl)amine ligand framework, N(XpiR)3 (XLR; X = H, Br; R = cyclohexyl (Cy), phenyl (Ph), 2,6- diisopropylphenyl (DIPP)), is reported. Modular ligand synthesis allows for facile modification of both the primary and secondary coordination sphere electronics. The iron(II)-hydroxo complexes, N(XpiR)(XafaR)2Fe(II)OH (XLRFeIIOH), are synthesized to establish the impact of the ligand modifications on the complexes’ electronic properties, including their chemical and electrochemical oxidation. Cyclic voltammetry demonstrates that the Fe(II/III) redox couple spans a 400 mV range across the series. The origin of the shifted potential is explained based on spectroscopic, structural, and theoretical analyses of the iron(II) and iron(III) compounds.

Original languageEnglish (US)
Pages (from-to)4852-4863
Number of pages12
JournalInorganic Chemistry
Volume56
Issue number9
DOIs
StatePublished - May 1 2017

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry
  • Inorganic Chemistry

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