Structural implications of the paramagnetically shifted NMR signals from pyridine H atoms on synthetic nonheme FeIV=O complexes

J Biol Inorg Chem. 2019 Jun;24(4):533-545. doi: 10.1007/s00775-019-01672-3. Epub 2019 Jun 6.

Abstract

Oxoiron(IV) motifs are found in important intermediates in many enzymatic cycles that involve oxidations. Over half of the reported synthetic nonheme oxoiron(IV) analogs incorporate heterocyclic donors, with a majority of them comprising pyridines. Herein, we report 1H-NMR studies of oxoiron(IV) complexes containing pyridines that are arranged in different configurations relative to the Fe = O unit and give rise to paramagnetically shifted resonances that differ by as much as 50 ppm. The strong dependence of 1H-NMR shifts on the different configurations and orientation of pyridines relative to the oxoiron(IV) unit demonstrates how unpaired electronic spin density of the iron center affects the chemical shifts of these protons.

Keywords: Iron(IV)-oxo complexes; NMR; Nonheme iron.

Publication types

  • Research Support, Non-U.S. Gov't
  • Research Support, U.S. Gov't, Non-P.H.S.

MeSH terms

  • Density Functional Theory
  • Hydrogen / chemistry*
  • Iron / chemistry*
  • Magnetic Resonance Spectroscopy
  • Models, Molecular
  • Molecular Conformation
  • Oxygen / chemistry*
  • Pyridines / chemistry*

Substances

  • Pyridines
  • Hydrogen
  • Iron
  • Oxygen