Temperature-dependent ESR and computational studies on antiferromagnetic electron transfer in the yeast NADH dehydrogenase Ndi1

Phys Chem Chem Phys. 2017 Feb 8;19(6):4849-4854. doi: 10.1039/c6cp08107j.

Abstract

Ndi1 is a special type-II complex I nicotinamide-adenine-dinucleotide (NADH):ubiquinone (UQ) oxidoreductase in the yeast respiratory chain, with two bound UQs (UQI and UQII) mediating electron transfer from flavin cofactors to ubiquinone, in the absence of Fe-S chains. Here, we elucidate the underlying mechanism of electron transfer in Ndi1 through temperature-dependent Electron Spin Resonance (ESR) experiments in conjunction with quantum chemical calculations. It is revealed that electron transfer is mediated by antiferromagnetic (AFM) interactions between flavin-adenosine-dinucleotide (FAD) and UQI and between UQI and UQII. The π-stacking interactions among the aromatic complexes also enhance the through-space electron transfer. The FAD/UQI pair works as a rectifier converting double-electron co-transfer into sequential single-electron transfer events. The results not only expand our understanding on the observed AFM interactions among p-orbital aromatic mixed-stack in proteins, but also provide significant insights into the fabrication of materials with special magnetic properties using biological samples.

MeSH terms

  • Electron Spin Resonance Spectroscopy*
  • Electron Transport Complex I / chemistry
  • Electron Transport Complex I / metabolism*
  • Electron Transport*
  • Iron / chemistry
  • Magnetics
  • Models, Chemical*
  • Saccharomyces cerevisiae Proteins / chemistry
  • Saccharomyces cerevisiae Proteins / metabolism*
  • Temperature*

Substances

  • Ndi1 protein, S cerevisiae
  • Saccharomyces cerevisiae Proteins
  • Iron
  • Electron Transport Complex I