Electrophilic nitro-fatty acids activate NRF2 by a KEAP1 cysteine 151-independent mechanism

J Biol Chem. 2011 Apr 22;286(16):14019-27. doi: 10.1074/jbc.M110.190710. Epub 2011 Feb 25.

Abstract

Nitro-fatty acids (NO(2)-FAs) are electrophilic signaling mediators formed in vivo via nitric oxide (NO)- and nitrite (NO(2)(-))-dependent reactions. Nitro-fatty acids modulate signaling cascades via reversible covalent post-translational modification of nucleophilic amino acids in regulatory proteins and enzymes, thus altering downstream signaling events, such as Keap1-Nrf2-antioxidant response element (ARE)-regulated gene expression. In this study, we investigate the molecular mechanisms by which 9- and 10-nitro-octadec-9-enoic acid (OA-NO(2)) activate the transcription factor Nrf2, focusing on the post-translational modifications of cysteines in the Nrf2 inhibitor Keap1 by nitroalkylation and its downstream responses. Of the two regioisomers, 9-nitro-octadec-9-enoic acid was a more potent ARE inducer than 10-nitro-octadec-9-enoic acid. The most OA-NO(2)-reactive Cys residues in Keap1 were Cys(38), Cys(226), Cys(257), Cys(273), Cys(288), and Cys(489). Of these, Cys(273) and Cys(288) accounted for ∼50% of OA-NO(2) reactions in a cellular milieu. Notably, Cys(151) was among the least OA-NO(2)-reactive of the Keap1 Cys residues, with mutation of Cys(151) having no effect on net OA-NO(2) reaction with Keap1 or on ARE activation. Unlike many other Nrf2-activating electrophiles, OA-NO(2) enhanced rather than diminished the binding between Keap1 and the Cul3 subunit of the E3 ligase for Nrf2. OA-NO(2) can therefore be categorized as a Cys(151)-independent Nrf2 activator, which in turn can influence the pattern of gene expression and therapeutic actions of nitroalkenes.

Publication types

  • Research Support, N.I.H., Extramural
  • Research Support, Non-U.S. Gov't

MeSH terms

  • Adaptor Proteins, Signal Transducing / chemistry*
  • Animals
  • Chromatography, Liquid / methods
  • Cysteine / chemistry*
  • Cytoskeletal Proteins / chemistry*
  • Fatty Acids / chemistry*
  • Gene Expression Regulation
  • Humans
  • Intracellular Signaling Peptides and Proteins / chemistry*
  • Kelch-Like ECH-Associated Protein 1
  • Linoleic Acids / chemistry
  • Mass Spectrometry / methods
  • Mice
  • Mutation
  • NF-E2-Related Factor 2 / chemistry*
  • Nitro Compounds / chemistry
  • Oleic Acids / chemistry
  • Protein Processing, Post-Translational
  • Signal Transduction
  • Transcription Factors / metabolism
  • Ubiquitin-Protein Ligases / chemistry

Substances

  • 9-nitrooctadec-9-enoic acid
  • Adaptor Proteins, Signal Transducing
  • Cytoskeletal Proteins
  • Fatty Acids
  • Intracellular Signaling Peptides and Proteins
  • KEAP1 protein, human
  • Keap1 protein, mouse
  • Kelch-Like ECH-Associated Protein 1
  • Linoleic Acids
  • NF-E2-Related Factor 2
  • Nitro Compounds
  • Oleic Acids
  • Transcription Factors
  • Ubiquitin-Protein Ligases
  • Cysteine