An Oncometabolite Isomer Rapidly Induces a Pathophysiological Protein Modification

ACS Chem Biol. 2020 Apr 17;15(4):856-861. doi: 10.1021/acschembio.0c00044. Epub 2020 Apr 6.

Abstract

Metabolites regulate protein function via covalent and noncovalent interactions. However, manipulating these interactions in living cells remains a major challenge. Here, we report a chemical strategy for inducing cysteine S-succination, a nonenzymatic post-translational modification derived from the oncometabolite fumarate. Using a combination of antibody-based detection and kinetic assays, we benchmark the in vitro and cellular reactivity of two novel S-succination "agonists," maleate and 2-bromosuccinate. Cellular assays reveal maleate to be a more potent and less toxic inducer of S-succination, which can activate KEAP1-NRF2 signaling in living cells. By enabling the cellular reconstitution of an oncometabolite-protein interaction with physiochemical accuracy and minimal toxicity, this study provides a methodological basis for better understanding the signaling role of metabolites in disease.

Publication types

  • Research Support, N.I.H., Intramural

MeSH terms

  • Acylation
  • Cell Line, Tumor
  • Cysteine / chemistry*
  • Fumarates / chemistry
  • Fumarates / pharmacology*
  • Fumarates / toxicity
  • HEK293 Cells
  • Humans
  • Hydrogen-Ion Concentration
  • Maleates / chemistry
  • Maleates / pharmacology*
  • Maleates / toxicity
  • Phenols / chemistry
  • Protein Processing, Post-Translational / drug effects*
  • Proteome / chemistry
  • Proteome / metabolism*
  • Proteomics / methods
  • Succinates / chemistry
  • Succinates / pharmacology*
  • Succinates / toxicity
  • Sulfhydryl Compounds / chemistry

Substances

  • Fumarates
  • Maleates
  • Phenols
  • Proteome
  • Succinates
  • Sulfhydryl Compounds
  • thiophenol
  • maleic acid
  • Cysteine
  • bromosuccinic acid