Redox-based reagents for chemoselective methionine bioconjugation

Science. 2017 Feb 10;355(6325):597-602. doi: 10.1126/science.aal3316.

Abstract

Cysteine can be specifically functionalized by a myriad of acid-base conjugation strategies for applications ranging from probing protein function to antibody-drug conjugates and proteomics. In contrast, selective ligation to the other sulfur-containing amino acid, methionine, has been precluded by its intrinsically weaker nucleophilicity. Here, we report a strategy for chemoselective methionine bioconjugation through redox reactivity, using oxaziridine-based reagents to achieve highly selective, rapid, and robust methionine labeling under a range of biocompatible reaction conditions. We highlight the broad utility of this conjugation method to enable precise addition of payloads to proteins, synthesis of antibody-drug conjugates, and identification of hyperreactive methionine residues in whole proteomes.

Publication types

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

MeSH terms

  • Actins / chemistry
  • Aziridines / chemistry*
  • Cysteine / chemistry*
  • Gene Editing
  • Gene Knockout Techniques
  • Immunoconjugates / chemistry*
  • Methionine / analysis
  • Methionine / chemistry*
  • Mutation
  • Oxidation-Reduction
  • Phosphopyruvate Hydratase / genetics
  • Protein Domains
  • Proteins / chemistry
  • Proteomics / methods
  • Saccharomyces cerevisiae / drug effects
  • Saccharomyces cerevisiae / enzymology
  • Saccharomyces cerevisiae / genetics
  • Saccharomyces cerevisiae / growth & development
  • Saccharomyces cerevisiae Proteins / genetics
  • Sodium Hypochlorite / pharmacology

Substances

  • Actins
  • Aziridines
  • Immunoconjugates
  • Proteins
  • Saccharomyces cerevisiae Proteins
  • Methionine
  • Sodium Hypochlorite
  • ENO1 protein, S cerevisiae
  • Phosphopyruvate Hydratase
  • Cysteine