Proton demand inversion in a mutant protein tyrosine kinase reaction

J Am Chem Soc. 2002 May 29;124(21):5956-7. doi: 10.1021/ja025993a.

Abstract

In contrast to previous studies that have shown that the neutral phenol serves as the nucleophile for WT Csk-promoted phosphorylation of a tyrosine-containing substrate, the phenolate ion acts as primary nucleophile for the D314N Csk-catalyzed reaction. Rate comparisons of D314N Csk-promoted phosphotransfer using a series of fluorotyrosine-containing peptide substrates reveal a near zero beta(nuc), consistent with a dissociative mechanism of phosphotransfer. These combined results argue against a hydroxy nucleophile-to-phosphate proton transfer occurring prior to an associative transition state of phosphoryl transfer.

Publication types

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

MeSH terms

  • Aspartic Acid / chemistry
  • Aspartic Acid / metabolism
  • Kinetics
  • Mutation
  • Oligopeptides / chemistry
  • Oligopeptides / metabolism
  • Protein-Tyrosine Kinases / chemistry*
  • Protein-Tyrosine Kinases / metabolism*
  • Proto-Oncogene Proteins pp60(c-src)*
  • Protons
  • Substrate Specificity

Substances

  • Oligopeptides
  • Protons
  • Aspartic Acid
  • Matk protein, mouse
  • Protein-Tyrosine Kinases
  • Proto-Oncogene Proteins pp60(c-src)