Differences in the transient kinetics of the binding of D-ADP and its mirror image L-ADP to human 3-phosphoglycerate kinase revealed by the presence of 3-phosphoglycerate

Biochemistry. 2008 Mar 18;47(11):3462-73. doi: 10.1021/bi7023145. Epub 2008 Feb 21.

Abstract

L-Nucleosides comprise a new class of antiviral and anticancer agents that are converted in vivo by a cascade of kinases to pharmacologically active nucleoside triphosphates. The last step of the cascade may be catalyzed by 3-phosphoglycerate kinase (PGK), an enzyme that has low specificity for nucleoside diphosphate (NDP): NDP + 1,3-bisphosphoglycerate <--> NTP + 3-phosphoglycerate. Here we compared the kinetics of the formation of the complexes of human PGK with d- and its mirror image l-ADP and the effect of 3-phosphoglycerate (PG) on these by exploiting the fluorescence signal of PGK that occurs upon its interaction with nucleotide substrate. Two types of experiment were carried out: equilibrium (estimation of dissociation constants) and stopped-flow (transient kinetics of the interactions). We show that under our experimental conditions (buffer containing 30% methanol, 4 degrees C) PGK binds d- and l-ADP with similar kinetics. However, whereas PG increased the dissociation rate constant for d-ADP by a factor of 8-which is a kinetic explanation for "substrate antagonism"-PG had little effect on this constant for l-ADP. We explain this difference by a molecular modeling study that showed that the beta-phosphates of d- and l-ADP have different orientations when bound to the active site of human PGK. The difference is unexpected because l-ADP is almost as catalytically competent as d-ADP [ Varga, A. et al. (2008) Biochem. Biophys. Res. Commun. 366, 994-1000].

Publication types

  • Comparative Study
  • Research Support, Non-U.S. Gov't

MeSH terms

  • Adenosine Diphosphate / chemistry*
  • Adenosine Diphosphate / metabolism*
  • Binding Sites
  • Buffers
  • Catalysis
  • Cold Temperature
  • Glyceric Acids / chemistry*
  • Glyceric Acids / metabolism
  • Humans
  • Kinetics
  • Methanol
  • Models, Molecular
  • Phosphoglycerate Kinase / chemistry*
  • Phosphoglycerate Kinase / metabolism*
  • Stereoisomerism

Substances

  • Buffers
  • Glyceric Acids
  • Adenosine Diphosphate
  • 3-phosphoglycerate
  • Phosphoglycerate Kinase
  • Methanol