Use of photoaffinity labeling and site-directed mutagenesis for identification of the key residue responsible for extraordinarily high affinity binding of UCN-01 in human alpha1-acid glycoprotein

J Biol Chem. 2005 Jan 14;280(2):1384-91. doi: 10.1074/jbc.M411076200. Epub 2004 Oct 27.

Abstract

7-Hydroxystaurosporine (UCN-01) is a protein kinase inhibitor anticancer drug currently undergoing a phase II clinical trial. The low distribution volumes and systemic clearance of UCN-01 in human patients have been found to be caused in part by its extraordinarily high affinity binding to human alpha1-acid glycoprotein (hAGP). In the present study, we photolabeled hAGP with [3H]UCN-01 without further chemical modification. The photolabeling specificity of [3H]UCN-01 was confirmed by findings in which other hAGP binding ligands inhibited formation of covalent bonds between hAGP and [3H]UCN-01. The amino acid sequence of the photolabeled peptide was concluded to be SDVVYTDXK, corresponding to residues Ser-153 to Lys-161 of hAGP. No PTH derivatives were detected at the 8th cycle, which corresponded to the 160th Trp residue. This strongly implies that Trp-160 was photolabeled by [3H]UCN-01. Three recombinant hAGP mutants (W25A, W122A, and W160A) and wild-type recombinant hAGP were photolabeled by [3H]UCN-01. Only mutant W160A showed a marked decrease in the extent of photoincorporation. These results strongly suggest that Trp-160 plays a prominent role in the high affinity binding of [3H]UCN-01 to hAGP. A docking model of UCN-01 and hAGP around Trp-160 provided further details of the binding site topology.

MeSH terms

  • Amino Acid Sequence
  • Binding, Competitive
  • Chromatography, High Pressure Liquid
  • Humans
  • Models, Molecular
  • Molecular Sequence Data
  • Mutagenesis, Site-Directed / genetics*
  • Mutation / genetics
  • Orosomucoid / chemistry*
  • Orosomucoid / genetics
  • Orosomucoid / metabolism*
  • Photoaffinity Labels*
  • Protein Binding
  • Protein Conformation
  • Staurosporine / analogs & derivatives*
  • Staurosporine / metabolism*
  • Time Factors
  • Trypsin / metabolism

Substances

  • Orosomucoid
  • Photoaffinity Labels
  • 7-hydroxystaurosporine
  • Trypsin
  • Staurosporine