Enzyme specific activation of benzoquinone ansamycin prodrugs using HuCC49DeltaCH2-beta-galactosidase conjugates

J Med Chem. 2006 Oct 19;49(21):6290-7. doi: 10.1021/jm060647f.

Abstract

To activate prodrugs for cancer treatment, an anti-TAG-72 antibody (HuCC49DeltaCH2) was used for delivery of an activation enzyme (beta-galactosidase) to specifically activate a geldanamycin prodrug (17-AG-C2-Gal) against colon cancer. The geldanamycin prodrug 17-AG-C2-Gal was synthesized by coupling a galactose-amine derivative with geldanamycin at the C-17 position. Molecular docking with two different programs (Affinity and Autodock) showed that the prodrug (17-AG-C2-Gal) was unable to bind to Hsp90; however, the product (17-AG-C2), enzymatically cleaved by beta-galactosidase conjugate, bound to Hsp90 in a similar way as geldanamycin and 17-AG. The computational docking results were further confirmed in experimental testing by the tetrazolium [3-(4,5-dimethythiazol-2-yl)]-5-(3-carboxymethoxyphenyl)-2-(4-sulfophenyl)-2H-tetrazolium assay and mass spectrometry. HuCC49DeltaCH2 was chemically conjugated to beta-galactosidase. The antibody-enzyme conjugate was able to target tumor antigen TAG-72 with the well-preserved enzymatic activity to activate 17-AG-C2-Gal prodrug. The released active drug 17-AG-C2 was demonstrated to induce up to 70% AKT degradation and enhance anticancer activity by more than 25-fold compared to the prodrug.

Publication types

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

MeSH terms

  • Antibodies, Monoclonal / chemistry*
  • Antigens, Neoplasm / immunology*
  • Antineoplastic Agents / administration & dosage
  • Antineoplastic Agents / chemistry*
  • Antineoplastic Agents / pharmacology
  • Benzoquinones / chemistry*
  • Cell Line, Tumor
  • Colonic Neoplasms
  • Drug Carriers
  • Drug Delivery Systems
  • Galactosides / administration & dosage
  • Galactosides / chemistry*
  • Glycoproteins / immunology*
  • HSP90 Heat-Shock Proteins / chemistry
  • HSP90 Heat-Shock Proteins / metabolism
  • Humans
  • Indicators and Reagents
  • Lactams, Macrocyclic / administration & dosage
  • Lactams, Macrocyclic / chemistry*
  • Mass Spectrometry
  • Models, Molecular
  • Prodrugs / administration & dosage
  • Prodrugs / chemistry*
  • Prodrugs / pharmacology
  • Protein Binding
  • Proto-Oncogene Proteins c-akt / metabolism
  • Tetrazolium Salts
  • Thiazoles
  • beta-Galactosidase / chemistry*

Substances

  • 17-amino-17-demethoxygeldanamycin -C2-galactose
  • Antibodies, Monoclonal
  • Antigens, Neoplasm
  • Antineoplastic Agents
  • Benzoquinones
  • Drug Carriers
  • Galactosides
  • Glycoproteins
  • HSP90 Heat-Shock Proteins
  • Indicators and Reagents
  • Lactams, Macrocyclic
  • Prodrugs
  • Tetrazolium Salts
  • Thiazoles
  • tumor-associated antigen 72
  • 3-(4,5-dimethylthiazol-2-yl)-5-(3-carboxymethoxyphenyl)-2-(4-sulfophenyl)-2H-tetrazolium
  • Proto-Oncogene Proteins c-akt
  • beta-Galactosidase
  • 17-aminogeldanamycin
  • geldanamycin