Design, synthesis, and pharmacological evaluation of thapsigargin analogues for targeting apoptosis to prostatic cancer cells

J Med Chem. 2001 Dec 20;44(26):4696-703. doi: 10.1021/jm010985a.

Abstract

A series of thapsigargin (TG) analogues, containing an amino acid applicable for conjugation to a peptide specifically cleaved by prostate-specific antigen (PSA), has been prepared to develop the drug-moiety of prodrugs for treatment of prostatic cancer. The analogues were synthesized by converting TG into O-8-debutanoylthapsigargin (DBTG) and esterifying O-8 of DBTG with various amino acid linkers. The compounds were evaluated for their ability to elevate the cytosolic Ca(2+) concentration ([Ca(2+)](i)) in TSU-Pr1 cells, their ability to inhibit the rabbit skeletal muscle SERCA pump, and their ability to induce apoptosis in TSU-Pr1 human prostatic cancer cells. The activity of analogues, in which DBTG were esterified with omega-amino acids [HOOC(CH(2))(n)()NH(2), n = 5-7, 10, 11], increased with the linker length. Analogues with 3-[4-(L-leucinoylamino)phenyl]propanoyl, 6-(L-leucinoylamino)hexanoyl, and 12-(L-serinoylamino)dodecanoyl were considerably less active than TG, and analogues with 12-(L-alaninoylamino)dodecanoyl and 12-(L-phenylalaninoylamino)dodecanoyl were almost as active as TG. The 12-(L-leucinoylamino)dodecanoyl gave an analogue equipotent with TG, making this compound promising as the drug-moiety of a PSA sensitive prodrug of TG.

Publication types

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

MeSH terms

  • Animals
  • Antineoplastic Agents / chemical synthesis*
  • Antineoplastic Agents / chemistry
  • Antineoplastic Agents / pharmacology
  • Apoptosis*
  • Calcium / metabolism
  • Calcium-Transporting ATPases / metabolism
  • Drug Design
  • Drug Screening Assays, Antitumor
  • Humans
  • Male
  • Muscle, Skeletal / enzymology
  • Prostatic Neoplasms / pathology*
  • Rabbits
  • Sarcoplasmic Reticulum Calcium-Transporting ATPases
  • Structure-Activity Relationship
  • Thapsigargin / analogs & derivatives*
  • Thapsigargin / chemical synthesis*
  • Thapsigargin / chemistry
  • Thapsigargin / pharmacology
  • Tumor Cells, Cultured

Substances

  • 8-O-(12-(leucinoylamino)dodecanoyl)-8-O-debutanoylthapsigargin
  • Antineoplastic Agents
  • Thapsigargin
  • Sarcoplasmic Reticulum Calcium-Transporting ATPases
  • Calcium-Transporting ATPases
  • Calcium