Self-immolative nitrogen mustards prodrugs cleavable by carboxypeptidase G2 (CPG2) showing large cytotoxicity differentials in GDEPT

J Med Chem. 2003 Apr 24;46(9):1690-705. doi: 10.1021/jm020462i.

Abstract

Nineteen novel potential self-immolative prodrugs and their corresponding drugs have been synthesized for gene-directed enzyme prodrug therapy (GDEPT) with carboxypeptidase G2 (CPG2) as the activating enzyme. The compounds are derived from o- and p-amino and p-methylamino aniline nitrogen mustards. Their aqueous stability, kinetics of drug release by CPG2, and cytotoxicity in the colon carcinoma cell line WiDr, expressing either surface-tethered CPG2 (stCPG2(Q)3) or control beta-galactosidase, are assessed. The effect of various structural features on stability, kinetics of activation, and biological activity is discussed. The p-methylamino prodrugs are the most stable compounds from this series, with the largest cytotoxicity differentials between CPG2-expressing and nonexpressing cells. The most potent compounds in all series are prodrugs of bis-iodo nitrogen mustards. 4-[N-[4'-Bis(2' '-iodoethyl)aminophenyl]-N'-methylcarbamoyloxymethyl]phenylcarbamoyl-l-glutamic acid, compound 39b, is 124-fold more cytotoxic to WiDr cells expressing CPG2 than to cells expressing beta-galactosidase. An additional six compounds show better cytotoxicity differential than the published N-[4-[(2-chloroethyl)(2-mesyloxyethyl)amino]benzoyl]-l-glutamic acid (CMDA) prodrug.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Aniline Mustard / chemical synthesis*
  • Aniline Mustard / chemistry
  • Aniline Mustard / pharmacokinetics
  • Antineoplastic Agents, Alkylating / chemical synthesis*
  • Antineoplastic Agents, Alkylating / chemistry
  • Antineoplastic Agents, Alkylating / pharmacokinetics
  • Carbamates / chemical synthesis*
  • Carbamates / chemistry
  • Carbamates / pharmacokinetics
  • Gene Transfer Techniques
  • Glutamic Acid / analogs & derivatives
  • Glutamic Acid / chemical synthesis*
  • Glutamic Acid / chemistry
  • Glutamic Acid / pharmacokinetics
  • Half-Life
  • Humans
  • Prodrugs / chemical synthesis*
  • Prodrugs / chemistry
  • Prodrugs / pharmacokinetics
  • Quantitative Structure-Activity Relationship
  • Tumor Cells, Cultured
  • gamma-Glutamyl Hydrolase / genetics
  • gamma-Glutamyl Hydrolase / metabolism*

Substances

  • 4-(N-(4'-bis(2''-iodoethyl)aminophenyl)-N-methylcarbamoyloxymethyl)phenylcarbamoylglutamic acid
  • Antineoplastic Agents, Alkylating
  • Carbamates
  • Prodrugs
  • Glutamic Acid
  • Aniline Mustard
  • gamma-Glutamyl Hydrolase