Symbiotic prodrugs (SymProDs) dual targeting of NFkappaB and CDK

Chem Biol Drug Des. 2020 Aug;96(2):773-784. doi: 10.1111/cbdd.13684. Epub 2020 Apr 22.

Abstract

The release of an active drug from the prodrug generates a pro-fragment that typically has no biological activity and could result in adverse effects. By combining two drugs, wherein each drug acts as a pro-fragment of the other drug will eliminate the pro-fragment in the prodrug. As they are prodrugs of each other and are symbiotic, we termed these as symbiotic prodrugs (SymProDs). To test this idea, we generated SymProDs using NFκB inhibitors that contain the reactive α-methylene-γ-butyrolactone moiety and CDK inhibitors with solvent exposed secondary nitrogen atoms. We show that secondary amine prodrugs of α-methylene-γ-butyrolactone containing NFκB inhibitors undergo slow release over a 72 hr period. Using an alkyne-tagged secondary amine prodrug of α-methylene-γ-butyrolactone containing NFκB inhibitor, we demonstrate target engagement. The NFκB-CDK SymProDs were ~20- to 200-fold less active against the corresponding CDK inhibitors in in vitro CDK kinase assays. Growth inhibition studies in a panel of ovarian cancer cell lines revealed potency trends of the SymProDs mirrored those of the single treatments suggesting their dissociation in cells. In conclusion, our results suggest that SymProDs offer a productive path forward for advancing compounds with reactive functionality and can be used as dual targeting agents.

Keywords: CDK; NFkappaB; prodrugs.

Publication types

  • Research Support, N.I.H., Extramural
  • Research Support, Non-U.S. Gov't

MeSH terms

  • 4-Butyrolactone / analogs & derivatives*
  • 4-Butyrolactone / chemical synthesis
  • 4-Butyrolactone / pharmacology
  • Amines / chemistry
  • Antineoplastic Agents / chemical synthesis*
  • Antineoplastic Agents / pharmacology
  • Apoptosis / drug effects
  • Cell Line, Tumor
  • Cell Proliferation / drug effects
  • Cyclin-Dependent Kinases / metabolism*
  • Drug Screening Assays, Antitumor
  • Female
  • Humans
  • Molecular Targeted Therapy
  • NF-kappa B / metabolism*
  • Ovarian Neoplasms / drug therapy*
  • Piperazines / chemical synthesis
  • Piperazines / metabolism
  • Piperidines / chemical synthesis
  • Piperidines / metabolism
  • Prodrugs / chemistry*
  • Prodrugs / pharmacology
  • Protein Kinase Inhibitors / chemical synthesis*
  • Protein Kinase Inhibitors / pharmacology
  • Pyrazoles / chemical synthesis
  • Pyrazoles / metabolism
  • Pyridines / chemical synthesis
  • Pyridines / metabolism
  • Sesquiterpenes / chemical synthesis
  • Sesquiterpenes / pharmacology
  • Signal Transduction
  • Structure-Activity Relationship

Substances

  • 4-(2,6-dichlorobenzoylamino)-1H-pyrazole-3-carboxylic acid piperidin-4-ylamide
  • Amines
  • Antineoplastic Agents
  • NF-kappa B
  • Piperazines
  • Piperidines
  • Prodrugs
  • Protein Kinase Inhibitors
  • Pyrazoles
  • Pyridines
  • Sesquiterpenes
  • parthenolide
  • alpha-methylene gamma-butyrolactone
  • Cyclin-Dependent Kinases
  • palbociclib
  • 4-Butyrolactone