Discovery of 2-substituted 1H-benzo[d]immidazole-4-carboxamide derivatives as novel poly(ADP-ribose)polymerase-1 inhibitors with in vivo anti-tumor activity

Eur J Med Chem. 2017 May 26:132:26-41. doi: 10.1016/j.ejmech.2017.03.013. Epub 2017 Mar 18.

Abstract

Novel 1H-benzo[d]immidazole-4-carboxamide derivatives bearing five-membered or six-membered N-heterocyclic moieties at the 2-position were designed and synthesized as PARP-1 inhibitors. Structure-activity relationships were conducted and led to a number of potent PARP-1 inhibitors having IC50 values in the single or double digit nanomolar level. Some potent PARP-1 inhibitors also had similar inhibitory activities against PARP-2. Among all the synthesized compounds, compound 10a and 11e displayed strong potentiation effects on temozolomide (TMZ) in MX-1 cells (PF50 = 7.10, PF50 = 4.17). In vivo tumor growth inhibition was investigated using compound 10a in combination with TMZ, and it was demonstrated that compound 10a could strongly potentiate the cytotoxicity of TMZ in MX-1 xenograft tumor model. Two co-crystal structures of compounds 11b and 15e complexed with PARP-1 were achieved and demonstrated a unique binding mode of these benzo-imidazole derivatives.

Keywords: Anti-tumor agents; Benzo[d]immidazole-4-carboxamide; PARP-1 inhibitor; PARP-2 inhibitor.

MeSH terms

  • Antineoplastic Agents, Alkylating / pharmacology
  • Antineoplastic Combined Chemotherapy Protocols / pharmacology
  • Benzimidazoles / chemical synthesis*
  • Benzimidazoles / chemistry
  • Benzimidazoles / pharmacology*
  • Cell Line
  • Crystallography, X-Ray
  • Dacarbazine / analogs & derivatives
  • Dacarbazine / pharmacology
  • Drug Design
  • Drug Synergism
  • Enzyme Inhibitors / chemical synthesis
  • Enzyme Inhibitors / pharmacology
  • Heterografts
  • Inhibitory Concentration 50
  • Poly (ADP-Ribose) Polymerase-1 / antagonists & inhibitors*
  • Protein Binding
  • Structure-Activity Relationship
  • Temozolomide

Substances

  • Antineoplastic Agents, Alkylating
  • Benzimidazoles
  • Enzyme Inhibitors
  • Dacarbazine
  • Poly (ADP-Ribose) Polymerase-1
  • Temozolomide